光催化CO_(2)还原多原子催化剂的设计与制备进展  

Progress in design and preparation of multi-atom catalysts for photocatalytic CO_(2)reduction

作　　者：汪忠浩 邹国军 Jong Hyeok Park 张侃 Zhonghao Wang;Guojun Zou;Jong Hyeok Park;Kan Zhang(School of Materials Science and Engineering and School of Chemistry and Chemical Engineering,Nanjing University of Science and Technology,Nanjing 210094,China;Department of Chemical and Biomolecular Engineering,Yonsei University,50 Yonsei-ro,Seodaemun-gu,Seoul,120-749,Republic of Korea;Chemistry and Chemical Engineering Guangdong Laboratory,Shantou 515031,China)

机构地区：[1]School of Materials Science and Engineering and School of Chemistry and Chemical Engineering,Nanjing University of Science and Technology,Nanjing 210094,China [2]Department of Chemical and Biomolecular Engineering,Yonsei University,50 Yonsei-ro,Seodaemun-gu,Seoul,120-749,Republic of Korea [3]Chemistry and Chemical Engineering Guangdong Laboratory,Shantou 515031,China

出　　处：《Science China Materials》2024年第2期397-423,共27页中国科学（材料科学）（英文版）

基　　金：financially supported by National Natural Science Foundation of China(22172077,T2322013);the Scientific Research Foundation of Chemistry and Chemical Engineering Guangdong Laboratory(2011001);the support by the National Research Foundation of Korea(NRF)funded by the Ministry of Science and ICT(2018M3D1A1058624,2019R1A2C3010479)。

摘　　要：光催化CO_(2)还原合成太阳能燃料对缓解CO_(2)排放引起的全球变暖和降低化石燃料消耗具有重要意义.然而,目前的光催化剂仍然存在反应动力学缓慢和选择性不理想的问题,特别是对于C_(2+)产物的生成,极大地限制了光催化的工业化进程.过去几十年中,关于太阳能驱动的CO_(2)还原的研究展示出鼓舞人心的结果,包括活性位点的构建.本综述重点介绍了通过构建活性位点制备原子级分散催化剂在光催化CO_(2)还原中的最新进展,包括两个独立的活性位点、成对双活性位点和基于活性位点构型的纳米团簇.此外,详细讨论了CO_(2)在活性位点上的活化机制和表征方法.特别是考虑到实验研究与实际应用之间的差距,整合实验和理论的结果,以实现潜在的结构-活性关系和高目标产物选择性发展.最后,概述了该领域存在的挑战,并展望了活性位点的合理设计和机理研究.Photocatalytic CO_(2)reduction towards various fuels is of significant interest under the background of mitigating the global warming induced by CO_(2)emission and lowering the depletion of fossil fuels.However,state-of-the-art photocatalysts still suffer from sluggish reaction dynamics and frustrated product selectivity,especially for C_(2+)generations,which are of great interest for industrial applications.Over the past decades,comprehensive research on solar-driven CO_(2)reduction has consistently unveiled some encouraging results in meaningful pathways and architectural design of active sites over photocatalysts.This review highlights the recent advances in boosting photocatalytic CO_(2)reduction of atomically dispersed catalysts via engineered active sites,including two separated active sites,paired dual-active sites,and nanoclusters based on the configuration of active sites.Both the mechanism of CO_(2)activation over active sites and advanced characterization methods are discussed in detail.Particularly,in consideration of the wide gap between fundamental research and practical applications,the integrations of experimental and theoretical results are analyzed to realize the underlying structure-activity relationships as well as promising selectivity toward target products.Finally,the remaining challenges in the field are outlined,and inquisitive perspectives with a focus on the rational design of active sites and mechanistic investigation are proposed.

关 键 词：photocatalytic CO_(2)reduction precise engineering multiple active sites structure-activity relationships mechanistic investigation 

分 类 号：O643.36[理学—物理化学] O644.1[理学—化学]