@article{14733,
abstract = {Redox flow batteries (RFBs) rely on the development of cheap, highly soluble, and high-energy-density electrolytes. Several candidate quinones have already been investigated in the literature as two-electron anolytes or catholytes, benefiting from fast kinetics, high tunability, and low cost. Here, an investigation of nitrogen-rich fused heteroaromatic quinones was carried out to explore avenues for electrolyte development. These quinones were synthesized and screened by using electrochemical techniques. The most promising candidate, 4,8-dioxo-4,8-dihydrobenzo[1,2-d:4,5-d′]bis([1,2,3]triazole)-1,5-diide (−0.68 V(SHE)), was tested in both an asymmetric and symmetric full-cell setup resulting in capacity fade rates of 0.35% per cycle and 0.0124% per cycle, respectively. In situ ultraviolet-visible spectroscopy (UV–Vis), nuclear magnetic resonance (NMR), and electron paramagnetic resonance (EPR) spectroscopies were used to investigate the electrochemical stability of the charged species during operation. UV–Vis spectroscopy, supported by density functional theory (DFT) modeling, reaffirmed that the two-step charging mechanism observed during battery operation consisted of two, single-electron transfers. The radical concentration during battery operation and the degree of delocalization of the unpaired electron were quantified with NMR and EPR spectroscopy.},
author = {Jethwa, Rajesh B and Hey, Dominic and Kerber, Rachel N. and Bond, Andrew D. and Wright, Dominic S. and Grey, Clare P.},
issn = {2574-0962},
journal = {ACS Applied Energy Materials},
keywords = {Electrical and Electronic Engineering, Materials Chemistry, Electrochemistry, Energy Engineering and Power Technology, Chemical Engineering (miscellaneous)},
number = {2},
pages = {414--426},
publisher = {American Chemical Society},
title = {{Exploring the landscape of heterocyclic quinones for redox flow batteries}},
doi = {10.1021/acsaem.3c02223},
volume = {7},
year = {2024},
}
@article{14828,
abstract = {Production of hydrogen at large scale requires development of non-noble, inexpensive, and high-performing catalysts for constructing water-splitting devices. Herein, we report the synthesis of Zn-doped NiO heterostructure (ZnNiO) catalysts at room temperature via a coprecipitation method followed by drying (at 80 °C, 6 h) and calcination at an elevated temperature of 400 °C for 5 h under three distinct conditions, namely, air, N2, and vacuum. The vacuum-synthesized catalyst demonstrates a low overpotential of 88 mV at −10 mA cm–2 and a small Tafel slope of 73 mV dec–1 suggesting relatively higher charge transfer kinetics for hydrogen evolution reactions (HER) compared with the specimens synthesized under N2 or O2 atmosphere. It also demonstrates an oxygen evolution (OER) overpotential of 260 mV at 10 mA cm–2 with a low Tafel slope of 63 mV dec–1. In a full-cell water-splitting device, the vacuum-synthesized ZnNiO heterostructure demonstrates a cell voltage of 1.94 V at 50 mA cm–2 and shows remarkable stability over 24 h at a high current density of 100 mA cm–2. It is also demonstrated in this study that Zn-doping, surface, and interface engineering in transition-metal oxides play a crucial role in efficient electrocatalytic water splitting. Also, the results obtained from density functional theory (DFT + U = 0–8 eV), where U is the on-site Coulomb repulsion parameter also known as Hubbard U, based electronic structure calculations confirm that Zn doping constructively modifies the electronic structure, in both the valence band and the conduction band, and found to be suitable in tailoring the carrier’s effective masses of electrons and holes. The decrease in electron’s effective masses together with large differences between the effective masses of electrons and holes is noticed, which is found to be mainly responsible for achieving the best water-splitting performance from a 9% Zn-doped NiO sample prepared under vacuum.},
author = {Kiran, Gundegowda Kalligowdanadoddi and Singh, Saurabh and Mahato, Neelima and Sreekanth, Thupakula Venkata Madhukar and Dillip, Gowra Raghupathy and Yoo, Kisoo and Kim, Jonghoon},
issn = {2574-0962},
