Article Anomalous Interfacial Electron-Transfer Kinetics in Twisted Trilayer Graphene Caused by Layer-Specific Localization

Kaidi Zhang ; Yun Yu ; Stephen Carr ; Mohammad Babar ; Ziyan Zhu ; Bryan Junsuh Kim ; Catherine Groschner ; Nikta Khaloo ; Takashi Taniguchi SAMURAI ORCID (National Institute for Materials Science) ; Kenji Watanabe SAMURAI ORCID (National Institute for Materials Science) ; Venkatasubramanian Viswanathan ; D. Kwabena Bediako

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Kaidi Zhang, Yun Yu, Stephen Carr, Mohammad Babar, Ziyan Zhu, Bryan Junsuh Kim, Catherine Groschner, Nikta Khaloo, Takashi Taniguchi, Kenji Watanabe, Venkatasubramanian Viswanathan, D. Kwabena Bediako. Anomalous Interfacial Electron-Transfer Kinetics in Twisted Trilayer Graphene Caused by Layer-Specific Localization. ACS Central Science. 2023, 9 (6), 1119-1128. https://doi.org/10.1021/acscentsci.3c00326
SAMURAI

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(abstract)

Interfacial electron-transfer (ET) reactions underpin the interconversion of electrical and chem- ical energy. Pioneering experiments showed that the ET rate depends on the Fermi–Dirac dis- tribution of the electronic density of states (DOS) of the electrode, formalized in the Marcus– Hush–Chidsey (MHC) model. Here, by controlling interlayer twists in well-defined trilayer graphene moir ́es, we show that ET rates are strikingly dependent on electronic localization in each atomic layer, and not the overall DOS. The large degree of tunability inherent to moir ́e electrodes leads to local ET kinetics that range over three orders of magnitude across different constructions of only three atomic layers, even exceeding rates at bulk metals. Our results demonstrate that beyond the ensemble DOS, electronic localization is critical in facilitating interfacial ET, with implications for understanding the origin of high interfacial reactivity typ- ically exhibited by defects at electrode–electrolyte interfaces.

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Keyword: Interfacial electron-transfer, trilayer graphene, electronic localization

Date published: 2023-06-28

Publisher: American Chemical Society (ACS)

Journal:

  • ACS Central Science (ISSN: 23747943) vol. 9 issue. 6 p. 1119-1128

Funding:

  • Gordon and Betty Moore Foundation 10637
  • W. M. Keck Foundation 993922
  • Office of Naval Research N00014-18-S-F009
  • Office of Naval Research N00014-20-1-2599
  • Japan Society for the Promotion of Science 19H05790
  • Japan Society for the Promotion of Science 20H00354
  • Japan Society for the Promotion of Science 21H05233
  • U.S. Department of Energy DE-AC02-05CH11231
  • U.S. Department of Energy DE-SC0021049
  • 3M Foundation 67507585
  • Canadian Institute for Advanced Research GS21-011
  • National Science Foundation OIA-1921199

Manuscript type: Publisher's version (Version of record)

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First published URL: https://doi.org/10.1021/acscentsci.3c00326

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Updated at: 2025-02-26 08:30:33 +0900

Published on MDR: 2025-02-26 08:30:33 +0900

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