Oxidation kinetics and non-Marcusian charge transfer in dimensionally confined semiconductors

Ning Xu, Li Shi, Xudong Pei, Weiyang Zhang, Jian Chen, Zheng Han, Paolo Samorì, Jinlan Wang (), Peng Wang (), Yi Shi () and Songlin Li ()
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Ning Xu: Nanjing University
Li Shi: Southeast University
Xudong Pei: Nanjing University
Weiyang Zhang: Nanjing University
Jian Chen: Nanjing University
Zheng Han: Shanxi University
Paolo Samorì: University of Strasbourg, CNRS, ISIS UMR 7006
Jinlan Wang: Southeast University
Peng Wang: University of Warwick
Yi Shi: Nanjing University
Songlin Li: Nanjing University

Nature Communications, 2023, vol. 14, issue 1, 1-9

Abstract: 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.

Date: 2023
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DOI: 10.1038/s41467-023-39781-y

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