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用于加速光催化析氢动力学的原位形成 ZnIn S/MoTiC 肖特基结:局部配位和电子结构的调控。

In Situ Formation ZnIn S /Mo TiC Schottky Junction for Accelerating Photocatalytic Hydrogen Evolution Kinetics: Manipulation of Local Coordination and Electronic Structure.

机构信息

Shanxi Key Laboratory of Compound Air Pollutions Identification and Control College of Environmental Science and Engineering, Taiyuan University of Technology, Taiyuan, 030024, P. R. China.

College of Chemical Engineering and Technology, Taiyuan University of Technology, Taiyuan, 030024, P. R. China.

出版信息

Small. 2023 Jun;19(24):e2300717. doi: 10.1002/smll.202300717. Epub 2023 Mar 15.

DOI:10.1002/smll.202300717
PMID:36919813
Abstract

Regulating electronic structures of the active site by manipulating the local coordination is one of the advantageous means to improve photocatalytic hydrogen evolution (PHE) kinetics. Herein, the ZnIn S /Mo TiC Schottky junctions are designed to be constructed through the interfacial local coordination of In with the electronegative O terminal group on Mo TiC based on the different work functions. Kelvin probe force microscopy and charge density difference reveal that an electronic unidirectional transport channel across the Schottky interface from ZnIn S to Mo TiC is established by the formed local nucleophilic/electrophilic region. The increased local electron density of Mo TiC inhibits the backflow of electrons, boosts the charge transfer and separation, and optimizes the hydrogen adsorption energy. Therefore, the ZnIn S /Mo TiC photocatalyst exhibits a superior PHE rate of 3.12 mmol g h under visible light, reaching 3.03 times that of the pristine ZnIn S . This work provides some insights and inspiration for preparing MXene-based Schottky catalysts to accelerate PHE kinetics.

摘要

通过调控活性位点的局域配位来调节电子结构是提高光催化产氢(PHE)动力学的有利手段之一。在此,基于不同的功函数,通过在 MoTiC 上的电负性 O 端基与 In 的界面局域配位,设计了 ZnInS/MoTiC 肖特基结。通过 Kelvin 探针力显微镜和电荷密度差研究发现,通过形成的局部亲核/亲电区域,在肖特基界面上建立了从 ZnInS 到 MoTiC 的电子单向输运通道。MoTiC 局部电子密度的增加抑制了电子的回流,促进了电荷转移和分离,并优化了氢的吸附能。因此,ZnInS/MoTiC 光催化剂在可见光下表现出优越的 PHE 速率为 3.12mmol g h ,达到原始 ZnInS 的 3.03 倍。这项工作为制备基于 MXene 的肖特基催化剂以加速 PHE 动力学提供了一些见解和启示。

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