---
OA_place: publisher
OA_type: hybrid
PlanS_conform: '1'
_id: '21040'
abstract:
- lang: eng
text: Formation during the first cycles of Li-rich layered oxide (LRLO) cathode
materials consolidates the interphase and leads to structural changes that are
decisive for long-term cyclability. However, the nature and effect of the changes
are material-dependent and unknown for the important class of Co-free, Ni-poor
LRLOs. Here, we analyze the processes during the tailored formation procedure
of a typical class member, Li1.28Ni0.15Mn0.57O2, and demonstrate that it remarkably
changes lattice composition and structure as a prerequisite for stable cycling.
We combine electrochemistry, operando mass spectrometry, X-ray diffraction, and
X-ray absorption spectroscopy with density functional theory simulations. Activation
most prominently compresses the layer spacing along the c-axis and increases reversible
structural breathing. The large capacity of ∼250 mAh g–1 originates from the Ni2+/Ni4+
and O2–/O– redox couples. Electron exchange during O-redox is smeared over the
entire anionic sublattice rather than localized on specific oxygen atomic sites.
This redox mechanism is reversible without detrimental oxygen evolution, avoiding
continued degradation common in conventional LRLOs. Sequential Ni- and O-redox
during activation irreversibly distorts the coordination of the redox-inactive
Mn4+ centers. This structural evolution of the MnO6 octahedra appears to enable
the superior electrochemical performance of this LRLO phase. These findings define
an activation pathway for the important class of Co-free, Ni-poor LRLOs, offering
potential guidance for the rational design of high-performance, more sustainable
cathode materials.
acknowledged_ssus:
- _id: M-Shop
- _id: LifeSc
acknowledgement: 'Elettra-Sincrotrone Trieste S.C.p.A. and its staff are acknowledged
for providing synchrotron radiation beamtime and laboratory facilities, in particular
the MCX and XAFS beamlines, where the XRD and XAS experiments have been carried
out, supported by the projects number: 20217082, 20205109, and 20195014. This study
was carried out within the MOST─Sustainable Mobility Center and received funding
from the European Union Next-Generation EU (PIANO NAZIONALE DI RIPRESA E RESILIENZA
(PNRR)─MISSIONE 4 COMPONENTE 2, INVESTIMENTO 1.4─D.D. 1033 17/06/2022, CN00000023).
Moreover, the contribution of S.B. and A.C. to this study was carried out within
the NEST─Network for Energy Sustainable Transition and received funding from the
European Union Next-Generation EU (PNRR─MISSIONE 4 COMPONENTE 2, INVESTIMENTO 1.3─D.D.
1561 11/10/2022, B53C22004070006). This manuscript reflects only the authors’ views
and opinions, neither the European Union nor the European Commission can be considered
responsible for them. Two of us, S.B. and S.A.F., would like to thank the Alistore
ERI. L.S. received funds from the Ministry of Ecological Transition in the “Ricerca
di Sistema Elettrico” framework. S.A.F. is indebted to ISTA for support. The Scientific
Service Units of ISTA supported this research through resources provided by the
Lab Support Facility and the Miba Machine Shop.'
article_processing_charge: Yes (via OA deal)
article_type: original
author:
- first_name: Matteo
full_name: Busato, Matteo
last_name: Busato
- first_name: Mariarosaria
full_name: Tuccillo, Mariarosaria
last_name: Tuccillo
- first_name: Arcangelo
full_name: Celeste, Arcangelo
last_name: Celeste
- first_name: Alessandro
full_name: Tofoni, Alessandro
last_name: Tofoni
- first_name: Laura
full_name: Silvestri, Laura
last_name: Silvestri
- first_name: Paola
full_name: D’Angelo, Paola
last_name: D’Angelo
- first_name: Stefan Alexander
full_name: Freunberger, Stefan Alexander
id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425
last_name: Freunberger
orcid: 0000-0003-2902-5319
- first_name: Sergio
full_name: Brutti, Sergio
last_name: Brutti
citation:
ama: Busato M, Tuccillo M, Celeste A, et al. Structural rearrangements of a Cobalt-free
Lithium-rich layered oxide cathode during formation. ACS Applied Energy Materials.
2026;9(1):686-697. doi:10.1021/acsaem.5c03511
apa: Busato, M., Tuccillo, M., Celeste, A., Tofoni, A., Silvestri, L., D’Angelo,
P., … Brutti, S. (2026). Structural rearrangements of a Cobalt-free Lithium-rich
layered oxide cathode during formation. ACS Applied Energy Materials. American
Chemical Society. https://doi.org/10.1021/acsaem.5c03511
chicago: Busato, Matteo, Mariarosaria Tuccillo, Arcangelo Celeste, Alessandro Tofoni,
Laura Silvestri, Paola D’Angelo, Stefan Alexander Freunberger, and Sergio Brutti.
“Structural Rearrangements of a Cobalt-Free Lithium-Rich Layered Oxide Cathode
during Formation.” ACS Applied Energy Materials. American Chemical Society,
2026. https://doi.org/10.1021/acsaem.5c03511.
ieee: M. Busato et al., “Structural rearrangements of a Cobalt-free Lithium-rich
layered oxide cathode during formation,” ACS Applied Energy Materials,
vol. 9, no. 1. American Chemical Society, pp. 686–697, 2026.
ista: Busato M, Tuccillo M, Celeste A, Tofoni A, Silvestri L, D’Angelo P, Freunberger
SA, Brutti S. 2026. Structural rearrangements of a Cobalt-free Lithium-rich layered
oxide cathode during formation. ACS Applied Energy Materials. 9(1), 686–697.
mla: Busato, Matteo, et al. “Structural Rearrangements of a Cobalt-Free Lithium-Rich
Layered Oxide Cathode during Formation.” ACS Applied Energy Materials,
vol. 9, no. 1, American Chemical Society, 2026, pp. 686–97, doi:10.1021/acsaem.5c03511.
short: M. Busato, M. Tuccillo, A. Celeste, A. Tofoni, L. Silvestri, P. D’Angelo,
S.A. Freunberger, S. Brutti, ACS Applied Energy Materials 9 (2026) 686–697.
corr_author: '1'
date_created: 2026-01-25T23:01:40Z
date_published: 2026-01-12T00:00:00Z
date_updated: 2026-02-12T14:04:04Z
day: '12'
ddc:
- '540'
department:
- _id: StFr
doi: 10.1021/acsaem.5c03511
file:
- access_level: open_access
checksum: 81272c19df41c696c1737168d3ea8c16
content_type: application/pdf
creator: dernst
date_created: 2026-02-12T13:55:28Z
date_updated: 2026-02-12T13:55:28Z
file_id: '21222'
file_name: 2026_AppliedEnergyMaterials_Busato.pdf
file_size: 5977526
relation: main_file
success: 1
file_date_updated: 2026-02-12T13:55:28Z
has_accepted_license: '1'
intvolume: ' 9'
issue: '1'
language:
- iso: eng
license: https://creativecommons.org/licenses/by/4.0/
month: '01'
oa: 1
oa_version: Published Version
page: 686-697
publication: ACS Applied Energy Materials
publication_identifier:
eissn:
- 2574-0962
publication_status: published
publisher: American Chemical Society
quality_controlled: '1'
scopus_import: '1'
status: public
title: Structural rearrangements of a Cobalt-free Lithium-rich layered oxide cathode
during formation
tmp:
image: /images/cc_by.png
legal_code_url: https://creativecommons.org/licenses/by/4.0/legalcode
name: Creative Commons Attribution 4.0 International Public License (CC-BY 4.0)
short: CC BY (4.0)
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 9
year: '2026'
...
---
OA_type: closed access
_id: '21730'
abstract:
- lang: eng
text: Hydrogen peroxide (H2O2) is a crucial member of the reactive oxygen species
(ROS) family, playing roles in cellular signalling and immune responses in human
health. Moreover, it is a potential biomarker of diabetes when present in aberrant
concentrations. Therefore, monitoring trace levels of H2O2 has become a research
hotspot for analytical and sensor chemists. In this context, we report a rhodamine-based
fluorescent probe (RN), which shows excellent fluorescent enhancement at 555 nm
upon the addition of H2O2 along with a low limit of detection (LOD) of 0.67 ppm
and fast response (∼2 min). The probe is highly selective for H2O2, showing no
fluorescence enhancement with other ROS. RN is synthesised in a one-pot chemical
reaction using rhodamine 6G (R6G) and 4,7,10-trioxa-1,13-tridecanediamine (TTDA).
H2O2 detection in pre-treated milk samples proves its real-world viability. We
found that RN shows low cytotoxicity, which allowed us to successfully explore
its potential to monitor H2O2 generation in a diabetic L929 skin cell line and
diabetic mice liver tissue. This result demonstrates promising features for assessing
early diabetic progression through fluorescence imaging.
acknowledged_ssus:
- _id: LifeSc
acknowledgement: "MM acknowledges the Government of India for DST-INSPIRE\r\nfellowship
[IF200389] and Federal Ministry of Education, Science and Research (BMBWF) and the
OeAD – Austria’s Agency for Education and Internationalisation for an Ernst Mach
Grant, weltweit (grant number MPC-2024-01518) for research internship at ISTA. The
Scientific Service Units of ISTA supported this research through resources provided
by the Lab Support Facility. PG acknowledges the ANRF, India, for his NPDF fellowship
(File no. PDF/2022/001960). PB acknowledges ANRF, India, for the SERB-CRG sponsored
project GAP-240712 (vide reference no. CRG/2022/001679)."
article_processing_charge: No
article_type: original
author:
- first_name: Moumita
full_name: Mondal, Moumita
last_name: Mondal
- first_name: Pravat
full_name: Ghorai, Pravat
last_name: Ghorai
- first_name: Asmita
full_name: Samadder, Asmita
last_name: Samadder
- first_name: Stefan Alexander
full_name: Freunberger, Stefan Alexander
id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425
last_name: Freunberger
orcid: 0000-0003-2902-5319
- first_name: Priyabrata
full_name: Banerjee, Priyabrata
last_name: Banerjee
citation:
ama: Mondal M, Ghorai P, Samadder A, Freunberger SA, Banerjee P. H2O2 responsive
rhodamine-based probe for monitoring early-stage diabetes diagnosis. Journal
of Materials Chemistry B. 2026. doi:10.1039/d5tb02687c
apa: Mondal, M., Ghorai, P., Samadder, A., Freunberger, S. A., & Banerjee, P.
(2026). H2O2 responsive rhodamine-based probe for monitoring early-stage diabetes
diagnosis. Journal of Materials Chemistry B. Royal Society of Chemistry.
https://doi.org/10.1039/d5tb02687c
chicago: Mondal, Moumita, Pravat Ghorai, Asmita Samadder, Stefan Alexander Freunberger,
and Priyabrata Banerjee. “H2O2 Responsive Rhodamine-Based Probe for Monitoring
Early-Stage Diabetes Diagnosis.” Journal of Materials Chemistry B. Royal
Society of Chemistry, 2026. https://doi.org/10.1039/d5tb02687c.
ieee: M. Mondal, P. Ghorai, A. Samadder, S. A. Freunberger, and P. Banerjee, “H2O2
responsive rhodamine-based probe for monitoring early-stage diabetes diagnosis,”
Journal of Materials Chemistry B. Royal Society of Chemistry, 2026.
ista: Mondal M, Ghorai P, Samadder A, Freunberger SA, Banerjee P. 2026. H2O2 responsive
rhodamine-based probe for monitoring early-stage diabetes diagnosis. Journal of
Materials Chemistry B.
mla: Mondal, Moumita, et al. “H2O2 Responsive Rhodamine-Based Probe for Monitoring
Early-Stage Diabetes Diagnosis.” Journal of Materials Chemistry B, Royal
Society of Chemistry, 2026, doi:10.1039/d5tb02687c.
short: M. Mondal, P. Ghorai, A. Samadder, S.A. Freunberger, P. Banerjee, Journal
of Materials Chemistry B (2026).
corr_author: '1'
date_created: 2026-04-13T07:45:26Z
date_published: 2026-04-10T00:00:00Z
date_updated: 2026-04-16T05:44:49Z
day: '10'
department:
- _id: StFr
doi: 10.1039/d5tb02687c
external_id:
pmid:
- '41958432'
language:
- iso: eng
month: '04'
oa_version: None
pmid: 1
publication: Journal of Materials Chemistry B
publication_identifier:
eissn:
- 2050-7518
issn:
- 2050-750X
publication_status: epub_ahead
publisher: Royal Society of Chemistry
quality_controlled: '1'
scopus_import: '1'
status: public
title: H2O2 responsive rhodamine-based probe for monitoring early-stage diabetes diagnosis
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
year: '2026'
...
---
OA_place: publisher
OA_type: hybrid
PlanS_conform: '1'
_id: '20593'
abstract:
- lang: eng
text: “Quasi-solid-state” conversion mechanisms using sparingly solvating electrolytes
(SPSEs) bridge the gap between traditional solid–liquid–solid and solid-state
sulfur conversion in lithium–sulfur (Li–S) batteries. Although these terms are
commonly used, their precise distinctions and impacts on key performance metrics,
such as rate capability, energy density, and capacity fading, remain poorly understood.
In this work, we employ operando small- and wide-angle X-ray scattering alongside
cryogenic transmission electron microscopy (cryo-TEM) to compare Li–S batteries
in sparingly solvating and solvating ether-based electrolytes. We find that, unlike
solvating electrolytes, SPSEs lead to an extended presence of lithium sulfide
during cycling, coexisting with sulfur at a 50% state of charge and beyond. In
the charged state, solid sulfur is present in its amorphous form inside the carbon
black nanopores. These findings indicate that the limited solubility confines
polysulfides in regions near the carbon surface, where these polysulfides enable
conversion between the coexisting solid discharge and charge product.
acknowledgement: This work was funded by the European Union (ERC-2022-STG, SOLIDCON,
101078271). Views and opinions expressed are, however, those of the authors only
and do not necessarily reflect those of the European Union or the European Research
Council Executive Agency. Neither the European Union nor the granting authority
can be held responsible for them. TEM measurements were carried out on a JEOL JEM
F200 TEM equipped with an energy filter funded by the FFG (grant number 37120633).
