ReS 2 Nanosheets with In Situ Formed Sulfur Vacancies for Efficient and Highly Selective Photocatalytic CO 2 Reduction
ReS 2 Nanosheets with In Situ Formed Sulfur Vacancies for Efficient and Highly Selective Photocatalytic CO 2 Reduction
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DOI：
10.1002/smsc.202000052
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发表时间：
2020-12
期刊：
影响因子：
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通讯作者：
Yanzhao Zhang;Dazhi Yao;Bingquan Xia;Haolan Xu;Youhong Tang;K. Davey;J. Ran;S. Qiao
中科院分区：
文献类型：
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作者：
Yanzhao Zhang;Dazhi Yao;Bingquan Xia;Haolan Xu;Youhong Tang;K. Davey;J. Ran;S. Qiao
人工光合作用可以提供有价值的燃料，并通过使用基于半导体的光催化剂将二氧化碳（CO2）和水（H2O）转化为碳氢化合物来积极影响温室效应。然而，低效率的电荷载体解离和运输以及缺乏表面活性位点是提高其在光催化CO2还原中的活性和选择性的两个主要缺点。近年来，ReS 2由于其独特的物理化学性质而受到了人们的广泛关注。然而，ReS 2在光催化还原CO2中的应用却很少被报道。本文报道了ReS 2纳米片和CdS纳米颗粒之间形成的异质结，实现了7.1 μmol g− 1的明显提高的CO产量和93.4%的高选择性。所制备的ReS 2/CdS异质结表现出增强的可见光吸收、高效的电子-空穴对分离/转移以及在原位产生的ReS 2硫空位上增加的CO2吸附/活化/还原，因此都有利于CO2光还原。这些都得到了先进的表征技术的证实，例如，基于同步加速器的X射线吸收近边结构和基于密度泛函理论的计算。这些发现将在催化、电子学和光电子学中应用的表面活性位点和半导体异质结的实际设计和制造中具有广泛的意义。
Artificial photosynthesis can provide valuable fuels and positively impact greenhouse effects, via transforming carbon dioxide (CO2) and water (H2O) into hydrocarbons using semiconductor‐based photocatalysts. However, the inefficient charge‐carrier dissociation and transportation as well as the lack of surface active sites are two major drawbacks to boosting their activity and selectivity in photocatalytic CO2reduction. Recently, ReS2has received tremendous attention in the photocatalysis area due to its intriguing physicochemical properties. Nevertheless, the application of ReS2in photocatalytic CO2reduction is scarcely covered. Herein, a heterojunction formed between ReS2nanosheets and CdS nanoparticles is reported, achieving an apparently raised CO production of 7.1 μmol g−1and high selectivity of 93.4%. The as‐prepared ReS2/CdS heterojunction exhibits strengthened visible‐light absorption, high‐efficiency electron–hole pair separation/transfer, and increased adsorption/activation/reduction of CO2on in situ created sulfur vacancies of ReS2, thus all favoring CO2photoreduction. These are corroborated by advanced characterization techniques, e.g., synchrotron‐based X‐ray absorption near‐edge structure, and density functional theory–based computations. The findings will be of broad interest in practical design and fabrication of surface active sites and semiconductor heterojunctions for applications in catalysis, electronics, and optoelectronics.