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Oxidation kinetics and non-Marcusian charge transfer in dimensionally confined semiconductors
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Xu, Ning, Shi, Li, Pei, Xudong, Zhang, Weiyang, Chen, Jian, Han, Zheng, Samorì, Paolo, Wang, Jinlan, Wang, Peng, Shi, Yi and Li, Songlin (2023) Oxidation kinetics and non-Marcusian charge transfer in dimensionally confined semiconductors. Nature Communications, 14 (1). 4074. doi:10.1038/s41467-023-39781-y ISSN 2041-1723.
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WRAP-oxidation-kinetics-non-Marcusian-charge-transfer-dimensionally-confined-semiconductor-Wang-2023.pdf - Published Version - Requires a PDF viewer. Available under License Creative Commons Attribution 4.0. Download (3781Kb) | Preview |
Official URL: https://doi.org/10.1038/s41467-023-39781-y
Abstract
Electrochemical reactions represent essential processes in fundamental chemistry that foster a wide range of applications. Although most electrochemical reactions in bulk substances can be well described by the classical Marcus-Gerischer charge transfer theory, the realistic reaction character and mechanism in dimensionally confined systems remain unknown. Here, we report the multiparametric survey on the kinetics of lateral photooxidation in structurally identical WS2 and MoS2 monolayers, where electrochemical oxidation occurs at the atomically thin monolayer edges. The oxidation rate is correlated quantitatively with various crystallographic and environmental parameters, including the density of reactive sites, humidity, temperature, and illumination fluence. In particular, we observe distinctive reaction barriers of 1.4 and 0.9 eV for the two structurally identical semiconductors and uncover an unusual non-Marcusian charge transfer mechanism in these dimensionally confined monolayers due to the limit in reactant supplies. A scenario of band bending is proposed to explain the discrepancy in reaction barriers. These results add important knowledge into the fundamental electrochemical reaction theory in low-dimensional systems.
Item Type: | Journal Article | |||||||||||||||||||||||||||
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Subjects: | Q Science > QC Physics Q Science > QD Chemistry T Technology > TK Electrical engineering. Electronics Nuclear engineering |
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Divisions: | Faculty of Science, Engineering and Medicine > Science > Physics | |||||||||||||||||||||||||||
SWORD Depositor: | Library Publications Router | |||||||||||||||||||||||||||
Library of Congress Subject Headings (LCSH): | Electrochemical analysis, Oxidation-reduction reaction, Charge transfer , Semiconductors | |||||||||||||||||||||||||||
Journal or Publication Title: | Nature Communications | |||||||||||||||||||||||||||
Publisher: | Nature Publishing Group | |||||||||||||||||||||||||||
ISSN: | 2041-1723 | |||||||||||||||||||||||||||
Official Date: | 10 July 2023 | |||||||||||||||||||||||||||
Dates: |
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Volume: | 14 | |||||||||||||||||||||||||||
Number: | 1 | |||||||||||||||||||||||||||
Article Number: | 4074 | |||||||||||||||||||||||||||
DOI: | 10.1038/s41467-023-39781-y | |||||||||||||||||||||||||||
Status: | Peer Reviewed | |||||||||||||||||||||||||||
Publication Status: | Published | |||||||||||||||||||||||||||
Access rights to Published version: | Open Access (Creative Commons) | |||||||||||||||||||||||||||
Date of first compliant deposit: | 21 September 2023 | |||||||||||||||||||||||||||
Date of first compliant Open Access: | 25 September 2023 | |||||||||||||||||||||||||||
RIOXX Funder/Project Grant: |
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