Dual-Defective Two-Dimensional/Two-Dimensional Z-Scheme Heterojunctions for CO 2 Reduction

作者：Shuwen Cheng, Zhehao Sun, Kang Hui Lim, Ary Anggara Wibowo, Tianxi Zhang, Tao Du, Liying Liu, Hieu Trong Nguyen, Gang Kevin Li, Zongyou Yin, Sibudjing Kawi · 发表于：ACS Catalysis · 年份：2023 · DOI：10.1021/acscatal.3c00219 · 被引用次数：152 · 研究领域：Advanced Photocatalysis Techniques、Perovskite Materials and Applications、Ga2O3 and related materials

The target of photocatalytic CO 2 reduction is to achieve high selectivity, efficiency, and stability for a single chemical/fuel production. The construction of conventional Z-scheme heterojunctions is beneficial to improve the interfacial charge separation and redox capacities. However, the random dimensions of junction component(s) undermine the charge-to-surface transport for catalytic reactions, and the limited chemical structures of catalysts restrict surface activity/selectivity tailoring. In this work, we successfully overcome these issues by stacking/constructing an ultrathin dual-defective two-dimensional (2D)/2D Z-scheme heterojunction with growing functional anionic vacancies onto both reductive and oxidative components of the Z-scheme. The O-vacancy-rich BiOCl/N-vacancy-rich g-C 3 N 4 -based 2D Z-scheme exhibits excellent photoactivity in CO 2 reduction. The rate of CO 2 photoreduction to CO is around 45.33 μmol g –1 h –1, which is 11.7- and 12.2-fold those of untreated bulk g-C 3 N 4 and pristine BiOCl, respectively. Among them, N-vacancy-rich g-C 3 N 4 exhibits active and selective photoreduction ability, accompanied with oxidation reactions from O-vacancy-rich BiOCl. Such ultrathin defective Z-schemes not only retain their original features, i.e., enhanced charge separation and redox capacities, but also extend to lower energy photon absorption and ameliorate charge-to-surface transport in two redox components. Besides, density functional theory calculations un...