journal = {ACS Applied Energy Materials},
keywords = {Electrical and Electronic Engineering, Materials Chemistry, Electrochemistry, Energy Engineering and Power Technology, Chemical Engineering (miscellaneous)},
number = {1},
pages = {214--229},
publisher = {American Chemical Society},
title = {{Interface engineering modulation combined with electronic structure modification of Zn-doped NiO heterostructure for efficient water-splitting activity}},
doi = {10.1021/acsaem.3c02519},
volume = {7},
year = {2024},
}
@article{14831,
abstract = {Catalysis, the acceleration of product formation by a substance that is left unchanged, typically results from multiple elementary processes, including diffusion of the reactants toward the catalyst, chemical steps, and release of the products. While efforts to design catalysts are often focused on accelerating the chemical reaction on the catalyst, catalysis is a global property of the catalytic cycle that involves all processes. These are controlled by both intrinsic parameters such as the composition and shape of the catalyst and extrinsic parameters such as the concentration of the chemical species at play. We examine here the conditions that catalysis imposes on the different steps of a reaction cycle and the respective role of intrinsic and extrinsic parameters of the system on the emergence of catalysis by using an approach based on first-passage times. We illustrate this approach for various decompositions of a catalytic cycle into elementary steps, including non-Markovian decompositions, which are useful when the presence and nature of intermediate states are a priori unknown. Our examples cover different types of reactions and clarify the constraints on elementary steps and the impact of species concentrations on catalysis.},
author = {Sakref, Yann and Muñoz Basagoiti, Maitane and Zeravcic, Zorana and Rivoire, Olivier},
issn = {1520-5207},
journal = {The Journal of Physical Chemistry B},
keywords = {Materials Chemistry, Surfaces, Coatings and Films, Physical and Theoretical Chemistry},
number = {51},
pages = {10950--10959},
publisher = {American Chemical Society},
title = {{On kinetic constraints that catalysis imposes on elementary processes}},
doi = {10.1021/acs.jpcb.3c04627},
volume = {127},
year = {2023},
}
@article{12227,
abstract = {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.},
author = {Kovačič, Sebastijan and Schafzahl, Bettina and Matsko, Nadejda B. and Gruber, Katharina and Schmuck, Martin and Koller, Stefan and Freunberger, Stefan Alexander and Slugovc, Christian},
issn = {2574-0962},
journal = {ACS Applied Energy Materials},
keywords = {Electrical and Electronic Engineering, Materials Chemistry, Electrochemistry, Energy Engineering and Power Technology, Chemical Engineering (miscellaneous)},
number = {11},
pages = {14381--14390},
publisher = {American Chemical Society},
title = {{Carbon foams via ring-opening metathesis polymerization of emulsion templates: A facile method to make carbon current collectors for battery applications}},
doi = {10.1021/acsaem.2c02787},
volume = {5},
year = {2022},
}
@article{13347,
abstract = {Confining molecules within well-defined nanosized spaces can profoundly alter their physicochemical characteristics. For example, the controlled aggregation of chromophores into discrete oligomers has been shown to tune their optical properties whereas encapsulation of reactive species within molecular hosts can increase their stability. The resazurin/resorufin pair has been widely used for detecting redox processes in biological settings; yet, how tight confinement affects the properties of these two dyes remains to be explored. Here, we show that a flexible PdII6L4 coordination cage can efficiently encapsulate both resorufin and resazurin in the form of dimers, dramatically modulating their optical properties. Furthermore, binding within the cage significantly decreases the reduction rate of resazurin to resorufin, and the rate of the subsequent reduction of resorufin to dihydroresorufin. During our studies, we also found that upon dilution, the PdII6L4 cage disassembles to afford PdII2L2 species, which lacks the ability to form inclusion complexes – a process that can be reversed upon the addition of the strongly binding resorufin/resazurin guests. We expect that the herein disclosed ability of a water-soluble cage to reversibly modulate the optical and chemical properties of a molecular redox probe will expand the versatility of synthetic fluorescent probes in biologically relevant environments.},