The authors thank Klara Neumayr, Ayca Senol Güngör, and Lorenz Gruber for valuable
discussions and support with lab work. N.K. thanks Oskar Paris from Montanuniversität
Leoben for providing access to the gas sorption analyzer.
article_processing_charge: Yes (in subscription journal)
article_type: letter_note
author:
- first_name: Pronoy
full_name: Dutta, Pronoy
last_name: Dutta
- first_name: Jean Marc
full_name: Von Mentlen, Jean Marc
last_name: Von Mentlen
- first_name: Soumyadip
full_name: Mondal, Soumyadip
id: d25d21ef-dc8d-11ea-abe3-ec4576307f48
last_name: Mondal
- first_name: Nikolaos
full_name: Kostoglou, Nikolaos
last_name: Kostoglou
- first_name: Bodo D.
full_name: Wilts, Bodo D.
last_name: Wilts
- first_name: Stefan Alexander
full_name: Freunberger, Stefan Alexander
id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425
last_name: Freunberger
orcid: 0000-0003-2902-5319
- first_name: Gregor A.
full_name: Zickler, Gregor A.
last_name: Zickler
- first_name: Christian
full_name: Prehal, Christian
last_name: Prehal
citation:
ama: 'Dutta P, Von Mentlen JM, Mondal S, et al. Bridging solution and solid-state
mechanism: Confined quasi-solid-state conversion in Li–S batteries. ACS Energy
Letters. 2025;10:5722-5732. doi:10.1021/acsenergylett.5c02093'
apa: 'Dutta, P., Von Mentlen, J. M., Mondal, S., Kostoglou, N., Wilts, B. D., Freunberger,
S. A., … Prehal, C. (2025). Bridging solution and solid-state mechanism: Confined
quasi-solid-state conversion in Li–S batteries. ACS Energy Letters. American
Chemical Society. https://doi.org/10.1021/acsenergylett.5c02093'
chicago: 'Dutta, Pronoy, Jean Marc Von Mentlen, Soumyadip Mondal, Nikolaos Kostoglou,
Bodo D. Wilts, Stefan Alexander Freunberger, Gregor A. Zickler, and Christian
Prehal. “Bridging Solution and Solid-State Mechanism: Confined Quasi-Solid-State
Conversion in Li–S Batteries.” ACS Energy Letters. American Chemical Society,
2025. https://doi.org/10.1021/acsenergylett.5c02093.'
ieee: 'P. Dutta et al., “Bridging solution and solid-state mechanism: Confined
quasi-solid-state conversion in Li–S batteries,” ACS Energy Letters, vol.
10. American Chemical Society, pp. 5722–5732, 2025.'
ista: 'Dutta P, Von Mentlen JM, Mondal S, Kostoglou N, Wilts BD, Freunberger SA,
Zickler GA, Prehal C. 2025. Bridging solution and solid-state mechanism: Confined
quasi-solid-state conversion in Li–S batteries. ACS Energy Letters. 10, 5722–5732.'
mla: 'Dutta, Pronoy, et al. “Bridging Solution and Solid-State Mechanism: Confined
Quasi-Solid-State Conversion in Li–S Batteries.” ACS Energy Letters, vol.
10, American Chemical Society, 2025, pp. 5722–32, doi:10.1021/acsenergylett.5c02093.'
short: P. Dutta, J.M. Von Mentlen, S. Mondal, N. Kostoglou, B.D. Wilts, S.A. Freunberger,
G.A. Zickler, C. Prehal, ACS Energy Letters 10 (2025) 5722–5732.
date_created: 2025-11-02T23:01:35Z
date_published: 2025-10-25T00:00:00Z
date_updated: 2025-12-01T15:11:44Z
day: '25'
ddc:
- '540'
department:
- _id: StFr
doi: 10.1021/acsenergylett.5c02093
external_id:
isi:
- '001600396000001'
file:
- access_level: open_access
checksum: 368eb041c395a5155218f858947df419
content_type: application/pdf
creator: dernst
date_created: 2025-11-04T07:56:19Z
date_updated: 2025-11-04T07:56:19Z
file_id: '20597'
file_name: 2025_ACSEnergyLetters_Dutta.pdf
file_size: 9307654
relation: main_file
success: 1
file_date_updated: 2025-11-04T07:56:19Z
has_accepted_license: '1'
intvolume: ' 10'
isi: 1
language:
- iso: eng
month: '10'
oa: 1
oa_version: Published Version
page: 5722-5732
publication: ACS Energy Letters
publication_identifier:
eissn:
- 2380-8195
publication_status: published
publisher: American Chemical Society
quality_controlled: '1'
related_material:
link:
- relation: software
url: ' https://doi.org/10.5281/zenodo.17144229'
scopus_import: '1'
status: public
title: 'Bridging solution and solid-state mechanism: Confined quasi-solid-state conversion
in Li–S batteries'
tmp:
image: /images/cc_by.png
legal_code_url: https://creativecommons.org/licenses/by/4.0/legalcode
name: Creative Commons Attribution 4.0 International Public License (CC-BY 4.0)
short: CC BY (4.0)
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 10
year: '2025'
...
---
OA_place: publisher
OA_type: hybrid
PlanS_conform: '1'
_id: '17468'
abstract:
- lang: eng
text: Oxygen redox chemistry is central to life1 and many human-made technologies,
such as in energy storage2,3,4. The large energy gain from oxygen redox reactions
is often connected with the occurrence of harmful reactive oxygen species3,5,6.
Key species are superoxide and the highly reactive singlet oxygen3,4,5,6,7, which
may evolve from superoxide. However, the factors determining the formation of
singlet oxygen, rather than the relatively unreactive triplet oxygen, are unknown.
Here we report that the release of triplet or singlet oxygen is governed by individual
Marcus normal and inverted region behaviour. We found that as the driving force
for the reaction increases, the initially dominant evolution of triplet oxygen
slows down, and singlet oxygen evolution becomes predominant with higher maximum
kinetics. This behaviour also applies to the widely observed superoxide disproportionation,
in which one superoxide is oxidized by another, in both non-aqueous and aqueous
systems, with Lewis and Brønsted acidity controlling the driving forces. Singlet
oxygen yields governed by these conditions are relevant, for example, in batteries
or cellular organelles in which superoxide forms. Our findings suggest ways to
understand and control spin states and kinetics in oxygen redox chemistry, with
implications for fields, including life sciences, pure chemistry and energy storage.
acknowledged_ssus:
- _id: Bio
- _id: LifeSc
- _id: M-Shop
- _id: ScienComp
acknowledgement: S.A.F. thanks the Institute of Science and Technology Austria (ISTA)
for the support. The Scientific Service Units of ISTA supported this research through
resources provided by the Imaging and Optics Facility, the Lab Support Facility,
the Miba Machine Shop and Scientific Computing. This research was partly funded
by the Austrian Science Fund (FWF) (10.55776/P37169 and 10.55776/COE5). For open
access purposes, the author has applied for a CC BY public copyright licence to
any author-accepted manuscript version arising from this submission. R.H. acknowledges
funding through CZI grant DAF2020-225401 (10.37921/120055ratwvi) from the Chan Zuckerberg
Initiative DAF, an advised fund of Silicon Valley Community Foundation (10.13039/100014989).
H.T.K.N. acknowledges funding by the European Commission Erasmus Mundus Joint Masters
programme. We thank M. Sixt and M. Chinon for the discussions about O-redox in life
and R. Jethwa for proofreading. Open access funding was provided by ISTA.
article_processing_charge: Yes (via OA deal)
article_type: original
author:
- first_name: Soumyadip
full_name: Mondal, Soumyadip
id: d25d21ef-dc8d-11ea-abe3-ec4576307f48
last_name: Mondal
- first_name: Huyen T.K.
full_name: Nguyen, Huyen T.K.
last_name: Nguyen
- first_name: Robert
full_name: Hauschild, Robert
id: 4E01D6B4-F248-11E8-B48F-1D18A9856A87
last_name: Hauschild
orcid: 0000-0001-9843-3522
- first_name: Stefan Alexander
full_name: Freunberger, Stefan Alexander
id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425
last_name: Freunberger
orcid: 0000-0003-2902-5319
citation:
ama: Mondal S, Nguyen HTK, Hauschild R, Freunberger SA. Marcus kinetics control
singlet and triplet oxygen evolving from superoxide. Nature. 2025;646(8085):601–605.
doi:10.1038/s41586-025-09587-7
apa: Mondal, S., Nguyen, H. T. K., Hauschild, R., & Freunberger, S. A. (2025).
Marcus kinetics control singlet and triplet oxygen evolving from superoxide. Nature.
Springer Nature. https://doi.org/10.1038/s41586-025-09587-7
chicago: Mondal, Soumyadip, Huyen T.K. Nguyen, Robert Hauschild, and Stefan Alexander
Freunberger. “Marcus Kinetics Control Singlet and Triplet Oxygen Evolving from
Superoxide.” Nature. Springer Nature, 2025. https://doi.org/10.1038/s41586-025-09587-7.
ieee: S. Mondal, H. T. K. Nguyen, R. Hauschild, and S. A. Freunberger, “Marcus kinetics
control singlet and triplet oxygen evolving from superoxide,” Nature, vol.
646, no. 8085. Springer Nature, pp. 601–605, 2025.
ista: Mondal S, Nguyen HTK, Hauschild R, Freunberger SA. 2025. Marcus kinetics control
singlet and triplet oxygen evolving from superoxide. Nature. 646(8085), 601–605.
mla: Mondal, Soumyadip, et al. “Marcus Kinetics Control Singlet and Triplet Oxygen
Evolving from Superoxide.” Nature, vol. 646, no. 8085, Springer Nature,
2025, pp. 601–605, doi:10.1038/s41586-025-09587-7.
short: S. Mondal, H.T.K. Nguyen, R. Hauschild, S.A. Freunberger, Nature 646 (2025)
601–605.
corr_author: '1'
date_created: 2024-08-29T10:40:23Z
date_published: 2025-10-16T00:00:00Z
date_updated: 2026-04-28T13:18:33Z
day: '16'
ddc:
- '540'
department:
- _id: StFr
- _id: Bio
doi: 10.1038/s41586-025-09587-7
external_id:
isi:
- '001586378900001'
pmid:
- '41044415'
file:
- access_level: open_access
checksum: b507ddd23df0388aa65d04dc9b00fe3d
content_type: application/pdf
creator: dernst
date_created: 2025-10-20T10:26:13Z
date_updated: 2025-10-20T10:26:13Z
file_id: '20500'
file_name: 2025_Nature_Mondal.pdf
file_size: 3809247
relation: main_file
success: 1
file_date_updated: 2025-10-20T10:26:13Z
has_accepted_license: '1'
intvolume: ' 646'
isi: 1
issue: '8085'
language:
- iso: eng
month: '10'
oa: 1
oa_version: Published Version
page: 601–605
pmid: 1
project:
- _id: 8df062be-16d5-11f0-9cad-f559b6612c7e
grant_number: P37169
name: Singlet oxygen in non-aqueous oxygen redox chemistry
- _id: c08e9ad1-5a5b-11eb-8a69-9d1cf3b07473
grant_number: CZI01
name: Tools for automation and feedback microscopy
publication: Nature
publication_identifier:
eissn:
- 1476-4687
issn:
- 0028-0836
publication_status: published
publisher: Springer Nature
quality_controlled: '1'
related_material:
link:
- description: News on ISTA website
relation: press_release
url: https://ista.ac.at/en/news/taming-the-bad-oxygen/
scopus_import: '1'
status: public
title: Marcus kinetics control singlet and triplet oxygen evolving from superoxide
tmp:
image: /images/cc_by.png
legal_code_url: https://creativecommons.org/licenses/by/4.0/legalcode
name: Creative Commons Attribution 4.0 International Public License (CC-BY 4.0)
short: CC BY (4.0)
type: journal_article
user_id: ba8df636-2132-11f1-aed0-ed93e2281fdd
volume: 646
year: '2025'
...
---
_id: '14701'
article_processing_charge: No
article_type: letter_note
author:
- first_name: Lynden A.
full_name: Archer, Lynden A.
last_name: Archer
- first_name: Peter G.
full_name: Bruce, Peter G.
last_name: Bruce
- first_name: Ernesto J.
full_name: Calvo, Ernesto J.
last_name: Calvo
- first_name: Daniel
full_name: Dewar, Daniel
last_name: Dewar
- first_name: James H. J.
full_name: Ellison, James H. J.
last_name: Ellison
- first_name: Stefan Alexander
full_name: Freunberger, Stefan Alexander
id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425
last_name: Freunberger
orcid: 0000-0003-2902-5319
- first_name: Xiangwen
full_name: Gao, Xiangwen
last_name: Gao
- first_name: Laurence J.
full_name: Hardwick, Laurence J.
last_name: Hardwick
- first_name: Gabriela
full_name: Horwitz, Gabriela
last_name: Horwitz
- first_name: Jürgen
full_name: Janek, Jürgen
last_name: Janek
- first_name: Lee R.
full_name: Johnson, Lee R.
last_name: Johnson
- first_name: Jack W.
full_name: Jordan, Jack W.
last_name: Jordan
- first_name: Shoichi
full_name: Matsuda, Shoichi
last_name: Matsuda
- first_name: Svetlana
full_name: Menkin, Svetlana
last_name: Menkin
- first_name: Soumyadip
full_name: Mondal, Soumyadip
id: d25d21ef-dc8d-11ea-abe3-ec4576307f48
last_name: Mondal
- first_name: Qianyuan
full_name: Qiu, Qianyuan
last_name: Qiu
- first_name: Thukshan
full_name: Samarakoon, Thukshan
last_name: Samarakoon
- first_name: Israel
full_name: Temprano, Israel
last_name: Temprano
- first_name: Kohei
full_name: Uosaki, Kohei
last_name: Uosaki
- first_name: Ganesh
full_name: Vailaya, Ganesh
last_name: Vailaya
- first_name: Eric D.
full_name: Wachsman, Eric D.
last_name: Wachsman
- first_name: Yiying
full_name: Wu, Yiying
last_name: Wu
- first_name: Shen
full_name: Ye, Shen
last_name: Ye
citation:
ama: 'Archer LA, Bruce PG, Calvo EJ, et al. Towards practical metal–oxygen batteries:
General discussion. Faraday Discussions. 2024;248:392-411. doi:10.1039/d3fd90062b'
apa: 'Archer, L. A., Bruce, P. G., Calvo, E. J., Dewar, D., Ellison, J. H. J., Freunberger,
S. A., … Ye, S. (2024). Towards practical metal–oxygen batteries: General discussion.
Faraday Discussions. Royal Society of Chemistry. https://doi.org/10.1039/d3fd90062b'
chicago: 'Archer, Lynden A., Peter G. Bruce, Ernesto J. Calvo, Daniel Dewar, James
H. J. Ellison, Stefan Alexander Freunberger, Xiangwen Gao, et al. “Towards Practical
Metal–Oxygen Batteries: General Discussion.” Faraday Discussions. Royal
Society of Chemistry, 2024. https://doi.org/10.1039/d3fd90062b.'
ieee: 'L. A. Archer et al., “Towards practical metal–oxygen batteries: General
discussion,” Faraday Discussions, vol. 248. Royal Society of Chemistry,
pp. 392–411, 2024.'
ista: 'Archer LA, Bruce PG, Calvo EJ, Dewar D, Ellison JHJ, Freunberger SA, Gao
X, Hardwick LJ, Horwitz G, Janek J, Johnson LR, Jordan JW, Matsuda S, Menkin S,
Mondal S, Qiu Q, Samarakoon T, Temprano I, Uosaki K, Vailaya G, Wachsman ED, Wu
Y, Ye S. 2024. Towards practical metal–oxygen batteries: General discussion. Faraday
Discussions. 248, 392–411.'
mla: 'Archer, Lynden A., et al. “Towards Practical Metal–Oxygen Batteries: General
Discussion.” Faraday Discussions, vol. 248, Royal Society of Chemistry,
2024, pp. 392–411, doi:10.1039/d3fd90062b.'
short: L.A. Archer, P.G. Bruce, E.J. Calvo, D. Dewar, J.H.J. Ellison, S.A. Freunberger,
X. Gao, L.J. Hardwick, G. Horwitz, J. Janek, L.R. Johnson, J.W. Jordan, S. Matsuda,
S. Menkin, S. Mondal, Q. Qiu, T. Samarakoon, I. Temprano, K. Uosaki, G. Vailaya,
E.D. Wachsman, Y. Wu, S. Ye, Faraday Discussions 248 (2024) 392–411.
date_created: 2023-12-20T10:48:09Z
date_published: 2024-01-29T00:00:00Z
date_updated: 2025-09-04T11:34:30Z
day: '29'
department:
- _id: StFr
doi: 10.1039/d3fd90062b
external_id:
isi:
- '001130090400001'
pmid:
- '38112202'
intvolume: ' 248'
isi: 1
keyword:
- Physical and Theoretical Chemistry
language:
- iso: eng
month: '01'
oa_version: None
page: 392-411
pmid: 1
publication: Faraday Discussions
publication_identifier:
eissn:
- 1364-5498
issn:
- 1359-6640
publication_status: published
publisher: Royal Society of Chemistry
quality_controlled: '1'
scopus_import: '1'
status: public
title: 'Towards practical metal–oxygen batteries: General discussion'
type: journal_article
user_id: 317138e5-6ab7-11ef-aa6d-ffef3953e345
volume: 248
year: '2024'
...
