---
_id: '13216'
abstract:
- lang: eng
  text: Physical catalysts often have multiple sites where reactions can take place.
    One prominent example is single-atom alloys, where the reactive dopant atoms can
    preferentially locate in the bulk or at different sites on the surface of the
    nanoparticle. However, ab initio modeling of catalysts usually only considers
    one site of the catalyst, neglecting the effects of multiple sites. Here, nanoparticles
    of copper doped with single-atom rhodium or palladium are modeled for the dehydrogenation
    of propane. Single-atom alloy nanoparticles are simulated at 400–600 K, using
    machine learning potentials trained on density functional theory calculations,
    and then the occupation of different single-atom active sites is identified using
    a similarity kernel. Further, the turnover frequency for all possible sites is
    calculated for propane dehydrogenation to propene through microkinetic modeling
    using density functional theory calculations. The total turnover frequencies of
    the whole nanoparticle are then described from both the population and the individual
    turnover frequency of each site. Under operating conditions, rhodium as a dopant
    is found to almost exclusively occupy (111) surface sites while palladium as a
    dopant occupies a greater variety of facets. Undercoordinated dopant surface sites
    are found to tend to be more reactive for propane dehydrogenation compared to
    the (111) surface. It is found that considering the dynamics of the single-atom
    alloy nanoparticle has a profound effect on the calculated catalytic activity
    of single-atom alloys by several orders of magnitude.
acknowledgement: "B.C. acknowledges resources provided by the Cambridge Tier2 system
  operated by the University of Cambridge Research\r\nComputing Service funded by
  EPSRC Tier-2 capital grant EP/\r\nP020259/1."
article_processing_charge: Yes (via OA deal)
article_type: original
author:
- first_name: Rhys
  full_name: Bunting, Rhys
  id: 91deeae8-1207-11ec-b130-c194ad5b50c6
  last_name: Bunting
  orcid: 0000-0001-6928-074X
- first_name: Felix
  full_name: Wodaczek, Felix
  id: 8b4b6a9f-32b0-11ee-9fa8-bbe85e26258e
  last_name: Wodaczek
  orcid: 0009-0000-1457-795X
- first_name: Tina
  full_name: Torabi, Tina
  last_name: Torabi
- first_name: Bingqing
  full_name: Cheng, Bingqing
  id: cbe3cda4-d82c-11eb-8dc7-8ff94289fcc9
  last_name: Cheng
  orcid: 0000-0002-3584-9632
citation:
  ama: 'Bunting R, Wodaczek F, Torabi T, Cheng B. Reactivity of single-atom alloy
    nanoparticles: Modeling the dehydrogenation of propane. <i>Journal of the American
    Chemical Society</i>. 2023;145(27):14894-14902. doi:<a href="https://doi.org/10.1021/jacs.3c04030">10.1021/jacs.3c04030</a>'
  apa: 'Bunting, R., Wodaczek, F., Torabi, T., &#38; Cheng, B. (2023). Reactivity
    of single-atom alloy nanoparticles: Modeling the dehydrogenation of propane. <i>Journal
    of the American Chemical Society</i>. American Chemical Society. <a href="https://doi.org/10.1021/jacs.3c04030">https://doi.org/10.1021/jacs.3c04030</a>'
  chicago: 'Bunting, Rhys, Felix Wodaczek, Tina Torabi, and Bingqing Cheng. “Reactivity
    of Single-Atom Alloy Nanoparticles: Modeling the Dehydrogenation of Propane.”
    <i>Journal of the American Chemical Society</i>. American Chemical Society, 2023.
    <a href="https://doi.org/10.1021/jacs.3c04030">https://doi.org/10.1021/jacs.3c04030</a>.'
  ieee: 'R. Bunting, F. Wodaczek, T. Torabi, and B. Cheng, “Reactivity of single-atom
    alloy nanoparticles: Modeling the dehydrogenation of propane,” <i>Journal of the
    American Chemical Society</i>, vol. 145, no. 27. American Chemical Society, pp.
    14894–14902, 2023.'
  ista: 'Bunting R, Wodaczek F, Torabi T, Cheng B. 2023. Reactivity of single-atom
    alloy nanoparticles: Modeling the dehydrogenation of propane. Journal of the American
    Chemical Society. 145(27), 14894–14902.'
  mla: 'Bunting, Rhys, et al. “Reactivity of Single-Atom Alloy Nanoparticles: Modeling
    the Dehydrogenation of Propane.” <i>Journal of the American Chemical Society</i>,
    vol. 145, no. 27, American Chemical Society, 2023, pp. 14894–902, doi:<a href="https://doi.org/10.1021/jacs.3c04030">10.1021/jacs.3c04030</a>.'
  short: R. Bunting, F. Wodaczek, T. Torabi, B. Cheng, Journal of the American Chemical
    Society 145 (2023) 14894–14902.
corr_author: '1'
date_created: 2023-07-12T09:16:40Z
date_published: 2023-06-30T00:00:00Z
date_updated: 2024-10-21T06:01:30Z
day: '30'
ddc:
- '540'
department:
- _id: MaIb
- _id: BiCh
doi: 10.1021/jacs.3c04030
external_id:
  isi:
  - '001020623900001'
  pmid:
  - '37390457'
file:
- access_level: open_access
  checksum: e07d5323f9c0e5cbd1ad6453f29440ab
  content_type: application/pdf
  creator: cchlebak
  date_created: 2023-07-12T10:22:04Z
  date_updated: 2023-07-12T10:22:04Z
  file_id: '13219'
  file_name: 2023_JACS_Bunting.pdf
  file_size: 3155843
  relation: main_file
  success: 1
file_date_updated: 2023-07-12T10:22:04Z
has_accepted_license: '1'
intvolume: '       145'
isi: 1
issue: '27'
keyword:
- Colloid and Surface Chemistry
- Biochemistry
- General Chemistry
- Catalysis
language:
- iso: eng
license: https://creativecommons.org/licenses/by/4.0/
month: '06'
oa: 1
oa_version: Published Version
page: 14894-14902
pmid: 1
publication: Journal of the American Chemical Society
publication_identifier:
  eissn:
  - 1520-5126
  issn:
  - 0002-7863
publication_status: published
publisher: American Chemical Society
quality_controlled: '1'
scopus_import: '1'
status: public
title: 'Reactivity of single-atom alloy nanoparticles: Modeling the dehydrogenation
  of propane'
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: 8b945eb4-e2f2-11eb-945a-df72226e66a9
volume: 145
year: '2023'
...