用于电催化CO_(2)还原的新兴双原子位点催化剂(DASCs)

Emerging dual-atomic-site catalysts for electrocatalytic CO_(2)reduction

用于生产高附加值燃料和化学品的电化学CO_(2)还原反应(CO_(2)RR)为实现全球碳中和提供了一种有前景的方法.近年来,单原子催化剂(SACs)由于金属的最大原子利用率和独特的催化性能受到越来越多的关注.相比之下,除了具有单原子催化剂的上述优点外,双原子位点催化剂(DASCs)还可以通过调节另一种相邻金属从而实现更复杂、可调的原子结构.作为SAC的更深层次的延伸,DASCs可以为CO_(2)RR带来新的机遇,最近引起了人们的浓厚兴趣.本文中,我们重点介绍了DASCs在提升CO_(2)RR性能方面的最新进展.首先,根据双原子活性位点的几何结构和电子配置,对DASCs的分类、合成和证实进行了讨论.之后,根据结合型、异核和同核双原子位点对DASCs在CO_(2)RR中的催化应用进行了分类.特别是通过系统地分析反应途径和原子结构,详细总结了DASCs在CO_(2)RR中的构效关系.最后,提出了未来设计DASCs面临的机遇和挑战,以启发设计具有高结构精度和高CO_(2)RR活性、选择性的DASCs.

The electrochemical CO_(2)reduction reaction(CO_(2)RR)to yield high-value added fuels and chemicals provides a promising approach towards global carbon neutrality.Constant endeavors have been devoted to the exploration of high-efficiency catalyst with rapid reaction kinetics,low energy input,and high selectivity.In addition to the maximum metal atomic utilization and unique catalytic performance of single-atom catalyst(SAC),dual-atomic-site catalysts(DASCs)offer more sophisticated and tunable atomic structure through the modulations of another adjacent metal atom,which can bring new opportunities for CO_(2)RR as a deeper extension of SACs and have recently aroused surging interest.In this review,we highlight the recent advances on DASCs for enhancing CO_(2)RR.First,the classification,synthesis,and identification of DASCs are provided according to the geometric structure and electronic configuration of dual-atomic active sites.Then,the catalytic applications of DASCs in CO_(2)RR are categorized based on marriage-type,hetero-nuclear,and homo-nuclear dual-atomic sites.Particularly,the structure-activity relationship of DASCs in CO_(2)RR is elaborately summarized through systematically analyzing the reaction pathways and the atom structures.Finally,the opportunities and challenges are proposed for inspiring the design of future DASCs with high structural accuracy and high CO_(2)RR activity and selectivity.