---
_id: '17333'
abstract:
- lang: eng
text: Aqueous zinc-ion batteries are attractive due to their low cost, environmental
friendliness, and exceptional performance, but the latter remains poorly understood.
Now, a fast catalytic step involved in oxygen redox catalysis is shown to contribute
to capacity at a high rate.
article_processing_charge: No
article_type: letter_note
author:
- first_name: Soumyadip
full_name: Mondal, Soumyadip
id: d25d21ef-dc8d-11ea-abe3-ec4576307f48
last_name: Mondal
- first_name: Stefan Alexander
full_name: Freunberger, Stefan Alexander
id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425
last_name: Freunberger
orcid: 0000-0003-2902-5319
citation:
ama: Mondal S, Freunberger SA. Catalysing rate and capacity. Nature Catalysis.
2024;7(7):759-760. doi:10.1038/s41929-024-01184-7
apa: Mondal, S., & Freunberger, S. A. (2024). Catalysing rate and capacity.
Nature Catalysis. Springer Nature. https://doi.org/10.1038/s41929-024-01184-7
chicago: Mondal, Soumyadip, and Stefan Alexander Freunberger. “Catalysing Rate and
Capacity.” Nature Catalysis. Springer Nature, 2024. https://doi.org/10.1038/s41929-024-01184-7.
ieee: S. Mondal and S. A. Freunberger, “Catalysing rate and capacity,” Nature
Catalysis, vol. 7, no. 7. Springer Nature, pp. 759–760, 2024.
ista: Mondal S, Freunberger SA. 2024. Catalysing rate and capacity. Nature Catalysis.
7(7), 759–760.
mla: Mondal, Soumyadip, and Stefan Alexander Freunberger. “Catalysing Rate and Capacity.”
Nature Catalysis, vol. 7, no. 7, Springer Nature, 2024, pp. 759–60, doi:10.1038/s41929-024-01184-7.
short: S. Mondal, S.A. Freunberger, Nature Catalysis 7 (2024) 759–760.
corr_author: '1'
date_created: 2024-07-29T07:05:33Z
date_published: 2024-07-26T00:00:00Z
date_updated: 2025-09-08T08:30:59Z
day: '26'
department:
- _id: StFr
doi: 10.1038/s41929-024-01184-7
external_id:
isi:
- '001278986700012'
intvolume: ' 7'
isi: 1
issue: '7'
language:
- iso: eng
month: '07'
oa_version: None
page: 759-760
publication: Nature Catalysis
publication_identifier:
issn:
- 2520-1158
publication_status: published
publisher: Springer Nature
quality_controlled: '1'
scopus_import: '1'
status: public
title: Catalysing rate and capacity
type: journal_article
user_id: 317138e5-6ab7-11ef-aa6d-ffef3953e345
volume: 7
year: '2024'
...
---
_id: '14687'
abstract:
- lang: eng
text: The short history of research on Li-O2 batteries has seen a remarkable number
of mechanistic U-turns over the years. From the initial use of carbonate electrolytes,
that were then found to be entirely unsuitable, to the belief that (su)peroxide
was solely responsible for degradation, before the more reactive singlet oxygen
was found to form, to the hypothesis that capacity depends on a competing surface/solution
mechanism before a practically exclusive solution mechanism was identified. Herein,
we argue for an ever-fresh look at the reported data without bias towards supposedly
established explanations. We explain how the latest findings on rate and capacity
limits, as well as the origin of side reactions, are connected via the disproportionation
(DISP) step in the (dis)charge mechanism. Therefrom, directions emerge for the
design of electrolytes and mediators on how to suppress side reactions and to
enable high rate and high reversible capacity.
acknowledgement: S.A.F. is indebted to ISTA for support. R.B.J. thanks the European
Union's Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie
grant agreement No 101034413 for funding. B.P. thanks Alistore ERI for providing
a PhD scholarship.
article_number: e202316476
article_processing_charge: Yes (via OA deal)
article_type: review
author:
- first_name: Rajesh B
full_name: Jethwa, Rajesh B
id: 4cc538d5-803f-11ed-ab7e-8139573aad8f
last_name: Jethwa
orcid: 0000-0002-0404-4356
- first_name: Soumyadip
full_name: Mondal, Soumyadip
id: d25d21ef-dc8d-11ea-abe3-ec4576307f48
last_name: Mondal
- first_name: Bhargavi
full_name: Pant, Bhargavi
id: 50c64d4d-eb97-11eb-a6c2-d33e5e14f112
last_name: Pant
- first_name: Stefan Alexander
full_name: Freunberger, Stefan Alexander
id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425
last_name: Freunberger
orcid: 0000-0003-2902-5319
citation:
ama: Jethwa RB, Mondal S, Pant B, Freunberger SA. To DISP or not? The far‐reaching
reaction mechanisms underpinning Lithium‐air batteries. Angewandte Chemie International
Edition. 2024;63(28). doi:10.1002/anie.202316476
apa: Jethwa, R. B., Mondal, S., Pant, B., & Freunberger, S. A. (2024). To DISP
or not? The far‐reaching reaction mechanisms underpinning Lithium‐air batteries.
Angewandte Chemie International Edition. Wiley. https://doi.org/10.1002/anie.202316476
chicago: Jethwa, Rajesh B, Soumyadip Mondal, Bhargavi Pant, and Stefan Alexander
Freunberger. “To DISP or Not? The Far‐reaching Reaction Mechanisms Underpinning
Lithium‐air Batteries.” Angewandte Chemie International Edition. Wiley,
2024. https://doi.org/10.1002/anie.202316476.
ieee: R. B. Jethwa, S. Mondal, B. Pant, and S. A. Freunberger, “To DISP or not?
The far‐reaching reaction mechanisms underpinning Lithium‐air batteries,” Angewandte
Chemie International Edition, vol. 63, no. 28. Wiley, 2024.
ista: Jethwa RB, Mondal S, Pant B, Freunberger SA. 2024. To DISP or not? The far‐reaching
reaction mechanisms underpinning Lithium‐air batteries. Angewandte Chemie International
Edition. 63(28), e202316476.
mla: Jethwa, Rajesh B., et al. “To DISP or Not? The Far‐reaching Reaction Mechanisms
Underpinning Lithium‐air Batteries.” Angewandte Chemie International Edition,
vol. 63, no. 28, e202316476, Wiley, 2024, doi:10.1002/anie.202316476.
short: R.B. Jethwa, S. Mondal, B. Pant, S.A. Freunberger, Angewandte Chemie International
Edition 63 (2024).
corr_author: '1'
date_created: 2023-12-15T16:10:13Z
date_published: 2024-07-08T00:00:00Z
date_updated: 2026-04-07T12:27:23Z
day: '08'
ddc:
- '540'
department:
- _id: StFr
- _id: GradSch
doi: 10.1002/anie.202316476
ec_funded: 1
external_id:
isi:
- '001241932700001'
pmid:
- '38095355'
file:
- access_level: open_access
checksum: fe2c23454279eb9d76ed6ca9970c21c7
content_type: application/pdf
creator: dernst
date_created: 2024-07-16T11:54:46Z
date_updated: 2024-07-16T11:54:46Z
file_id: '17261'
file_name: 2024_AngChemieInt_Jethwa.pdf
file_size: 4766445
relation: main_file
success: 1
file_date_updated: 2024-07-16T11:54:46Z
has_accepted_license: '1'
intvolume: ' 63'
isi: 1
issue: '28'
keyword:
- General Chemistry
- Catalysis
language:
- iso: eng
license: https://creativecommons.org/licenses/by-nc-nd/4.0/
month: '07'
oa: 1
oa_version: Published Version
pmid: 1
project:
- _id: fc2ed2f7-9c52-11eb-aca3-c01059dda49c
call_identifier: H2020
grant_number: '101034413'
name: 'IST-BRIDGE: International postdoctoral program'
publication: Angewandte Chemie International Edition
publication_identifier:
eissn:
- 1521-3773
issn:
- 1433-7851
publication_status: published
publisher: Wiley
quality_controlled: '1'
related_material:
record:
- id: '20607'
relation: dissertation_contains
status: public
scopus_import: '1'
status: public
title: To DISP or not? The far‐reaching reaction mechanisms underpinning Lithium‐air
batteries
tmp:
image: /images/cc_by_nc_nd.png
legal_code_url: https://creativecommons.org/licenses/by-nc-nd/4.0/legalcode
name: Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International
(CC BY-NC-ND 4.0)
short: CC BY-NC-ND (4.0)
type: journal_article
user_id: 317138e5-6ab7-11ef-aa6d-ffef3953e345
volume: 63
year: '2024'
...
---
_id: '13044'
abstract:
- lang: eng
text: Singlet oxygen (1O2) formation is now recognised as a key aspect of non-aqueous
oxygen redox chemistry. For identifying 1O2, chemical trapping via 9,10-dimethylanthracene
(DMA) to form the endoperoxide (DMA-O2) has become the mainstay method due to
its sensitivity, selectivity, and ease of use. While DMA has been shown to be
selective for 1O2, rather than forming DMA-O2 with a wide variety of potentially
reactive O-containing species, false positives might hypothetically be obtained
in the presence of previously overlooked species. Here, we first give unequivocal
direct spectroscopic proof by the 1O2-specific near infrared (NIR) emission at
1270 nm for the previously proposed 1O2 formation pathways, which centre around
superoxide disproportionation. We then show that peroxocarbonates, common intermediates
in metal-O2 and metal carbonate electrochemistry, do not produce false-positive
DMA-O2. Moreover, we identify a previously unreported 1O2-forming pathway through
the reaction of CO2 with superoxide. Overall, we give unequivocal proof for 1O2
formation in non-aqueous oxygen redox and show that chemical trapping with DMA
is a reliable method to assess 1O2 formation.
article_processing_charge: Yes (via OA deal)
article_type: original
author:
- first_name: Soumyadip
full_name: Mondal, Soumyadip
id: d25d21ef-dc8d-11ea-abe3-ec4576307f48
last_name: Mondal
- first_name: Rajesh B
full_name: Jethwa, Rajesh B
id: 4cc538d5-803f-11ed-ab7e-8139573aad8f
last_name: Jethwa
orcid: 0000-0002-0404-4356
- first_name: Bhargavi
full_name: Pant, Bhargavi
id: 50c64d4d-eb97-11eb-a6c2-d33e5e14f112
last_name: Pant
- first_name: Robert
full_name: Hauschild, Robert
id: 4E01D6B4-F248-11E8-B48F-1D18A9856A87
last_name: Hauschild
orcid: 0000-0001-9843-3522
- first_name: Stefan Alexander
full_name: Freunberger, Stefan Alexander
id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425
last_name: Freunberger
orcid: 0000-0003-2902-5319
citation:
ama: 'Mondal S, Jethwa RB, Pant B, Hauschild R, Freunberger SA. Singlet oxygen in
non-aqueous oxygen redox: Direct spectroscopic evidence for formation pathways
and reliability of chemical probes. Faraday Discussions. 2024;248:175-189.
doi:10.1039/d3fd00088e'
apa: 'Mondal, S., Jethwa, R. B., Pant, B., Hauschild, R., & Freunberger, S.
A. (2024). Singlet oxygen in non-aqueous oxygen redox: Direct spectroscopic evidence
for formation pathways and reliability of chemical probes. Faraday Discussions.
Royal Society of Chemistry. https://doi.org/10.1039/d3fd00088e'
chicago: 'Mondal, Soumyadip, Rajesh B Jethwa, Bhargavi Pant, Robert Hauschild, and
Stefan Alexander Freunberger. “Singlet Oxygen in Non-Aqueous Oxygen Redox: Direct
Spectroscopic Evidence for Formation Pathways and Reliability of Chemical Probes.”
Faraday Discussions. Royal Society of Chemistry, 2024. https://doi.org/10.1039/d3fd00088e.'
ieee: 'S. Mondal, R. B. Jethwa, B. Pant, R. Hauschild, and S. A. Freunberger, “Singlet
oxygen in non-aqueous oxygen redox: Direct spectroscopic evidence for formation
pathways and reliability of chemical probes,” Faraday Discussions, vol.
248. Royal Society of Chemistry, pp. 175–189, 2024.'
ista: 'Mondal S, Jethwa RB, Pant B, Hauschild R, Freunberger SA. 2024. Singlet oxygen
in non-aqueous oxygen redox: Direct spectroscopic evidence for formation pathways
and reliability of chemical probes. Faraday Discussions. 248, 175–189.'
mla: 'Mondal, Soumyadip, et al. “Singlet Oxygen in Non-Aqueous Oxygen Redox: Direct
Spectroscopic Evidence for Formation Pathways and Reliability of Chemical Probes.”