author = {Yanshyna, Oksana and Białek, Michał J. and Chashchikhin, Oleg V. and Klajn, Rafal},
issn = {2399-3669},
journal = {Communications Chemistry},
keywords = {Materials Chemistry, Biochemistry, Environmental Chemistry, General Chemistry},
publisher = {Springer Nature},
title = {{Encapsulation within a coordination cage modulates the reactivity of redox-active dyes}},
doi = {10.1038/s42004-022-00658-8},
volume = {5},
year = {2022},
}
@article{13350,
abstract = {Confinement within molecular cages can dramatically modify the physicochemical properties of the encapsulated guest molecules, but such host-guest complexes have mainly been studied in a static context. Combining confinement effects with fast guest exchange kinetics could pave the way toward stimuli-responsive supramolecular systems—and ultimately materials—whose desired properties could be tailored “on demand” rapidly and reversibly. Here, we demonstrate rapid guest exchange between inclusion complexes of an open-window coordination cage that can simultaneously accommodate two guest molecules. Working with two types of guests, anthracene derivatives and BODIPY dyes, we show that the former can substantially modify the optical properties of the latter upon noncovalent heterodimer formation. We also studied the light-induced covalent dimerization of encapsulated anthracenes and found large effects of confinement on reaction rates. By coupling the photodimerization with the rapid guest exchange, we developed a new way to modulate fluorescence using external irradiation.},
author = {Gemen, Julius and Białek, Michał J. and Kazes, Miri and Shimon, Linda J.W. and Feller, Moran and Semenov, Sergey N. and Diskin-Posner, Yael and Oron, Dan and Klajn, Rafal},
issn = {2451-9294},
journal = {Chem},
keywords = {Materials Chemistry, Biochemistry (medical), General Chemical Engineering, Environmental Chemistry, Biochemistry, General Chemistry},
number = {9},
pages = {2362--2379},
publisher = {Elsevier},
title = {{Ternary host-guest complexes with rapid exchange kinetics and photoswitchable fluorescence}},
doi = {10.1016/j.chempr.2022.05.008},
volume = {8},
year = {2022},
}
@article{13351,
abstract = {Molecular recognition is at the heart of the noncovalent synthesis of supramolecular assemblies and, at higher length scales, supramolecular materials. In a recent publication in Nature, Stoddart and co-workers demonstrate that the formation of host-guest complexes can be catalyzed by one of the simplest possible catalysts: the electron.},
author = {Gemen, Julius and Klajn, Rafal},
issn = {2451-9294},
journal = {Chem},
keywords = {Materials Chemistry, Biochemistry (medical), General Chemical Engineering, Environmental Chemistry, Biochemistry, General Chemistry},
number = {5},
pages = {1183--1186},
publisher = {Elsevier},
title = {{Electron catalysis expands the supramolecular chemist’s toolbox}},
doi = {10.1016/j.chempr.2022.04.022},
volume = {8},
year = {2022},
}
@article{13353,
abstract = {We show that the optical properties of indigo carmine can be modulated by encapsulation within a coordination cage. Depending on the host/guest molar ratio, the cage can predominantly encapsulate either one or two dye molecules. The 1 : 1 complex is fluorescent, unique for an indigo dye in an aqueous solution. We have also found that binding two dye molecules stabilizes a previously unknown conformation of the cage.},
author = {Yanshyna, Oksana and Avram, Liat and Shimon, Linda J. W. and Klajn, Rafal},
issn = {1364-548X},
journal = {Chemical Communications},
keywords = {Materials Chemistry, Metals and Alloys, Surfaces, Coatings and Films, General Chemistry, Ceramics and Composites, Electronic, Optical and Magnetic Materials, Catalysis},
number = {21},
pages = {3461--3464},
publisher = {Royal Society of Chemistry},
title = {{Coexistence of 1:1 and 2:1 inclusion complexes of indigo carmine}},
