Jia Guangri, Zhang Yingchuan, Yu Jimmy C, Guo Zhengxiao
Department of Chemistry and HKU-CAS Joint Laboratory on New Materials, The University of Hong Kong, Hong Kong SAR, 999077, P. R. China.
Department of Chemistry, The Chinese University of Hong Kong, Shatin, New Territories, Hong Kong SAR, 999077, P. R. China.
Adv Mater. 2024 Sep;36(38):e2403153. doi: 10.1002/adma.202403153. Epub 2024 Jul 23.
Atomically dispersed active sites in a photocatalyst offer unique advantages such as locally tuned electronic structures, quantum size effects, and maximum utilization of atomic species. Among these, asymmetric atomic dual-sites are of particular interest because their asymmetric charge distribution generates a local built-in electric potential to enhance charge separation and transfer. Moreover, the dual sites provide flexibility for tuning complex multielectron and multireaction pathways, such as CO reduction reactions. The coordination of dual sites opens new possibilities for engineering the structure-activity-selectivity relationship. This comprehensive overview discusses efficient and sustainable photocatalysis processes in photocatalytic CO reduction, focusing on strategic active-site design and future challenges. It serves as a timely reference for the design and development of photocatalytic conversion processes, specifically exploring the utilization of asymmetric atomic dual-sites for complex photocatalytic conversion pathways, here exemplified by the conversion of CO into valuable chemicals.
光催化剂中原子级分散的活性位点具有独特优势,如局部可调谐的电子结构、量子尺寸效应以及原子物种的最大利用率。其中,不对称原子双位点尤其引人关注,因为其不对称电荷分布会产生局部内建电势,以增强电荷分离和转移。此外,双位点为调节复杂的多电子和多反应途径(如CO还原反应)提供了灵活性。双位点的配位为构建结构-活性-选择性关系开辟了新的可能性。本综述讨论了光催化CO还原中高效且可持续的光催化过程,重点关注战略性活性位点设计及未来挑战。它为光催化转化过程的设计和开发提供了及时的参考,特别探讨了利用不对称原子双位点实现复杂光催化转化途径,此处以将CO转化为有价值的化学品为例。