Faraday Discussions, vol. 248, Royal Society of Chemistry, 2024, pp. 175–89,
doi:10.1039/d3fd00088e.'
short: S. Mondal, R.B. Jethwa, B. Pant, R. Hauschild, S.A. Freunberger, Faraday
Discussions 248 (2024) 175–189.
corr_author: '1'
date_created: 2023-05-22T06:53:34Z
date_published: 2024-01-01T00:00:00Z
date_updated: 2026-04-07T12:27:23Z
day: '01'
ddc:
- '540'
department:
- _id: StFr
- _id: Bio
doi: 10.1039/d3fd00088e
external_id:
isi:
- '001070423500001'
pmid:
- '37750344'
file:
- access_level: open_access
checksum: 6515a227ed3e8942496fe6a1feeffd18
content_type: application/pdf
creator: dernst
date_created: 2024-07-16T07:46:39Z
date_updated: 2024-07-16T07:46:39Z
file_id: '17249'
file_name: 2024_FaradayDiscussions_Mondal.pdf
file_size: 1303733
relation: main_file
success: 1
file_date_updated: 2024-07-16T07:46:39Z
has_accepted_license: '1'
intvolume: ' 248'
isi: 1
keyword:
- Physical and Theoretical Chemistry
language:
- iso: eng
license: https://creativecommons.org/licenses/by-nc/3.0/
month: '01'
oa: 1
oa_version: Published Version
page: 175-189
pmid: 1
publication: Faraday Discussions
publication_identifier:
eissn:
- 1364-5498
issn:
- 1359-6640
publication_status: published
publisher: Royal Society of Chemistry
quality_controlled: '1'
related_material:
record:
- id: '20607'
relation: dissertation_contains
status: public
scopus_import: '1'
status: public
title: 'Singlet oxygen in non-aqueous oxygen redox: Direct spectroscopic evidence
for formation pathways and reliability of chemical probes'
tmp:
image: /images/cc_by_nc.png
legal_code_url: https://creativecommons.org/licenses/by-nc/3.0/legalcode
name: Creative Commons Attribution-NonCommercial 3.0 Unported (CC BY-NC 3.0)
short: CC BY-NC (3.0)
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 248
year: '2024'
...
---
_id: '12208'
abstract:
- lang: eng
text: The inadequate understanding of the mechanisms that reversibly convert molecular
sulfur (S) into lithium sulfide (Li2S) via soluble polysulfides
(PSs) formation impedes the development of high-performance lithium-sulfur (Li-S)
batteries with non-aqueous electrolyte solutions. Here, we use operando small
and wide angle X-ray scattering and operando small angle neutron scattering (SANS)
measurements to track the nucleation, growth and dissolution of solid deposits
from atomic to sub-micron scales during real-time Li-S cell operation. In particular,
stochastic modelling based on the SANS data allows quantifying the nanoscale phase
evolution during battery cycling. We show that next to nano-crystalline Li2S
the deposit comprises solid short-chain PSs particles. The analysis of the experimental
data suggests that initially, Li2S2
precipitates from the solution and then is partially converted via solid-state
electroreduction to Li2S. We further demonstrate that mass
transport, rather than electron transport through a thin passivating film, limits
the discharge capacity and rate performance in Li-S cells.
acknowledgement: "This project has received funding from the European Union’s Horizon
2020 research and innovation program under the Marie Skłodowska-Curie grant NanoEvolution,
grant agreement No 894042. The authors acknowledge the CERIC-ERIC Consortium for
the access to the Austrian SAXS beamline and TU Graz for support through the Lead
Project LP-03.\r\nLikewise, the use of SOMAPP Lab, a core facility supported by
the Austrian Federal Ministry of Education, Science and Research, the Graz University
of Technology, the University of Graz, and Anton Paar GmbH is acknowledged. In addition,
the authors acknowledge access to the D-22SANS beamline at the ILL neutron source.
Electron microscopy measurements were performed at the Scientific Scenter for Optical
and Electron Microscopy (ScopeM) of the Swiss Federal Institute of Technology. C.P.
and J.M.M. thank A. Senol for her support with the SANS\r\nbeamtime preparation.
S.D.T, A.V. and R.D. acknowledge the financial support by the Slovenian Research
Agency (ARRS) research core funding P2-0393 and P2-0423. Furthermore, A.V. acknowledge
the funding from the Slovenian Research Agency, research project Z2−1863.\r\nS.A.F.
is indebted to IST Austria for support. "
article_number: '6326'
article_processing_charge: No
article_type: original
author:
- first_name: Christian
full_name: Prehal, Christian
last_name: Prehal
- first_name: Jean-Marc
full_name: von Mentlen, Jean-Marc
last_name: von Mentlen
- first_name: Sara
full_name: Drvarič Talian, Sara
last_name: Drvarič Talian
- first_name: Alen
full_name: Vizintin, Alen
last_name: Vizintin
- first_name: Robert
full_name: Dominko, Robert
last_name: Dominko
- first_name: Heinz
full_name: Amenitsch, Heinz
last_name: Amenitsch
- first_name: Lionel
full_name: Porcar, Lionel
last_name: Porcar
- first_name: Stefan Alexander
full_name: Freunberger, Stefan Alexander
id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425
last_name: Freunberger
orcid: 0000-0003-2902-5319
- first_name: Vanessa
full_name: Wood, Vanessa
last_name: Wood
citation:
ama: Prehal C, von Mentlen J-M, Drvarič Talian S, et al. On the nanoscale structural
evolution of solid discharge products in lithium-sulfur batteries using operando
scattering. Nature Communications. 2022;13. doi:10.1038/s41467-022-33931-4
apa: Prehal, C., von Mentlen, J.-M., Drvarič Talian, S., Vizintin, A., Dominko,
R., Amenitsch, H., … Wood, V. (2022). On the nanoscale structural evolution of
solid discharge products in lithium-sulfur batteries using operando scattering.
Nature Communications. Springer Nature. https://doi.org/10.1038/s41467-022-33931-4
chicago: Prehal, Christian, Jean-Marc von Mentlen, Sara Drvarič Talian, Alen Vizintin,
Robert Dominko, Heinz Amenitsch, Lionel Porcar, Stefan Alexander Freunberger,
and Vanessa Wood. “On the Nanoscale Structural Evolution of Solid Discharge Products
in Lithium-Sulfur Batteries Using Operando Scattering.” Nature Communications.
Springer Nature, 2022. https://doi.org/10.1038/s41467-022-33931-4.
ieee: C. Prehal et al., “On the nanoscale structural evolution of solid discharge
products in lithium-sulfur batteries using operando scattering,” Nature Communications,
vol. 13. Springer Nature, 2022.
ista: Prehal C, von Mentlen J-M, Drvarič Talian S, Vizintin A, Dominko R, Amenitsch
H, Porcar L, Freunberger SA, Wood V. 2022. On the nanoscale structural evolution
of solid discharge products in lithium-sulfur batteries using operando scattering.
Nature Communications. 13, 6326.
mla: Prehal, Christian, et al. “On the Nanoscale Structural Evolution of Solid Discharge
Products in Lithium-Sulfur Batteries Using Operando Scattering.” Nature Communications,
vol. 13, 6326, Springer Nature, 2022, doi:10.1038/s41467-022-33931-4.
short: C. Prehal, J.-M. von Mentlen, S. Drvarič Talian, A. Vizintin, R. Dominko,
H. Amenitsch, L. Porcar, S.A. Freunberger, V. Wood, Nature Communications 13 (2022).
corr_author: '1'
date_created: 2023-01-16T09:45:09Z
date_published: 2022-10-24T00:00:00Z
date_updated: 2024-10-09T21:03:47Z
day: '24'
ddc:
- '540'
department:
- _id: StFr
doi: 10.1038/s41467-022-33931-4
external_id:
isi:
- '000871563700006'
pmid:
- '36280671'
file:
- access_level: open_access
checksum: 5034336dbf0f860030ef745c08df9e0e
content_type: application/pdf
creator: dernst
date_created: 2023-01-27T07:19:11Z
date_updated: 2023-01-27T07:19:11Z
file_id: '12411'
file_name: 2022_NatureCommunications_Prehal.pdf
file_size: 4216931
relation: main_file
success: 1
file_date_updated: 2023-01-27T07:19:11Z
has_accepted_license: '1'
intvolume: ' 13'
isi: 1
keyword:
- General Physics and Astronomy
- General Biochemistry
- Genetics and Molecular Biology
- General Chemistry
- Multidisciplinary
language:
- iso: eng
month: '10'
oa: 1
oa_version: Published Version
pmid: 1
publication: Nature Communications
publication_identifier:
issn:
- 2041-1723
publication_status: published
publisher: Springer Nature
quality_controlled: '1'
scopus_import: '1'
status: public
title: On the nanoscale structural evolution of solid discharge products in lithium-sulfur
batteries using operando scattering
tmp:
image: /images/cc_by.png
legal_code_url: https://creativecommons.org/licenses/by/4.0/legalcode
name: Creative Commons Attribution 4.0 International Public License (CC-BY 4.0)
short: CC BY (4.0)
type: journal_article
user_id: 4359f0d1-fa6c-11eb-b949-802e58b17ae8
volume: 13
year: '2022'
...
---
_id: '12227'
abstract:
- lang: eng
text: Polydicyclopentadiene (pDCPD), a thermoset with excellent mechanical properties,
has enormous potential as a lightweight, tough, and stable matrix material owing
to its highly cross-linked macromolecular network. This work describes generating
pDCPD-based foams and hierarchically porous carbons derived therefrom by combining
ring-opening metathesis polymerization (ROMP) of DCPD, high internal phase emulsions
(HIPEs) as structural templates, and subsequent carbonization. The structure and
function of the carbon foams were characterized and discussed in detail using
scanning electron, transmission electron, or atomic force microscopy (SEM, TEM,
AFM), electron energy-loss spectroscopy (TEM-EELS), N2 sorption, and analyses
of electrical conductivity as well as mechanical properties. The resulting materials
exhibited uniform, shape-retaining shrinkage of only ∼1/3 after carbonization.
No structural failure was observed even when the pDCPD precursor foams were heated
to 1400 °C. Instead, the high porosity, void size, and 3D interconnectivity were
fully preserved, and the void diameters could be adjusted between 87 and 2.5 μm.
Moreover, foams have a carbon content >97%, an electronic conductivity of up to
2800 S·m–1, a Young’s modulus of up to 2.1 GPa, and a specific surface area of
up to 1200 m2·g–1. Surprisingly, the pDCPD foams were carbonized into shapes other
than monoliths, such as 10’s of micron thick membranes or foamy coatings adhered
to a metal foil or grid substrate. The latter coatings even adhere upon bending.
Finally, as a use case, carbonized foams were applied as porous cathodes for Li–O2
batteries where the foams show a favorable combination of porosity, active surface
area, and pore size for outstanding capacity.
acknowledgement: S.K. acknowledges the financial support from the Slovenian Research
Agency (grants P1-0021, P2-0150). Support by Graz University of Technology (LP-03
– Porous Materials@Work) and from VARTA Innovation GmbH is kindly acknowledged.
We thank Umicore for providing the initiator and Matjaž Mazaj (National Institute
of Chemistry, Ljubljana) and Karel Jerabek (Czech Academy of Sciences) for measurements
and fruitful discussions. S.A.F. is indebted to the Austrian Federal Ministry of
Science, Research and Economy; the Austrian Research Promotion Agency (Grant No.
845364); and ISTA for support.
article_processing_charge: No
article_type: original
author:
- first_name: Sebastijan
full_name: Kovačič, Sebastijan
last_name: Kovačič
- first_name: Bettina
full_name: Schafzahl, Bettina
last_name: Schafzahl
- first_name: Nadejda B.
full_name: Matsko, Nadejda B.
last_name: Matsko
- first_name: Katharina
full_name: Gruber, Katharina
last_name: Gruber
- first_name: Martin
full_name: Schmuck, Martin
last_name: Schmuck
- first_name: Stefan
full_name: Koller, Stefan
last_name: Koller
- first_name: Stefan Alexander
full_name: Freunberger, Stefan Alexander
id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425
last_name: Freunberger
orcid: 0000-0003-2902-5319
- first_name: Christian
full_name: Slugovc, Christian
last_name: Slugovc
citation:
ama: 'Kovačič S, Schafzahl B, Matsko NB, et al. Carbon foams via ring-opening metathesis
polymerization of emulsion templates: A facile method to make carbon current collectors
for battery applications. ACS Applied Energy Materials. 2022;5(11):14381-14390.
doi:10.1021/acsaem.2c02787'
apa: 'Kovačič, S., Schafzahl, B., Matsko, N. B., Gruber, K., Schmuck, M., Koller,
S., … Slugovc, C. (2022). Carbon foams via ring-opening metathesis polymerization
of emulsion templates: A facile method to make carbon current collectors for battery
applications. ACS Applied Energy Materials. American Chemical Society.
https://doi.org/10.1021/acsaem.2c02787'
chicago: 'Kovačič, Sebastijan, Bettina Schafzahl, Nadejda B. Matsko, Katharina Gruber,
Martin Schmuck, Stefan Koller, Stefan Alexander Freunberger, and Christian Slugovc.
“Carbon Foams via Ring-Opening Metathesis Polymerization of Emulsion Templates:
A Facile Method to Make Carbon Current Collectors for Battery Applications.” ACS
Applied Energy Materials. American Chemical Society, 2022. https://doi.org/10.1021/acsaem.2c02787.'
ieee: 'S. Kovačič et al., “Carbon foams via ring-opening metathesis polymerization
of emulsion templates: A facile method to make carbon current collectors for battery
applications,” ACS Applied Energy Materials, vol. 5, no. 11. American Chemical
Society, pp. 14381–14390, 2022.'
ista: 'Kovačič S, Schafzahl B, Matsko NB, Gruber K, Schmuck M, Koller S, Freunberger
SA, Slugovc C. 2022. Carbon foams via ring-opening metathesis polymerization of
emulsion templates: A facile method to make carbon current collectors for battery
applications. ACS Applied Energy Materials. 5(11), 14381–14390.'
mla: 'Kovačič, Sebastijan, et al. “Carbon Foams via Ring-Opening Metathesis Polymerization
of Emulsion Templates: A Facile Method to Make Carbon Current Collectors for Battery
Applications.” ACS Applied Energy Materials, vol. 5, no. 11, American Chemical
Society, 2022, pp. 14381–90, doi:10.1021/acsaem.2c02787.'
short: S. Kovačič, B. Schafzahl, N.B. Matsko, K. Gruber, M. Schmuck, S. Koller,
S.A. Freunberger, C. Slugovc, ACS Applied Energy Materials 5 (2022) 14381–14390.
corr_author: '1'
date_created: 2023-01-16T09:48:53Z
date_published: 2022-10-16T00:00:00Z
date_updated: 2024-10-09T21:03:48Z
day: '16'
ddc:
- '540'
department:
- _id: StFr
doi: 10.1021/acsaem.2c02787
external_id:
isi:
- '000875635900001'
file:
- access_level: open_access
checksum: 572d15c250ab83d44f4e2c3aeb5f7388
content_type: application/pdf
creator: dernst
date_created: 2023-01-27T09:09:15Z
date_updated: 2023-01-27T09:09:15Z
file_id: '12420'
file_name: 2022_AppliedEnergyMaterials_Kovacic.pdf
file_size: 13105589
relation: main_file
success: 1
file_date_updated: 2023-01-27T09:09:15Z
has_accepted_license: '1'
intvolume: ' 5'
isi: 1
issue: '11'
keyword:
- Electrical and Electronic Engineering
- Materials Chemistry
- Electrochemistry
- Energy Engineering and Power Technology
- Chemical Engineering (miscellaneous)
language:
- iso: eng
month: '10'
oa: 1
oa_version: Published Version
page: 14381-14390
publication: ACS Applied Energy Materials
publication_identifier:
issn:
- 2574-0962
publication_status: published
publisher: American Chemical Society
quality_controlled: '1'
scopus_import: '1'
status: public
title: 'Carbon foams via ring-opening metathesis polymerization of emulsion templates:
A facile method to make carbon current collectors for battery applications'
tmp:
image: /images/cc_by.png
legal_code_url: https://creativecommons.org/licenses/by/4.0/legalcode
name: Creative Commons Attribution 4.0 International Public License (CC-BY 4.0)
short: CC BY (4.0)
type: journal_article
user_id: 4359f0d1-fa6c-11eb-b949-802e58b17ae8
volume: 5
year: '2022'
...