doi = {10.1039/d1cc07081a},
volume = {58},
year = {2022},
}
@article{12237,
abstract = {Thermoelectric technology requires synthesizing complex materials where not only the crystal structure but also other structural features such as defects, grain size and orientation, and interfaces must be controlled. To date, conventional solid-state techniques are unable to provide this level of control. Herein, we present a synthetic approach in which dense inorganic thermoelectric materials are produced by the consolidation of well-defined nanoparticle powders. The idea is that controlling the characteristics of the powder allows the chemical transformations that take place during consolidation to be guided, ultimately yielding inorganic solids with targeted features. Different from conventional methods, syntheses in solution can produce particles with unprecedented control over their size, shape, crystal structure, composition, and surface chemistry. However, to date, most works have focused only on the low-cost benefits of this strategy. In this perspective, we first cover the opportunities that solution processing of the powder offers, emphasizing the potential structural features that can be controlled by precisely engineering the inorganic core of the particle, the surface, and the organization of the particles before consolidation. We then discuss the challenges of this synthetic approach and more practical matters related to solution processing. Finally, we suggest some good practices for adequate knowledge transfer and improving reproducibility among different laboratories.},
author = {Fiedler, Christine and Kleinhanns, Tobias and Garcia, Maria and Lee, Seungho and Calcabrini, Mariano and Ibáñez, Maria},
issn = {1520-5002},
journal = {Chemistry of Materials},
keywords = {Materials Chemistry, General Chemical Engineering, General Chemistry},
number = {19},
pages = {8471--8489},
publisher = {American Chemical Society},
title = {{Solution-processed inorganic thermoelectric materials: Opportunities and challenges ∇}},
doi = {10.1021/acs.chemmater.2c01967},
volume = {34},
year = {2022},
}
@article{13359,
abstract = {Dissipative self-assembly is ubiquitous in nature, where it gives rise to complex structures and functions such as self-healing, homeostasis, and camouflage. These phenomena are enabled by the continuous conversion of energy stored in chemical fuels, such as ATP. Over the past decade, an increasing number of synthetic chemically driven systems have been reported that mimic the features of their natural counterparts. At the same time, it has been shown that dissipative self-assembly can also be fueled by light; these optically fueled systems have been developed in parallel to the chemically fueled ones. In this perspective, we critically compare these two classes of systems. Despite the complementarity and fundamental differences between these two modes of dissipative self-assembly, our analysis reveals that multiple analogies exist between chemically and light-fueled systems. We hope that these considerations will facilitate further development of the field of dissipative self-assembly.},
author = {Weißenfels, Maren and Gemen, Julius and Klajn, Rafal},
issn = {2451-9294},
journal = {Chem},
keywords = {Materials Chemistry, Biochemistry (medical), General Chemical Engineering, Environmental Chemistry, Biochemistry, General Chemistry},
number = {1},
pages = {23--37},
publisher = {Elsevier},
title = {{Dissipative self-assembly: Fueling with chemicals versus light}},
doi = {10.1016/j.chempr.2020.11.025},
volume = {7},
year = {2021},
}
@article{15260,
