金属相1T-MoS2/ZnIn2S4异质结调控电荷传输从而促进光催化氧化还原反应

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中文摘要：近年来,光催化产氢与有机物氧化的偶联反应备受关注,如何设计高效双功能光催化剂实现偶联反应成为研究重点.在众多光催化剂中,ZnIn2S4以其优异的可见光吸收能力、本征的极化电场以及较强的氧化还原能力成为双功能催化剂的热点备选材料.然而,电子空穴分离效率低以及光生电子空穴复合率高的问题限制了ZnIn2S4光电转化效率的进一步提高.针对这一问题,我们采用了具有较高导电性和独特结构的金属相1T-MoS2作为助催化剂与花状ZnIn2S4复合形成"海胆状"的1T-MoS2/ZnIn2S4欧姆结复合材料.理论计算结合XPS数据揭示了欧姆结与内建电场的形成,一系列光谱表征表明由欧姆结所形成的强内建电场促进了ZnIn2S4体内光生电子快速向1T-MoS2转移,同时活性测试与EPR表征证明了苯甲醇的氧化反应可以作为光生空穴的有效捕获剂.最终,1T-MoS2/ZnIn2S4复合光催化剂实现了4.6倍光催化性能的提高,420 nm波长下表光量子效率达6.75％.本项工作通过精确调节电荷转移机制,实现了ZnIn2S4双功能催化剂光电效率的进一步提高,为光催化剂载流子调控设计提供了新思路.

外文标题：Metallic 1T-MoS2/ZnIn2S4 heterojunction photocatalysts for enhanced photoredox reaction via guiding charge migration

外文摘要：The synergistic coupling of photocatalytic hy-drogen evolution and α-C-H bond activation reactions en-ables the comprehensive harnessing of the redox potential of semiconductor catalysts,yielding exceptionally high utiliza-tion of photocatalytic technology.Guiding and optimizing the charge migration within photocatalysts constitute a pivotal strategy for achieving remarkable overall solar energy con-version efficiency.Here,we engineer metallic 1T-MoS2/ZnIn2S4 heterojunction photocatalysts by incorporating the distinctive 1T-MoS2 structure into the intricate flower-like ZnIn2S4 framework.The modulation of charge migration within the 1T-MoS2/ZnIn2S4 heterojunction photocatalysts is induced by an engineered interfacial electric field and an ef-ficient hole transfer agent(benzyl alcohol).Steering charge migration results in an impressive 4.6-fold enhancement in photocatalytic performance compared with the pristine ZnIn2S4.Moreover,comprehensive spectroscopy and theore-tical analyses prove that the interfacial electric field facilitates the rapid electron transfer along the direction from the[S-Mo]to[In-S]layers.Simultaneously,swift hole capture is achieved by dehydrogenating the α-C-H bond in benzyl al-cohol.

外文关键词：

metallic 1T-MoS2heterojunction photocatalystphotocatalytic hydrogen evolutionbenzyl alcohol oxidationguiding charge migration

作者：

张洪文、姚雪、山巍、刘玥、唐华

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作者单位：

School of Environmental Science and Engineering,Qingdao University,Qingdao 266071,China

School of Materials Science and Engineering,Jiangsu University,Zhenjiang 212013,China

关键词：

metallic 1T-MoS2 heterojunction photocatalyst photocatalytic hydrogen evolution benzyl alcohol oxidation guiding charge migration

基金：

National Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaTechnology Support Program for the Youth Innovation Team of Shandong Higher Education InstitutionsTaishan Youth Scholar Program of Shandong Province

项目编号：

2197511022378219223021062023KJ225

出版年：

2024

DOI：

10.1007/s40843-023-2769-8

中国科学:材料科学(英文)

CSTPCD

ISSN：

年,卷(期)：2024.67(2)

参考文献量76