---
_id: '10813'
abstract:
- lang: eng
text: Redox mediators could catalyse otherwise slow and energy-inefficient cycling
of Li–S and Li–O2 batteries by shuttling electrons or holes between the electrode
and the solid insulating storage materials. For mediators to work efficiently
they need to oxidize the solid with fast kinetics but with the lowest possible
overpotential. However, the dependence of kinetics and overpotential is unclear,
which hinders informed improvement. Here, we find that when the redox potentials
of mediators are tuned via, for example, Li+ concentration in the electrolyte,
they exhibit distinct threshold potentials, where the kinetics accelerate several-fold
within a range as small as 10 mV. This phenomenon is independent of types of mediator
and electrolyte. The acceleration originates from the overpotentials required
to activate fast Li+/e− extraction and the following chemical step at specific
abundant surface facets. Efficient redox catalysis at insulating solids therefore
requires careful consideration of the surface conditions of the storage materials
and electrolyte-dependent redox potentials, which may be tuned by salt concentrations
or solvents.
acknowledgement: This work was financially supported by the National Natural Science
Foundation of China (grant nos. 51773092, 21975124, 11874254, 51802187 and U2030206).
It was further supported by Fujian science & technology innovation laboratory for
energy devices of China (21C-LAB), Key Research Project of Zhejiang Laboratory (grant
no. 2021PE0AC02) and the Cultivation Program for the Excellent Doctoral Dissertation
of Nanjing Tech University. S.A.F. is indebted to IST Austria for support.
article_processing_charge: No
article_type: original
author:
- first_name: Deqing
full_name: Cao, Deqing
last_name: Cao
- first_name: Xiaoxiao
full_name: Shen, Xiaoxiao
last_name: Shen
- first_name: Aiping
full_name: Wang, Aiping
last_name: Wang
- first_name: Fengjiao
full_name: Yu, Fengjiao
last_name: Yu
- first_name: Yuping
full_name: Wu, Yuping
last_name: Wu
- first_name: Siqi
full_name: Shi, Siqi
last_name: Shi
- first_name: Stefan Alexander
full_name: Freunberger, Stefan Alexander
id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425
last_name: Freunberger
orcid: 0000-0003-2902-5319
- first_name: Yuhui
full_name: Chen, Yuhui
last_name: Chen
citation:
ama: Cao D, Shen X, Wang A, et al. Threshold potentials for fast kinetics during
mediated redox catalysis of insulators in Li–O2 and Li–S batteries. Nature
Catalysis. 2022;5:193-201. doi:10.1038/s41929-022-00752-z
apa: Cao, D., Shen, X., Wang, A., Yu, F., Wu, Y., Shi, S., … Chen, Y. (2022). Threshold
potentials for fast kinetics during mediated redox catalysis of insulators in
Li–O2 and Li–S batteries. Nature Catalysis. Springer Nature. https://doi.org/10.1038/s41929-022-00752-z
chicago: Cao, Deqing, Xiaoxiao Shen, Aiping Wang, Fengjiao Yu, Yuping Wu, Siqi Shi,
Stefan Alexander Freunberger, and Yuhui Chen. “Threshold Potentials for Fast Kinetics
during Mediated Redox Catalysis of Insulators in Li–O2 and Li–S Batteries.” Nature
Catalysis. Springer Nature, 2022. https://doi.org/10.1038/s41929-022-00752-z.
ieee: D. Cao et al., “Threshold potentials for fast kinetics during mediated
redox catalysis of insulators in Li–O2 and Li–S batteries,” Nature Catalysis,
vol. 5. Springer Nature, pp. 193–201, 2022.
ista: Cao D, Shen X, Wang A, Yu F, Wu Y, Shi S, Freunberger SA, Chen Y. 2022. Threshold
potentials for fast kinetics during mediated redox catalysis of insulators in
Li–O2 and Li–S batteries. Nature Catalysis. 5, 193–201.
mla: Cao, Deqing, et al. “Threshold Potentials for Fast Kinetics during Mediated
Redox Catalysis of Insulators in Li–O2 and Li–S Batteries.” Nature Catalysis,
vol. 5, Springer Nature, 2022, pp. 193–201, doi:10.1038/s41929-022-00752-z.
short: D. Cao, X. Shen, A. Wang, F. Yu, Y. Wu, S. Shi, S.A. Freunberger, Y. Chen,
Nature Catalysis 5 (2022) 193–201.
corr_author: '1'
date_created: 2022-03-04T07:50:10Z
date_published: 2022-03-03T00:00:00Z
date_updated: 2024-10-09T21:01:46Z
day: '03'
department:
- _id: StFr
doi: 10.1038/s41929-022-00752-z
external_id:
isi:
- '000763879400001'
intvolume: ' 5'
isi: 1
keyword:
- Process Chemistry and Technology
- Biochemistry
- Bioengineering
- Catalysis
language:
- iso: eng
main_file_link:
- open_access: '1'
url: https://doi.org/10.21203/rs.3.rs-750965/v1
month: '03'
oa: 1
oa_version: Preprint
page: 193-201
publication: Nature Catalysis
publication_identifier:
issn:
- 2520-1158
publication_status: published
publisher: Springer Nature
quality_controlled: '1'
related_material:
record:
- id: '9978'
relation: earlier_version
status: public
scopus_import: '1'
status: public
title: Threshold potentials for fast kinetics during mediated redox catalysis of insulators
in Li–O2 and Li–S batteries
type: journal_article
user_id: 4359f0d1-fa6c-11eb-b949-802e58b17ae8
volume: 5
year: '2022'
...
---
_id: '12065'
abstract:
- lang: eng
text: Capacity, rate performance, and cycle life of aprotic Li–O2 batteries critically
depend on reversible electrodeposition of Li2O2. Current understanding states
surface-adsorbed versus solvated LiO2 controls Li2O2 growth as surface film or
as large particles. Herein, we show that Li2O2 forms across a wide range of electrolytes,
carbons, and current densities as particles via solution-mediated LiO2 disproportionation,
bringing into question the prevalence of any surface growth under practical conditions.
We describe a unified O2 reduction mechanism, which can explain all found capacity
relations and Li2O2 morphologies with exclusive solution discharge. Determining
particle morphology and achievable capacities are species mobilities, true areal
rate, and the degree of LiO2 association in solution. Capacity is conclusively
limited by mass transport through the tortuous Li2O2 rather than electron transport
through a passivating Li2O2 film. Provided that species mobilities and surface
growth are high, high capacities are also achieved with weakly solvating electrolytes,
which were previously considered prototypical for low capacity via surface growth.
acknowledged_ssus:
- _id: EM-Fac
- _id: M-Shop
acknowledgement: S.A.F. and C.P. are indebted to the European Research Council (ERC)
under the European Union’s Horizon 2020 research and innovation program (Grant Agreement
No. 636069). This project has received funding from the European Union’s Horizon
2020 research and innovation program under the Marie Skłodowska-Curie Grant NanoEvolution,
Grant Agreement No. 894042. S.A.F. and S.M. are indebted to Institute of Science
and Technology Austria (ISTA) for support. This research was supported by the Scientific
Service Units of ISTA through resources provided by the Electron Microscopy Facility
and the Miba Machine Shop. C.P. thanks Vanessa Wood (ETH Zürich) for her continuing
support.
article_processing_charge: Yes (via OA deal)
article_type: original
author:
- first_name: Christian
full_name: Prehal, Christian
last_name: Prehal
- first_name: Soumyadip
full_name: Mondal, Soumyadip
id: d25d21ef-dc8d-11ea-abe3-ec4576307f48
last_name: Mondal
- first_name: Ludek
full_name: Lovicar, Ludek
id: 36DB3A20-F248-11E8-B48F-1D18A9856A87
last_name: Lovicar
orcid: 0000-0001-6206-4200
- first_name: Stefan Alexander
full_name: Freunberger, Stefan Alexander
id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425
last_name: Freunberger
orcid: 0000-0003-2902-5319
citation:
ama: Prehal C, Mondal S, Lovicar L, Freunberger SA. Exclusive solution discharge
in Li-O₂ batteries? ACS Energy Letters. 2022;7(9):3112-3119. doi:10.1021/acsenergylett.2c01711
apa: Prehal, C., Mondal, S., Lovicar, L., & Freunberger, S. A. (2022). Exclusive
solution discharge in Li-O₂ batteries? ACS Energy Letters. American Chemical
Society. https://doi.org/10.1021/acsenergylett.2c01711
chicago: Prehal, Christian, Soumyadip Mondal, Ludek Lovicar, and Stefan Alexander
Freunberger. “Exclusive Solution Discharge in Li-O₂ Batteries?” ACS Energy
Letters. American Chemical Society, 2022. https://doi.org/10.1021/acsenergylett.2c01711.
ieee: C. Prehal, S. Mondal, L. Lovicar, and S. A. Freunberger, “Exclusive solution
discharge in Li-O₂ batteries?,” ACS Energy Letters, vol. 7, no. 9. American
Chemical Society, pp. 3112–3119, 2022.
ista: Prehal C, Mondal S, Lovicar L, Freunberger SA. 2022. Exclusive solution discharge
in Li-O₂ batteries? ACS Energy Letters. 7(9), 3112–3119.
mla: Prehal, Christian, et al. “Exclusive Solution Discharge in Li-O₂ Batteries?”
ACS Energy Letters, vol. 7, no. 9, American Chemical Society, 2022, pp.
3112–19, doi:10.1021/acsenergylett.2c01711.
short: C. Prehal, S. Mondal, L. Lovicar, S.A. Freunberger, ACS Energy Letters 7
(2022) 3112–3119.
corr_author: '1'
date_created: 2022-09-08T09:51:09Z
date_published: 2022-08-29T00:00:00Z
date_updated: 2026-04-07T12:27:23Z
day: '29'
ddc:
- '540'
department:
- _id: StFr
- _id: EM-Fac
doi: 10.1021/acsenergylett.2c01711
external_id:
isi:
- '000860787000001'
pmid:
- '36120663'
file:
- access_level: open_access
checksum: cf0bed3a2535c11d27244cd029dbc1d0
content_type: application/pdf
creator: dernst
date_created: 2023-01-20T08:43:51Z
date_updated: 2023-01-20T08:43:51Z
file_id: '12319'
file_name: 2022_ACSEnergyLetters_Prehal.pdf
file_size: 3827583
relation: main_file
success: 1
file_date_updated: 2023-01-20T08:43:51Z
has_accepted_license: '1'
intvolume: ' 7'
isi: 1
issue: '9'
language:
- iso: eng
month: '08'
oa: 1
oa_version: Published Version
page: 3112-3119
pmid: 1
publication: ACS Energy Letters
publication_identifier:
eissn:
- 2380-8195
publication_status: published
publisher: American Chemical Society
quality_controlled: '1'
related_material:
record:
- id: '20607'
relation: dissertation_contains
status: public
scopus_import: '1'
status: public
title: Exclusive solution discharge in Li-O₂ batteries?
tmp:
image: /images/cc_by.png
legal_code_url: https://creativecommons.org/licenses/by/4.0/legalcode
name: Creative Commons Attribution 4.0 International Public License (CC-BY 4.0)
short: CC BY (4.0)
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 7
year: '2022'
...
---
_id: '9113'
abstract:
- lang: eng
text: “Hydrogen economy” could enable a carbon-neutral sustainable energy chain.
However, issues with safety, storage, and transport of molecular hydrogen impede
its realization. Alcohols as liquid H2 carriers could be enablers, but state-of-the-art
reforming is difficult, requiring high temperatures >200 °C and pressures >25
bar, and the resulting H2 is carbonized beyond tolerance levels for direct use
in fuel cells. Here, we demonstrate ambient temperature and pressure alcohol reforming
in a fuel cell (ARFC) with a simultaneous electrical power output. The alcohol
is oxidized at the alkaline anode, where the resulting CO2 is sequestrated as
carbonate. Carbon-free H2 is liberated at the acidic cathode. The neutralization
energy between the alkaline anode and the acidic cathode drives the process, particularly
the unusually high entropy gain (1.27-fold ΔH). The significantly positive temperature
coefficient of the resulting electromotive force allows us to harvest a large
fraction of the output energy from the surrounding, achieving a thermodynamic
efficiency as high as 2.27. MoS2 as the cathode catalyst allows alcohol reforming
even under open-air conditions, a challenge that state-of-the-art alcohol reforming
failed to overcome. We further show reforming of a wide range of alcohols. The
ARFC offers an unprecedented route toward hydrogen economy as CO2 is simultaneously
captured and pure H2 produced at mild conditions.
acknowledgement: M.O.T. acknowledges DST/TMD/HFC/2 K18/58, DST-SERB, MHRD fast track,
and DST Nanomission forfinancialassistance. Z.M.B. acknowledges CSIR-SRF fellowship
fromMHRD, India. S.A.F. acknowledges support from IST Austria.
article_processing_charge: No
article_type: original
author:
- first_name: Zahid Manzoor
full_name: Manzoor Bhat, Zahid Manzoor
last_name: Manzoor Bhat
- first_name: Ravikumar
full_name: Thimmappa, Ravikumar
last_name: Thimmappa
- first_name: 'Neethu Christudas '
full_name: 'Dargily, Neethu Christudas '
last_name: Dargily
- first_name: 'Abdul '
full_name: 'Raafik, Abdul '
last_name: Raafik
- first_name: 'Alagar Raja '
full_name: 'Kottaichamy, Alagar Raja '
last_name: Kottaichamy
- first_name: 'Mruthyunjayachari Chattanahalli '
full_name: 'Devendrachari, Mruthyunjayachari Chattanahalli '
last_name: Devendrachari
- first_name: Mahesh
full_name: Itagi, Mahesh
last_name: Itagi
- first_name: Harish
full_name: ' Makri Nimbegondi Kotresh, Harish'
last_name: ' Makri Nimbegondi Kotresh'
- first_name: Stefan Alexander
full_name: Freunberger, Stefan Alexander
id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425
last_name: Freunberger
orcid: 0000-0003-2902-5319
- first_name: 'Musthafa '
full_name: 'Ottakam Thotiyl, Musthafa '
last_name: Ottakam Thotiyl
citation:
ama: Manzoor Bhat ZM, Thimmappa R, Dargily NC, et al. Ambient condition alcohol
reforming to hydrogen with electricity output. ACS Sustainable Chemistry and
Engineering. 2021;9(8):3104-3111. doi:10.1021/acssuschemeng.0c07547
apa: Manzoor Bhat, Z. M., Thimmappa, R., Dargily, N. C., Raafik, A., Kottaichamy,
A. R., Devendrachari, M. C., … Ottakam Thotiyl, M. (2021). Ambient condition alcohol
reforming to hydrogen with electricity output. ACS Sustainable Chemistry and
Engineering. American Chemical Society. https://doi.org/10.1021/acssuschemeng.0c07547
chicago: Manzoor Bhat, Zahid Manzoor, Ravikumar Thimmappa, Neethu Christudas Dargily,
Abdul Raafik, Alagar Raja Kottaichamy, Mruthyunjayachari Chattanahalli Devendrachari,
Mahesh Itagi, Harish Makri Nimbegondi Kotresh, Stefan Alexander Freunberger,
and Musthafa Ottakam Thotiyl. “Ambient Condition Alcohol Reforming to Hydrogen
with Electricity Output.” ACS Sustainable Chemistry and Engineering. American
Chemical Society, 2021. https://doi.org/10.1021/acssuschemeng.0c07547.
ieee: Z. M. Manzoor Bhat et al., “Ambient condition alcohol reforming to
hydrogen with electricity output,” ACS Sustainable Chemistry and Engineering,
vol. 9, no. 8. American Chemical Society, pp. 3104–3111, 2021.
ista: Manzoor Bhat ZM, Thimmappa R, Dargily NC, Raafik A, Kottaichamy AR, Devendrachari
MC, Itagi M, Makri Nimbegondi Kotresh H, Freunberger SA, Ottakam Thotiyl M. 2021.