abstract = {Significant advances in the synthesis and processing of colloidal nanocrystals have given scientists and engineers access to a vast library of building blocks with precisely defined size, shape, and composition. These materials have inspired exciting prospects to enable bottom-up fabrication of programmable materials with properties by design. Successfully assembling and connecting the building blocks into superstructures in which constituent nanocrystals can purposefully interact requires robust understanding of and control over a complex interplay of dynamic physicochemical processes. Fluid interfaces provide an advantageous experimental workbench to both probe and control these processes. Despite the ostensible simplicity of fabricating nanocrystal assemblies at a fluid interface, sensitivity to processing conditions and limited reproducibility have underscored the complexity of this process. In situ studies have provided mechanistic insights into the competing dynamics of key subprocesses including solvent spreading and evaporation, superlattice formation, ligand detachment kinetics, and nanocrystal attachment. Understanding how these subprocesses influence the complex choreography of self-assembly, structure transformation, and oriented attachment processes presents a rich research challenge. In this context, we present a detailed methodology for self-assembly and attachment of lead chalcogenide nanocrystals at a liquid–gas interface as a model system for the fabrication of mono- and multilayer cubic connected superlattices. We discuss key experimental parameters such as the characteristics of the building blocks and processing conditions and detailed steps from colloidal nanocrystal injection to superlattice transfer. We hope that this Methods/Protocols paper will provide guidance for future advances in the exciting path toward bringing the prospect of nanocrystal-based programmable materials to fruition.},
author = {Cimada daSilva, Jessica and Balazs, Daniel and Dunbar, Tyler A. and Hanrath, Tobias},
issn = {1520-5002},
journal = {Chemistry of Materials},
keywords = {Materials Chemistry, General Chemical Engineering, General Chemistry},
number = {24},
pages = {9457--9472},
publisher = {American Chemical Society},
title = {{Fundamental processes and practical considerations of lead chalcogenide mesocrystals formed via self-assembly and directed attachment of nanocrystals at a fluid interface}},
doi = {10.1021/acs.chemmater.1c02910},
volume = {33},
year = {2021},
}
@article{15265,
abstract = {The highly enhanced thermoelectric figure of merit, zT ≈ 2.6 at 573 K, obtained recently in Cd-doped polycrystalline AgSbTe2 by Roychowdhury et al. ( Science 2021, 371, 722) brings it to the forefront of thermoelectric and energy materials research. Ag/Sb cationic ordering in polycrystalline AgSbTe2 was a challenging issue for a long time: their ordered arrangement in the cationic sublattice in polycrystalline samples remained elusive despite multiple theoretical predictions and experimental studies. Recently, selective cation doping has been used to enhance the Ag/Sb ordering, and cation ordered nanoscale (2–4 nm) domains were observed in polycrystalline AgSbTe2, which reduce lattice thermal conductivity. The enhanced cation ordering also delocalizes disorder-induced localized electronic states, and consequently the electronic transport enhances. In this Focus Review, we provide the details of the rational design of a high-performance thermoelectric material using the recently developed atomic order–disorder optimization strategy with AgSbTe2 as an example. Atomic disorder is ubiquitous in most thermoelectric materials, and the atomic order–disorder optimization strategy applies to a large variety of thermoelectric materials.},
author = {Ghosh, Tanmoy and Roychowdhury, Subhajit and Dutta, Moinak and Biswas, Kanishka},
issn = {2380-8195},
journal = {ACS Energy Letters},
keywords = {Materials Chemistry, Energy Engineering and Power Technology, Fuel Technology, Renewable Energy, Sustainability and the Environment, Chemistry (miscellaneous)},
number = {8},
pages = {2825--2837},
publisher = {American Chemical Society},
title = {{High-performance thermoelectric energy conversion: A tale of atomic ordering in AgSbTe2}},
doi = {10.1021/acsenergylett.1c01184},
volume = {6},
year = {2021},
}
@article{9447,
abstract = {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.},
author = {Maffre, Marion and Bouchal, Roza and Freunberger, Stefan Alexander and Lindahl, Niklas and Johansson, Patrik and Favier, Frédéric and Fontaine, Olivier and Bélanger, Daniel},
issn = {1945-7111},
journal = {Journal of The Electrochemical Society},