Ambient condition alcohol reforming to hydrogen with electricity output. ACS Sustainable
Chemistry and Engineering. 9(8), 3104–3111.
mla: Manzoor Bhat, Zahid Manzoor, et al. “Ambient Condition Alcohol Reforming to
Hydrogen with Electricity Output.” ACS Sustainable Chemistry and Engineering,
vol. 9, no. 8, American Chemical Society, 2021, pp. 3104–11, doi:10.1021/acssuschemeng.0c07547.
short: Z.M. Manzoor Bhat, R. Thimmappa, N.C. Dargily, A. Raafik, A.R. Kottaichamy,
M.C. Devendrachari, M. Itagi, H. Makri Nimbegondi Kotresh, S.A. Freunberger,
M. Ottakam Thotiyl, ACS Sustainable Chemistry and Engineering 9 (2021) 3104–3111.
corr_author: '1'
date_created: 2021-02-12T09:20:18Z
date_published: 2021-02-11T00:00:00Z
date_updated: 2024-10-09T21:00:24Z
day: '11'
department:
- _id: StFr
doi: 10.1021/acssuschemeng.0c07547
external_id:
isi:
- '000625460400010'
intvolume: ' 9'
isi: 1
issue: '8'
language:
- iso: eng
month: '02'
oa_version: None
page: 3104-3111
publication: ACS Sustainable Chemistry and Engineering
publication_identifier:
eissn:
- 2168-0485
publication_status: published
publisher: American Chemical Society
quality_controlled: '1'
scopus_import: '1'
status: public
title: Ambient condition alcohol reforming to hydrogen with electricity output
type: journal_article
user_id: 4359f0d1-fa6c-11eb-b949-802e58b17ae8
volume: 9
year: '2021'
...
---
_id: '9301'
abstract:
- lang: eng
text: Electrodepositing insulating lithium peroxide (Li2O2) is the key process during
discharge of aprotic Li–O2 batteries and determines rate, capacity, and reversibility.
Current understanding states that the partition between surface adsorbed and dissolved
lithium superoxide governs whether Li2O2 grows as a conformal surface film or
larger particles, leading to low or high capacities, respectively. However, better
understanding governing factors for Li2O2 packing density and capacity requires
structural sensitive in situ metrologies. Here, we establish in situ small- and
wide-angle X-ray scattering (SAXS/WAXS) as a suitable method to record the Li2O2
phase evolution with atomic to submicrometer resolution during cycling a custom-built
in situ Li–O2 cell. Combined with sophisticated data analysis, SAXS allows retrieving
rich quantitative structural information from complex multiphase systems. Surprisingly,
we find that features are absent that would point at a Li2O2 surface film formed
via two consecutive electron transfers, even in poorly solvating electrolytes
thought to be prototypical for surface growth. All scattering data can be modeled
by stacks of thin Li2O2 platelets potentially forming large toroidal particles.
Li2O2 solution growth is further justified by rotating ring-disk electrode measurements
and electron microscopy. Higher discharge overpotentials lead to smaller Li2O2
particles, but there is no transition to an electronically passivating, conformal
Li2O2 coating. Hence, mass transport of reactive species rather than electronic
transport through a Li2O2 film limits the discharge capacity. Provided that species
mobilities and carbon surface areas are high, this allows for high discharge capacities
even in weakly solvating electrolytes. The currently accepted Li–O2 reaction mechanism
ought to be reconsidered.
acknowledged_ssus:
- _id: EM-Fac
acknowledgement: S.A.F. and C.P. are indebted to the European Research Council under
the European Union's Horizon 2020 research and innovation program (Grant Agreement
No. 636069), the Austrian Federal Ministry of Science, Research and Economy, and
the Austrian Research Promotion Agency (Grant No. 845364). We acknowledge A. Zankel
and H. Schroettner for support with SEM measurements. C.P. thanks N. Kostoglou,
C. Koczwara, M. Hartmann, and M. Burian for discussions on gas sorption analysis,
C++ programming, Monte Carlo modeling, and in situ SAXS experiments, respectively.
We thank S. Stadlbauer for help with Karl Fischer titration, R. Riccò for gas sorption
measurements, and acknowledge Graz University of Technology for support through
the Lead Project LP-03. Likewise, the use of SOMAPP Lab, a core facility supported
by the Austrian Federal Ministry of Education, Science and Research, the Graz University
of Technology, the University of Graz, and Anton Paar GmbH is acknowledged. S.A.F.
is indebted to Institute of Science and Technology Austria (IST Austria) for support.
This research was supported by the Scientific Service Units of IST Austria through
resources provided by the Electron Microscopy Facility.
article_number: e2021893118
article_processing_charge: No
article_type: original
author:
- first_name: Christian
full_name: Prehal, Christian
last_name: Prehal
- first_name: Aleksej
full_name: Samojlov, Aleksej
last_name: Samojlov
- first_name: Manfred
full_name: Nachtnebel, Manfred
last_name: Nachtnebel
- first_name: Ludek
full_name: Lovicar, Ludek
id: 36DB3A20-F248-11E8-B48F-1D18A9856A87
last_name: Lovicar
orcid: 0000-0001-6206-4200
- first_name: Manfred
full_name: Kriechbaum, Manfred
last_name: Kriechbaum
- first_name: Heinz
full_name: Amenitsch, Heinz
last_name: Amenitsch
- first_name: Stefan Alexander
full_name: Freunberger, Stefan Alexander
id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425
last_name: Freunberger
orcid: 0000-0003-2902-5319
citation:
ama: Prehal C, Samojlov A, Nachtnebel M, et al. In situ small-angle X-ray scattering
reveals solution phase discharge of Li–O2 batteries with weakly solvating electrolytes.
Proceedings of the National Academy of Sciences of the United States of America.
2021;118(14). doi:10.1073/pnas.2021893118
apa: Prehal, C., Samojlov, A., Nachtnebel, M., Lovicar, L., Kriechbaum, M., Amenitsch,
H., & Freunberger, S. A. (2021). In situ small-angle X-ray scattering reveals
solution phase discharge of Li–O2 batteries with weakly solvating electrolytes.
Proceedings of the National Academy of Sciences of the United States of America.
National Academy of Sciences. https://doi.org/10.1073/pnas.2021893118
chicago: Prehal, Christian, Aleksej Samojlov, Manfred Nachtnebel, Ludek Lovicar,
Manfred Kriechbaum, Heinz Amenitsch, and Stefan Alexander Freunberger. “In Situ
Small-Angle X-Ray Scattering Reveals Solution Phase Discharge of Li–O2 Batteries
with Weakly Solvating Electrolytes.” Proceedings of the National Academy of
Sciences of the United States of America. National Academy of Sciences, 2021.
https://doi.org/10.1073/pnas.2021893118.
ieee: C. Prehal et al., “In situ small-angle X-ray scattering reveals solution
phase discharge of Li–O2 batteries with weakly solvating electrolytes,” Proceedings
of the National Academy of Sciences of the United States of America, vol.
118, no. 14. National Academy of Sciences, 2021.
ista: Prehal C, Samojlov A, Nachtnebel M, Lovicar L, Kriechbaum M, Amenitsch H,
Freunberger SA. 2021. In situ small-angle X-ray scattering reveals solution phase
discharge of Li–O2 batteries with weakly solvating electrolytes. Proceedings of
the National Academy of Sciences of the United States of America. 118(14), e2021893118.
mla: Prehal, Christian, et al. “In Situ Small-Angle X-Ray Scattering Reveals Solution
Phase Discharge of Li–O2 Batteries with Weakly Solvating Electrolytes.” Proceedings
of the National Academy of Sciences of the United States of America, vol.
118, no. 14, e2021893118, National Academy of Sciences, 2021, doi:10.1073/pnas.2021893118.
short: C. Prehal, A. Samojlov, M. Nachtnebel, L. Lovicar, M. Kriechbaum, H. Amenitsch,
S.A. Freunberger, Proceedings of the National Academy of Sciences of the United
States of America 118 (2021).
date_created: 2021-03-31T07:00:01Z
date_published: 2021-04-06T00:00:00Z
date_updated: 2025-06-12T06:56:39Z
day: '06'
department:
- _id: StFr
- _id: EM-Fac
doi: 10.1073/pnas.2021893118
external_id:
isi:
- '000637398300050'
pmid:
- '33785597'
intvolume: ' 118'
isi: 1
issue: '14'
keyword:
- small-angle X-ray scattering
- oxygen reduction
- disproportionation
- Li-air battery
language:
- iso: eng
main_file_link:
- open_access: '1'
url: https://doi.org/10.26434/chemrxiv.11447775
month: '04'
oa: 1
oa_version: Preprint
pmid: 1
publication: Proceedings of the National Academy of Sciences of the United States
of America
publication_identifier:
eissn:
- 1091-6490
issn:
- 0027-8424
publication_status: published
publisher: National Academy of Sciences
quality_controlled: '1'
scopus_import: '1'
status: public
title: In situ small-angle X-ray scattering reveals solution phase discharge of Li–O2
batteries with weakly solvating electrolytes
type: journal_article
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
volume: 118
year: '2021'
...
---
_id: '9447'
abstract:
- lang: eng
text: 'Lithium bis(trifluoromethylsulfonyl)imide (LiTFSI) based water-in-salt electrolytes
(WiSEs) has recently emerged as a new promising class of electrolytes, primarily
owing to their wide electrochemical stability windows (~3–4 V), that by far exceed
the thermodynamic stability window of water (1.23 V). Upon increasing the salt
concentration towards superconcentration the onset of the oxygen evolution reaction
(OER) shifts more significantly than the hydrogen evolution reaction (HER) does.
The OER shift has been explained by the accumulation of hydrophobic anions blocking
water access to the electrode surface, hence by double layer theory. Here we demonstrate
that the processes during oxidation are much more complex, involving OER, carbon
and salt decomposition by OER intermediates, and salt precipitation upon local
oversaturation. The positive shift in the onset potential of oxidation currents
was elucidated by combining several advanced analysis techniques: rotating ring-disk
electrode voltammetry, online electrochemical mass spectrometry, and X-ray photoelectron
spectroscopy, using both dilute and superconcentrated electrolytes. The results
demonstrate the importance of reactive OER intermediates and surface films for
electrolyte and electrode stability and motivate further studies of the nature
of the electrode.'
article_number: '050550'
article_processing_charge: No
author:
- first_name: Marion
full_name: Maffre, Marion
last_name: Maffre
- first_name: Roza
full_name: Bouchal, Roza
last_name: Bouchal
- first_name: Stefan Alexander
full_name: Freunberger, Stefan Alexander
id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425
last_name: Freunberger
orcid: 0000-0003-2902-5319
- first_name: Niklas
full_name: Lindahl, Niklas
last_name: Lindahl
- first_name: Patrik
full_name: Johansson, Patrik
last_name: Johansson
- first_name: Frédéric
full_name: Favier, Frédéric
last_name: Favier
- first_name: Olivier
full_name: Fontaine, Olivier
last_name: Fontaine
- first_name: Daniel
full_name: Bélanger, Daniel
last_name: Bélanger
citation:
ama: Maffre M, Bouchal R, Freunberger SA, et al. Investigation of electrochemical
and chemical processes occurring at positive potentials in “Water-in-Salt” electrolytes.
Journal of The Electrochemical Society. 2021;168(5). doi:10.1149/1945-7111/ac0300
apa: Maffre, M., Bouchal, R., Freunberger, S. A., Lindahl, N., Johansson, P., Favier,
F., … Bélanger, D. (2021). Investigation of electrochemical and chemical processes
occurring at positive potentials in “Water-in-Salt” electrolytes. Journal of
The Electrochemical Society. IOP Publishing. https://doi.org/10.1149/1945-7111/ac0300
chicago: Maffre, Marion, Roza Bouchal, Stefan Alexander Freunberger, Niklas Lindahl,
Patrik Johansson, Frédéric Favier, Olivier Fontaine, and Daniel Bélanger. “Investigation
of Electrochemical and Chemical Processes Occurring at Positive Potentials in
‘Water-in-Salt’ Electrolytes.” Journal of The Electrochemical Society.
IOP Publishing, 2021. https://doi.org/10.1149/1945-7111/ac0300.
ieee: M. Maffre et al., “Investigation of electrochemical and chemical processes
occurring at positive potentials in ‘Water-in-Salt’ electrolytes,” Journal
of The Electrochemical Society, vol. 168, no. 5. IOP Publishing, 2021.
ista: Maffre M, Bouchal R, Freunberger SA, Lindahl N, Johansson P, Favier F, Fontaine
O, Bélanger D. 2021. Investigation of electrochemical and chemical processes occurring
at positive potentials in “Water-in-Salt” electrolytes. Journal of The Electrochemical
Society. 168(5), 050550.
mla: Maffre, Marion, et al. “Investigation of Electrochemical and Chemical Processes
Occurring at Positive Potentials in ‘Water-in-Salt’ Electrolytes.” Journal
of The Electrochemical Society, vol. 168, no. 5, 050550, IOP Publishing, 2021,
doi:10.1149/1945-7111/ac0300.
short: M. Maffre, R. Bouchal, S.A. Freunberger, N. Lindahl, P. Johansson, F. Favier,
O. Fontaine, D. Bélanger, Journal of The Electrochemical Society 168 (2021).
date_created: 2021-06-03T09:58:38Z
date_published: 2021-05-01T00:00:00Z
date_updated: 2024-10-21T06:02:10Z
day: '01'
department:
- _id: StFr
doi: 10.1149/1945-7111/ac0300
external_id:
isi:
- '000657724200001'
intvolume: ' 168'
isi: 1
issue: '5'
keyword:
- Renewable Energy
- Sustainability and the Environment
- Electrochemistry
- Materials Chemistry
- Electronic
- Optical and Magnetic Materials
- Surfaces
- Coatings and Films
- Condensed Matter Physics
language:
- iso: eng
month: '05'
oa_version: None
publication: Journal of The Electrochemical Society
publication_identifier:
eissn:
- 1945-7111
issn:
- 0013-4651
publication_status: published
publisher: IOP Publishing
quality_controlled: '1'
scopus_import: '1'
status: public
title: Investigation of electrochemical and chemical processes occurring at positive
potentials in “Water-in-Salt” electrolytes
type: journal_article
user_id: c635000d-4b10-11ee-a964-aac5a93f6ac1
volume: 168
year: '2021'
...
---
_id: '9978'
abstract:
- lang: eng
text: Redox mediators could catalyse otherwise slow and energy-inefficient cycling
of Li-S and Li-O 2 batteries by shuttling electrons/holes between the electrode
and the solid insulating storage materials. For mediators to work efficiently
they need to oxidize the solid with fast kinetics yet the lowest possible overpotential.
Here, we found that when the redox potentials of mediators are tuned via, e.g.,
Li + concentration in the electrolyte, they exhibit distinct threshold potentials,
where the kinetics accelerate several-fold within a range as small as 10 mV. This
phenomenon is independent of types of mediators and electrolyte. The acceleration
originates from the overpotentials required to activate fast Li + /e – extraction
and the following chemical step at specific abundant surface facets. Efficient
redox catalysis at insulating solids requires therefore carefully considering
the surface conditions of the storage materials and electrolyte-dependent redox
potentials, which may be tuned by salt concentrations or solvents.
acknowledgement: 'This work was financially supported by the National Natural Science
Foundation of China (51773092, 21975124, 11874254, 51802187, U2030206). S.A.F. is
indebted to IST Austria for support. '
article_processing_charge: No
author:
- first_name: Deqing
full_name: Cao, Deqing
last_name: Cao
- first_name: Xiaoxiao
full_name: Shen, Xiaoxiao
last_name: Shen
- first_name: Aiping
full_name: Wang, Aiping
last_name: Wang
- first_name: Fengjiao
full_name: Yu, Fengjiao
last_name: Yu
- first_name: Yuping
full_name: Wu, Yuping
last_name: Wu
- first_name: Siqi
full_name: Shi, Siqi
last_name: Shi
- first_name: Stefan Alexander
full_name: Freunberger, Stefan Alexander
id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425
last_name: Freunberger
orcid: 0000-0003-2902-5319
- first_name: Yuhui
full_name: Chen, Yuhui
last_name: Chen
citation:
ama: Cao D, Shen X, Wang A, et al. Sharp kinetic acceleration potentials during
mediated redox catalysis of insulators. Research Square. doi:10.21203/rs.3.rs-750965/v1
apa: Cao, D., Shen, X., Wang, A., Yu, F., Wu, Y., Shi, S., … Chen, Y. (n.d.). Sharp
kinetic acceleration potentials during mediated redox catalysis of insulators.
Research Square. Research Square. https://doi.org/10.21203/rs.3.rs-750965/v1
chicago: Cao, Deqing, Xiaoxiao Shen, Aiping Wang, Fengjiao Yu, Yuping Wu, Siqi Shi,
Stefan Alexander Freunberger, and Yuhui Chen. “Sharp Kinetic Acceleration Potentials
during Mediated Redox Catalysis of Insulators.” Research Square. Research
Square, n.d. https://doi.org/10.21203/rs.3.rs-750965/v1.
ieee: D. Cao et al., “Sharp kinetic acceleration potentials during mediated
redox catalysis of insulators,” Research Square. Research Square.
ista: Cao D, Shen X, Wang A, Yu F, Wu Y, Shi S, Freunberger SA, Chen Y. Sharp kinetic
acceleration potentials during mediated redox catalysis of insulators. Research
Square, 10.21203/rs.3.rs-750965/v1.
mla: Cao, Deqing, et al. “Sharp Kinetic Acceleration Potentials during Mediated
Redox Catalysis of Insulators.” Research Square, Research Square, doi:10.21203/rs.3.rs-750965/v1.
short: D. Cao, X. Shen, A. Wang, F. Yu, Y. Wu, S. Shi, S.A. Freunberger, Y. Chen,
Research Square (n.d.).
corr_author: '1'
date_created: 2021-08-31T12:54:16Z
date_published: 2021-08-18T00:00:00Z
date_updated: 2024-10-09T21:01:46Z
day: '18'
ddc:
- '541'
department:
- _id: StFr
doi: 10.21203/rs.3.rs-750965/v1
file:
- access_level: open_access
checksum: 1878e91c29d5769ed5a827b0b7addf00
content_type: application/pdf
creator: cchlebak
date_created: 2021-08-31T14:02:19Z
date_updated: 2021-08-31T14:02:19Z
file_id: '9979'
file_name: 2021_ResearchSquare_Cao.pdf
file_size: 1019662
relation: main_file
success: 1
file_date_updated: 2021-08-31T14:02:19Z
has_accepted_license: '1'
keyword:
- Catalysis
- Energy engineering
- Materials theory and modeling
language:
- iso: eng
month: '08'
oa: 1
oa_version: Preprint
page: '21'
publication: Research Square
publication_identifier:
eissn:
- 2693-5015
publication_status: submitted
publisher: Research Square
related_material:
record:
- id: '10813'
relation: later_version
status: public
status: public
title: Sharp kinetic acceleration potentials during mediated redox catalysis of insulators
tmp:
image: /images/cc_by.png
legal_code_url: https://creativecommons.org/licenses/by/4.0/legalcode
name: Creative Commons Attribution 4.0 International Public License (CC-BY 4.0)
short: CC BY (4.0)
type: preprint
user_id: 2DF688A6-F248-11E8-B48F-1D18A9856A87
year: '2021'
...
---
_id: '9980'
abstract:
- lang: eng
text: Insufficient understanding of the mechanism that reversibly converts sulphur
into lithium sulphide (Li2S) via soluble polysulphides (PS) hampers the realization
of high performance lithium-sulphur cells. Typically Li2S formation is explained
by direct electroreduction of a PS to Li2S; however, this is not consistent with
the size of the insulating Li2S deposits. Here, we use in situ small and wide
angle X-ray scattering (SAXS/WAXS) to track the growth and dissolution of crystalline
and amorphous deposits from atomic to sub-micron scales during charge and discharge.
Stochastic modelling based on the SAXS data allows quantification of the chemical
phase evolution during discharge and charge. We show that Li2S deposits predominantly
via disproportionation of transient, solid Li2S2 to form primary Li2S crystallites
and solid Li2S4 particles. We further demonstrate that this process happens in
reverse during charge. These findings show that the discharge capacity and rate
capability in Li-S battery cathodes are therefore limited by mass transport through
the increasingly tortuous network of Li2S / Li2S4 / carbon pores rather than electron
transport through a passivating surface film.
acknowledgement: "This project has received funding from the European Union’s Horizon
2020 research and innovation program under the Marie Skłodowska-Curie grant NanoEvolution,
grant agreement No 894042. The authors acknowledge TU Graz for support through the
Lead Project LP-03. Likewise, the use of SOMAPP Lab, a core facility supported by
the Austrian Federal Ministry of Education, Science and Research, the Graz University\r\n6
of Technology, the University of Graz, and Anton Paar GmbH is acknowledged. S.D.T,
A.V. and R.D. acknowledge the financial support by the Slovenian Research Agency
(ARRS) research core funding P2-0393. Furthermore, A.V. acknowledge the funding
from the Slovenian Research Agency, research project Z2-1863. S.A.F. is indebted
to IST Austria for support. "
article_processing_charge: No
author:
- first_name: Christian
full_name: Prehal, Christian
last_name: Prehal
- first_name: Sara Drvarič
full_name: Talian, Sara Drvarič
last_name: Talian
- first_name: Alen
full_name: Vizintin, Alen
last_name: Vizintin
- first_name: Heinz
full_name: Amenitsch, Heinz
last_name: Amenitsch
- first_name: Robert
full_name: Dominko, Robert
last_name: Dominko
- first_name: Stefan Alexander
full_name: Freunberger, Stefan Alexander
id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425
last_name: Freunberger
orcid: 0000-0003-2902-5319
- first_name: Vanessa
full_name: Wood, Vanessa
last_name: Wood
citation:
ama: Prehal C, Talian SD, Vizintin A, et al. Mechanism of Li2S formation and dissolution
in Lithium-Sulphur batteries. Research Square. doi:10.21203/rs.3.rs-818607/v1
apa: Prehal, C., Talian, S. D., Vizintin, A., Amenitsch, H., Dominko, R., Freunberger,
S. A., & Wood, V. (n.d.). Mechanism of Li2S formation and dissolution in Lithium-Sulphur
batteries. Research Square. https://doi.org/10.21203/rs.3.rs-818607/v1
chicago: Prehal, Christian, Sara Drvarič Talian, Alen Vizintin, Heinz Amenitsch,
Robert Dominko, Stefan Alexander Freunberger, and Vanessa Wood. “Mechanism of
Li2S Formation and Dissolution in Lithium-Sulphur Batteries.” Research Square,
n.d. https://doi.org/10.21203/rs.3.rs-818607/v1.
ieee: C. Prehal et al., “Mechanism of Li2S formation and dissolution in Lithium-Sulphur
batteries,” Research Square. .
ista: Prehal C, Talian SD, Vizintin A, Amenitsch H, Dominko R, Freunberger SA, Wood
V. Mechanism of Li2S formation and dissolution in Lithium-Sulphur batteries. Research
Square, 10.21203/rs.3.rs-818607/v1.
mla: Prehal, Christian, et al. “Mechanism of Li2S Formation and Dissolution in Lithium-Sulphur
Batteries.” Research Square, doi:10.21203/rs.3.rs-818607/v1.
short: C. Prehal, S.D. Talian, A. Vizintin, H. Amenitsch, R. Dominko, S.A. Freunberger,
V. Wood, Research Square (n.d.).
date_created: 2021-09-02T08:45:00Z
date_published: 2021-08-16T00:00:00Z
date_updated: 2021-12-03T10:35:42Z
day: '16'
ddc:
- '621'
department:
- _id: StFr
doi: 10.21203/rs.3.rs-818607/v1
keyword:
- Li2S
- Lithium Sulphur Batteries
- SAXS
- WAXS
language:
- iso: eng
main_file_link:
- open_access: '1'
url: https://www.researchsquare.com/article/rs-818607/v1
month: '08'
oa: 1
oa_version: Preprint
page: '21'
publication: Research Square
publication_status: submitted
status: public
title: Mechanism of Li2S formation and dissolution in Lithium-Sulphur batteries
tmp:
image: /images/cc_by.png
legal_code_url: https://creativecommons.org/licenses/by/4.0/legalcode
name: Creative Commons Attribution 4.0 International Public License (CC-BY 4.0)
short: CC BY (4.0)
type: preprint
user_id: 8b945eb4-e2f2-11eb-945a-df72226e66a9
year: '2021'
...
---
_id: '9250'
abstract:
- lang: eng
text: Aprotic alkali metal–O2 batteries face two major obstacles to their chemistry
occurring efficiently, the insulating nature of the formed alkali superoxides/peroxides
and parasitic reactions that are caused by the highly reactive singlet oxygen
(1O2). Redox mediators are recognized to be key for improving rechargeability.
However, it is unclear how they affect 1O2 formation, which hinders strategies
for their improvement. Here we clarify the mechanism of mediated peroxide and
superoxide oxidation and thus explain how redox mediators either enhance or suppress
1O2 formation. We show that charging commences with peroxide oxidation to a superoxide
intermediate and that redox potentials above ~3.5 V versus Li/Li+ drive 1O2 evolution
from superoxide oxidation, while disproportionation always generates some 1O2.
We find that 1O2 suppression requires oxidation to be faster than the generation
of 1O2 from disproportionation. Oxidation rates decrease with growing driving
force following Marcus inverted-region behaviour, establishing a region of maximum
rate.
acknowledged_ssus:
- _id: M-Shop
acknowledgement: S.A.F. is indebted to the European Research Council (ERC) under the
European Union’s Horizon 2020 research and innovation programme (grant agreement
No. 636069) as well as IST Austria. O.F thanks the French National Research Agency
(STORE-EX Labex Project ANR-10-LABX-76-01). We thank EL-Cell GmbH (Hamburg, Germany)
for the pressure test cell. We thank R. Saf for help with the mass spectrometry,
J. Schlegl for manufacturing instrumentation, M. Winkler of Acib GmbH, G. Strohmeier
and R. Fürst for HPLC measurements and S. Mondal and S. Stadlbauer for kinetic measurements.
article_processing_charge: No
article_type: original
author:
- first_name: Yann K.
full_name: Petit, Yann K.
last_name: Petit
- first_name: Eléonore
full_name: Mourad, Eléonore
last_name: Mourad
- first_name: Christian
full_name: Prehal, Christian
last_name: Prehal
- first_name: Christian
full_name: Leypold, Christian
last_name: Leypold
- first_name: Andreas
full_name: Windischbacher, Andreas
last_name: Windischbacher
- first_name: Daniel
full_name: Mijailovic, Daniel
last_name: Mijailovic
- first_name: Christian
full_name: Slugovc, Christian
last_name: Slugovc
- first_name: Sergey M.
full_name: Borisov, Sergey M.
last_name: Borisov
- first_name: Egbert
full_name: Zojer, Egbert
last_name: Zojer
- first_name: Sergio
full_name: Brutti, Sergio
last_name: Brutti
- first_name: Olivier
full_name: Fontaine, Olivier
last_name: Fontaine
- first_name: Stefan Alexander
full_name: Freunberger, Stefan Alexander
id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425
last_name: Freunberger
orcid: 0000-0003-2902-5319
citation:
ama: Petit YK, Mourad E, Prehal C, et al. Mechanism of mediated alkali peroxide
oxidation and triplet versus singlet oxygen formation. Nature Chemistry.