keywords = {Renewable Energy, Sustainability and the Environment, Electrochemistry, Materials Chemistry, Electronic, Optical and Magnetic Materials, Surfaces, Coatings and Films, Condensed Matter Physics},
number = {5},
publisher = {IOP Publishing},
title = {{Investigation of electrochemical and chemical processes occurring at positive potentials in “Water-in-Salt” electrolytes}},
doi = {10.1149/1945-7111/ac0300},
volume = {168},
year = {2021},
}
@article{13371,
abstract = {Diamondoid nanoporous crystals represent a synthetically challenging class of materials that typically have been obtained from tetrahedral building blocks. In this issue of Chem, Stoddart and coworkers demonstrate that it is possible to generate diamondoid frameworks from a hexacationic building block lacking a tetrahedral symmetry. These results highlight the great potential of self-assembly for rapidly transforming small molecules into structurally complex functional materials.},
author = {Białek, Michał J. and Klajn, Rafal},
issn = {2451-9294},
journal = {Chem},
keywords = {Materials Chemistry, Biochemistry (medical), General Chemical Engineering, Environmental Chemistry, Biochemistry, General Chemistry},
number = {9},
pages = {2283--2285},
publisher = {Elsevier},
title = {{Diamond grows up}},
doi = {10.1016/j.chempr.2019.08.012},
volume = {5},
year = {2019},
}
@article{13379,
author = {Bléger, David and Klajn, Rafal},
issn = {1521-3927},
journal = {Macromolecular Rapid Communications},
keywords = {Materials Chemistry, Polymers and Plastics, Organic Chemistry},
number = {1},
publisher = {Wiley},
title = {{Integrating macromolecules with molecular switches}},
doi = {10.1002/marc.201700827},
volume = {39},
year = {2018},
}
@article{15107,
author = {Roy, Soumendu and Roy, Sumit and Rao, Anish and Devatha, Gayathri and Pillai, Pramod P.},
issn = {1520-5002},
journal = {Chemistry of Materials},
keywords = {Materials Chemistry, General Chemical Engineering, General Chemistry},
number = {23},
pages = {8415--8419},
publisher = {American Chemical Society},
title = {{Precise nanoparticle–reactant interaction outplays ligand poisoning in visible-light photocatalysis}},
doi = {10.1021/acs.chemmater.8b03108},
volume = {30},
year = {2018},
}
@article{10357,
abstract = {The misfolding and aggregation of proteins into linear fibrils is widespread in human biology, for example, in connection with amyloid formation and the pathology of neurodegenerative disorders such as Alzheimer’s and Parkinson’s diseases. The oligomeric species that are formed in the early stages of protein aggregation are of great interest, having been linked with the cellular toxicity associated with these conditions. However, these species are not characterized in any detail experimentally, and their properties are not well understood. Many of these species have been found to have approximately spherical morphology and to be held together by hydrophobic interactions. We present here an analytical statistical mechanical model of globular oligomer formation from simple idealized amphiphilic protein monomers and show that this correlates well with Monte Carlo simulations of oligomer formation. We identify the controlling parameters of the model, which are closely related to simple quantities that may be fitted directly from experiment. We predict that globular oligomers are unlikely to form at equilibrium in many polypeptide systems but instead form transiently in the early stages of amyloid formation. We contrast the globular model of oligomer formation to a well-established model of linear oligomer formation, highlighting how the differing ensemble properties of linear and globular oligomers offer a potential strategy for characterizing oligomers from experimental measurements.},
author = {Dear, Alexander J. and Šarić, Anđela and Michaels, Thomas C. T. and Dobson, Christopher M. and Knowles, Tuomas P. J.},
issn = {1520-5207},
journal = {The Journal of Physical Chemistry B},
keywords = {materials chemistry},
number = {49},
pages = {11721--11730},
publisher = {American Chemical Society},
title = {{Statistical mechanics of globular oligomer formation by protein molecules}},
doi = {10.1021/acs.jpcb.8b07805},
volume = {122},
year = {2018},
}
@article{8453,