2021;13(5):465-471. doi:10.1038/s41557-021-00643-z
apa: Petit, Y. K., Mourad, E., Prehal, C., Leypold, C., Windischbacher, A., Mijailovic,
D., … Freunberger, S. A. (2021). Mechanism of mediated alkali peroxide oxidation
and triplet versus singlet oxygen formation. Nature Chemistry. Springer
Nature. https://doi.org/10.1038/s41557-021-00643-z
chicago: Petit, Yann K., Eléonore Mourad, Christian Prehal, Christian Leypold, Andreas
Windischbacher, Daniel Mijailovic, Christian Slugovc, et al. “Mechanism of Mediated
Alkali Peroxide Oxidation and Triplet versus Singlet Oxygen Formation.” Nature
Chemistry. Springer Nature, 2021. https://doi.org/10.1038/s41557-021-00643-z.
ieee: Y. K. Petit et al., “Mechanism of mediated alkali peroxide oxidation
and triplet versus singlet oxygen formation,” Nature Chemistry, vol. 13,
no. 5. Springer Nature, pp. 465–471, 2021.
ista: Petit YK, Mourad E, Prehal C, Leypold C, Windischbacher A, Mijailovic D, Slugovc
C, Borisov SM, Zojer E, Brutti S, Fontaine O, Freunberger SA. 2021. Mechanism
of mediated alkali peroxide oxidation and triplet versus singlet oxygen formation.
Nature Chemistry. 13(5), 465–471.
mla: Petit, Yann K., et al. “Mechanism of Mediated Alkali Peroxide Oxidation and
Triplet versus Singlet Oxygen Formation.” Nature Chemistry, vol. 13, no.
5, Springer Nature, 2021, pp. 465–71, doi:10.1038/s41557-021-00643-z.
short: Y.K. Petit, E. Mourad, C. Prehal, C. Leypold, A. Windischbacher, D. Mijailovic,
C. Slugovc, S.M. Borisov, E. Zojer, S. Brutti, O. Fontaine, S.A. Freunberger,
Nature Chemistry 13 (2021) 465–471.
corr_author: '1'
date_created: 2021-03-16T11:12:20Z
date_published: 2021-03-15T00:00:00Z
date_updated: 2024-10-09T21:00:28Z
day: '15'
ddc:
- '540'
department:
- _id: StFr
doi: 10.1038/s41557-021-00643-z
external_id:
isi:
- '000629296400001'
pmid:
- '33723377'
file:
- access_level: open_access
checksum: 3ee3f8dd79ed1b7bb0929fce184c8012
content_type: application/pdf
creator: dernst
date_created: 2021-03-22T11:46:00Z
date_updated: 2021-09-16T22:30:03Z
embargo: 2021-09-15
file_id: '9276'
file_name: 2021_NatureChem_Petit_acceptedVersion.pdf
file_size: 1811448
relation: main_file
file_date_updated: 2021-09-16T22:30:03Z
has_accepted_license: '1'
intvolume: ' 13'
isi: 1
issue: '5'
keyword:
- General Chemistry
- General Chemical Engineering
language:
- iso: eng
month: '03'
oa: 1
oa_version: Submitted Version
page: 465-471
pmid: 1
publication: Nature Chemistry
publication_identifier:
eissn:
- 1755-4349
issn:
- 1755-4330
publication_status: published
publisher: Springer Nature
quality_controlled: '1'
scopus_import: '1'
status: public
title: Mechanism of mediated alkali peroxide oxidation and triplet versus singlet
oxygen formation
type: journal_article
user_id: c635000d-4b10-11ee-a964-aac5a93f6ac1
volume: 13
year: '2021'
...
---
_id: '7672'
abstract:
- lang: eng
text: Large overpotentials upon discharge and charge of Li-O2 cells have motivated
extensive research into heterogeneous solid electrocatalysts or non-carbon electrodes
with the aim to improve rate capability, round-trip efficiency and cycle life.
These features are equally governed by parasitic reactions, which are now recognized
to be caused by the highly reactive singlet oxygen (1O2). However, the link between
the presence of electrocatalysts and 1O2 formation in metal-O2 cells is unknown.
Here, we show that, compared to pristine carbon black electrodes, a representative
selection of electrocatalysts or non-carbon electrodes (noble metal, transition
metal compounds) may both slightly reduce or severely increase the 1O2 formation.
The individual reaction steps, where the surfaces impact the 1O2 yield are deciphered,
showing that 1O2 yield from superoxide disproportionation as well as the decomposition
of trace H2O2 are sensitive to catalysts. Transition metal compounds in general
are prone to increase 1O2.
acknowledgement: S.A.F. thanks the International Society of Electrochemistry for awarding
the Tajima Prize 2019 “in recognition of outstanding re- searches on Li-Air batteries
by the use of a range of in-situ elec- trochemical methods to achieve comprehensive
understanding of the reactions taking place at the oxygen electrode”. This article
is dedicated to the special issue of Electrochmica Acta associated with the awarding
conference. S.A.F. is indebted to and the Austrian Federal Ministry of Science,
Research and Economy and the Austrian Research Promotion Agency (grant No. 845364
) and the European Research Council (ERC) under the European Union’s Horizon 2020
research and innovation programme (grant agreement No 636069). The authors thank
J. Schlegl for manufacturing instrumentation, M. Winkler of Acib GmbH and G. Strohmeier
for help with HPLC measurements, S. Eder for cyclic voltammetry measurements, and
C. Slugovc for discussions and continuous support. We thank S. Borisov for access
and advice with fluorescence measurements. We thank EL-Cell GmbH, Hamburg, Germany
for providing the PAT-Cell-Press electrochemical cell.
article_number: '137175'
article_processing_charge: Yes (via OA deal)
article_type: original
author:
- first_name: Aleksej
full_name: Samojlov, Aleksej
last_name: Samojlov
- first_name: David
full_name: Schuster, David
last_name: Schuster
- first_name: Jürgen
full_name: Kahr, Jürgen
last_name: Kahr
- first_name: Stefan Alexander
full_name: Freunberger, Stefan Alexander
id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425
last_name: Freunberger
orcid: 0000-0003-2902-5319
citation:
ama: Samojlov A, Schuster D, Kahr J, Freunberger SA. Surface and catalyst driven
singlet oxygen formation in Li-O2 cells. Electrochimica Acta. 2020;362(12).
doi:10.1016/j.electacta.2020.137175
apa: Samojlov, A., Schuster, D., Kahr, J., & Freunberger, S. A. (2020). Surface
and catalyst driven singlet oxygen formation in Li-O2 cells. Electrochimica
Acta. Elsevier. https://doi.org/10.1016/j.electacta.2020.137175
chicago: Samojlov, Aleksej, David Schuster, Jürgen Kahr, and Stefan Alexander Freunberger.
“Surface and Catalyst Driven Singlet Oxygen Formation in Li-O2 Cells.” Electrochimica
Acta. Elsevier, 2020. https://doi.org/10.1016/j.electacta.2020.137175.
ieee: A. Samojlov, D. Schuster, J. Kahr, and S. A. Freunberger, “Surface and catalyst
driven singlet oxygen formation in Li-O2 cells,” Electrochimica Acta, vol.
362, no. 12. Elsevier, 2020.
ista: Samojlov A, Schuster D, Kahr J, Freunberger SA. 2020. Surface and catalyst
driven singlet oxygen formation in Li-O2 cells. Electrochimica Acta. 362(12),
137175.
mla: Samojlov, Aleksej, et al. “Surface and Catalyst Driven Singlet Oxygen Formation
in Li-O2 Cells.” Electrochimica Acta, vol. 362, no. 12, 137175, Elsevier,
2020, doi:10.1016/j.electacta.2020.137175.
short: A. Samojlov, D. Schuster, J. Kahr, S.A. Freunberger, Electrochimica Acta
362 (2020).
corr_author: '1'
date_created: 2020-04-20T19:29:31Z
date_published: 2020-12-01T00:00:00Z
date_updated: 2024-10-09T20:59:27Z
day: '01'
ddc:
- '540'
department:
- _id: StFr
doi: 10.1016/j.electacta.2020.137175
external_id:
isi:
- '000582869700060'
file:
- access_level: open_access
checksum: 1ab1aa2024d431e2a089ea336bc08298
content_type: application/pdf
creator: dernst
date_created: 2020-10-01T13:20:45Z
date_updated: 2020-10-01T13:20:45Z
file_id: '8593'
file_name: 2020_ElectrochimicaActa_Samojlov.pdf
file_size: 1404030
relation: main_file
success: 1
file_date_updated: 2020-10-01T13:20:45Z
has_accepted_license: '1'
intvolume: ' 362'
isi: 1
issue: '12'
language:
- iso: eng
month: '12'
oa: 1
oa_version: Published Version
publication: Electrochimica Acta
publication_status: published
publisher: Elsevier
quality_controlled: '1'
scopus_import: '1'
status: public
title: Surface and catalyst driven singlet oxygen formation in Li-O2 cells
tmp:
image: /images/cc_by_nc_nd.png
legal_code_url: https://creativecommons.org/licenses/by-nc-nd/4.0/legalcode
name: Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International
(CC BY-NC-ND 4.0)
short: CC BY-NC-ND (4.0)
type: journal_article
user_id: 4359f0d1-fa6c-11eb-b949-802e58b17ae8
volume: 362
year: '2020'
...
---
_id: '7847'
abstract:
- lang: eng
text: 'Water-in-salt electrolytes based on highly concentrated bis(trifluoromethyl)sulfonimide
(TFSI) promise aqueous electrolytes with stabilities nearing 3 V. However, especially
with an electrode approaching the cathodic (reductive) stability, cycling stability
is insufficient. While stability critically relies on a solid electrolyte interphase
(SEI), the mechanism behind the cathodic stability limit remains unclear. Here,
we reveal two distinct reduction potentials for the chemical environments of ''free''
and ''bound'' water and that both contribute to SEI formation. Free-water is reduced
~1V above bound water in a hydrogen evolution reaction (HER) and responsible for
SEI formation via reactive intermediates of the HER; concurrent LiTFSI precipitation/dissolution
establishes a dynamic interface. The free-water population emerges, therefore,
as the handle to extend the cathodic limit of aqueous electrolytes and the battery
cycling stability. '
article_processing_charge: No
article_type: original
author:
- first_name: Roza
full_name: Bouchal, Roza
last_name: Bouchal
- first_name: Zhujie
full_name: Li, Zhujie
last_name: Li
- first_name: Chandra
full_name: Bongu, Chandra
last_name: Bongu
- first_name: Steven
full_name: Le Vot, Steven
last_name: Le Vot
- first_name: Romain
full_name: Berthelot, Romain
last_name: Berthelot
- first_name: Benjamin
full_name: Rotenberg, Benjamin
last_name: Rotenberg
- first_name: Fréderic
full_name: Favier, Fréderic
last_name: Favier
- first_name: Stefan Alexander
full_name: Freunberger, Stefan Alexander
id: A8CA28E6-CE23-11E9-AD2D-EC27E6697425
last_name: Freunberger
orcid: 0000-0003-2902-5319
- first_name: Mathieu
full_name: Salanne, Mathieu
last_name: Salanne
- first_name: Olivier
full_name: Fontaine, Olivier
last_name: Fontaine
citation:
ama: Bouchal R, Li Z, Bongu C, et al. Competitive salt precipitation/dissolution
during free‐water reduction in water‐in‐salt electrolyte. Angewandte Chemie
International Edition. 2020;59(37):15913-1591. doi:10.1002/anie.202005378
apa: Bouchal, R., Li, Z., Bongu, C., Le Vot, S., Berthelot, R., Rotenberg, B., …
Fontaine, O. (2020). Competitive salt precipitation/dissolution during free‐water
reduction in water‐in‐salt electrolyte. Angewandte Chemie International Edition.
Wiley. https://doi.org/10.1002/anie.202005378
chicago: Bouchal, Roza, Zhujie Li, Chandra Bongu, Steven Le Vot, Romain Berthelot,
Benjamin Rotenberg, Fréderic Favier, Stefan Alexander Freunberger, Mathieu Salanne,
and Olivier Fontaine. “Competitive Salt Precipitation/Dissolution during Free‐water
Reduction in Water‐in‐salt Electrolyte.” Angewandte Chemie International Edition.
Wiley, 2020. https://doi.org/10.1002/anie.202005378.
ieee: R. Bouchal et al., “Competitive salt precipitation/dissolution during
free‐water reduction in water‐in‐salt electrolyte,” Angewandte Chemie International
Edition, vol. 59, no. 37. Wiley, pp. 15913–1591, 2020.
ista: Bouchal R, Li Z, Bongu C, Le Vot S, Berthelot R, Rotenberg B, Favier F, Freunberger
SA, Salanne M, Fontaine O. 2020. Competitive salt precipitation/dissolution during
free‐water reduction in water‐in‐salt electrolyte. Angewandte Chemie International
Edition. 59(37), 15913–1591.
mla: Bouchal, Roza, et al. “Competitive Salt Precipitation/Dissolution during Free‐water
Reduction in Water‐in‐salt Electrolyte.” Angewandte Chemie International Edition,
vol. 59, no. 37, Wiley, 2020, pp. 15913–1591, doi:10.1002/anie.202005378.
short: R. Bouchal, Z. Li, C. Bongu, S. Le Vot, R. Berthelot, B. Rotenberg, F. Favier,
S.A. Freunberger, M. Salanne, O. Fontaine, Angewandte Chemie International Edition
59 (2020) 15913–1591.
date_created: 2020-05-14T21:00:30Z
date_published: 2020-09-07T00:00:00Z
date_updated: 2023-09-05T16:02:53Z
day: '07'
ddc:
- '540'
- '546'
department:
- _id: StFr
doi: 10.1002/anie.202005378
external_id:
isi:
- '000541488700001'
pmid:
- '32390281'
file:
- access_level: open_access
checksum: 7b6c2fc20e9b0ff4353352f7a7004e2d
content_type: application/pdf
creator: dernst
date_created: 2020-09-17T08:57:16Z
date_updated: 2020-09-17T08:57:16Z
file_id: '8400'
file_name: 2020_AngChemieINT_Buchal.pdf
file_size: 1966184
relation: main_file
success: 1
file_date_updated: 2020-09-17T08:57:16Z
has_accepted_license: '1'
intvolume: ' 59'
isi: 1
issue: '37'
language:
- iso: eng
month: '09'
oa: 1
oa_version: Published Version
page: 15913-1591
pmid: 1
publication: Angewandte Chemie International Edition
publication_identifier:
eissn:
- 1521-3773
issn:
- 1433-7851
publication_status: published
publisher: Wiley
quality_controlled: '1'
scopus_import: '1'
status: public
title: Competitive salt precipitation/dissolution during free‐water reduction in water‐in‐salt
electrolyte
tmp:
image: /images/cc_by.png
legal_code_url: https://creativecommons.org/licenses/by/4.0/legalcode
name: Creative Commons Attribution 4.0 International Public License (CC-BY 4.0)
short: CC BY (4.0)
type: journal_article
user_id: c635000d-4b10-11ee-a964-aac5a93f6ac1
volume: 59
year: '2020'
...