abstract = {Transverse relaxation rate measurements in magic-angle spinning solid-state nuclear magnetic resonance provide information about molecular motions occurring on nanosecond-to-millisecond (ns–ms) time scales. The measurement of heteronuclear (13C, 15N) relaxation rate constants in the presence of a spin-lock radiofrequency field (R1ρ relaxation) provides access to such motions, and an increasing number of studies involving R1ρ relaxation in proteins have been reported. However, two factors that influence the observed relaxation rate constants have so far been neglected, namely, (1) the role of CSA/dipolar cross-correlated relaxation (CCR) and (2) the impact of fast proton spin flips (i.e., proton spin diffusion and relaxation). We show that CSA/D CCR in R1ρ experiments is measurable and that the CCR rate constant depends on ns–ms motions; it can thus provide insight into dynamics. We find that proton spin diffusion attenuates this CCR due to its decoupling effect on the doublet components. For measurements of dynamics, the use of R1ρ rate constants has practical advantages over the use of CCR rates, and this article reveals factors that have so far been disregarded and which are important for accurate measurements and interpretation.},
author = {Kurauskas, Vilius and Weber, Emmanuelle and Hessel, Audrey and Ayala, Isabel and Marion, Dominique and Schanda, Paul},
issn = {1520-6106},
journal = {The Journal of Physical Chemistry B},
keywords = {Physical and Theoretical Chemistry, Materials Chemistry, Surfaces, Coatings and Films},
number = {34},
pages = {8905--8913},
publisher = {American Chemical Society},
title = {{Cross-correlated relaxation of dipolar coupling and chemical-shift anisotropy in magic-angle spinning R1ρ NMR measurements: Application to protein backbone dynamics measurements}},
doi = {10.1021/acs.jpcb.6b06129},
volume = {120},
year = {2016},
}
@article{8455,
abstract = {Solid-state NMR spectroscopy allows the characterization of the structure, interactions and dynamics of insoluble and/or very large proteins. Sensitivity and resolution are often major challenges for obtaining atomic-resolution information, in particular for very large protein complexes. Here we show that the use of deuterated, specifically CH3-labelled proteins result in significant sensitivity gains compared to previously employed CHD2 labelling, while line widths increase only marginally. We apply this labelling strategy to a 468 kDa-large dodecameric aminopeptidase, TET2, and the 1.6 MDa-large 50S ribosome subunit of Thermus thermophilus.},
author = {Kurauskas, Vilius and Crublet, Elodie and Macek, Pavel and Kerfah, Rime and Gauto, Diego F. and Boisbouvier, Jérôme and Schanda, Paul},
issn = {1359-7345},
journal = {Chemical Communications},
keywords = {Materials Chemistry, Electronic, Optical and Magnetic Materials, General Chemistry, Surfaces, Coatings and Films, Metals and Alloys, Ceramics and Composites, Catalysis},
number = {61},
pages = {9558--9561},
publisher = {Royal Society of Chemistry},
title = {{Sensitive proton-detected solid-state NMR spectroscopy of large proteins with selective CH3labelling: Application to the 50S ribosome subunit}},
doi = {10.1039/c6cc04484k},
volume = {52},
year = {2016},
}
@article{13395,
abstract = {Metallic nanoparticles co-functionalised with monolayers of UV- and CO2-sensitive ligands were prepared and shown to respond to these two types of stimuli reversibly and in an orthogonal fashion. The composition of the coating could be tailored to yield nanoparticles capable of aggregating exclusively when both UV and CO2 were applied at the same time, analogously to the behaviour of an AND logic gate.},
author = {Lee, Ji-Woong and Klajn, Rafal},
issn = {1364-548X},
journal = {Chemical Communications},
keywords = {Materials Chemistry, Metals and Alloys, Surfaces, Coatings and Films, General Chemistry, Ceramics and Composites, Electronic, Optical and Magnetic Materials, Catalysis},
number = {11},
pages = {2036--2039},
publisher = {Royal Society of Chemistry},
title = {{Dual-responsive nanoparticles that aggregate under the simultaneous action of light and CO2}},
doi = {10.1039/c4cc08541h},
volume = {51},
year = {2015},
}