Xie Zhongkai, Xu Shengjie, Li Longhua, Gong Shanhe, Wu Xiaojie, Xu Dongbo, Mao Baodong, Zhou Ting, Chen Min, Wang Xiao, Shi Weidong, Song Shuyan
School of Chemistry and Chemical Engineering, Jiangsu University, Zhenjiang, 212013, China.
State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, 130022, China.
Nat Commun. 2024 Mar 18;15(1):2422. doi: 10.1038/s41467-024-46745-3.
Owing to the specific electronic-redistribution and spatial proximity, diatomic catalysts (DACs) have been identified as principal interest for efficient photoconversion of CO into CH. However, the predominant bottom-up strategy for DACs synthesis has critically constrained the development of highly ordered DACs due to the random distribution of heteronuclear atoms, which hinders the optimization of catalytic performance and the exploration of actual reaction mechanism. Here, an up-bottom ion-cutting architecture is proposed to fabricate the well-defined DACs, and the superior spatial proximity of CuAu diatomics (DAs) decorated TiO (CuAu-DAs-TiO) is successfully constructed due to the compact heteroatomic spacing (2-3 Å). Owing to the profoundly low C-C coupling energy barrier of CuAu-DAs-TiO, a considerable CH production with superior sustainability is achieved. Our discovery inspires a novel up-bottom strategy for the fabrication of well-defined DACs to motivate optimization of catalytic performance and distinct deduction of heteroatom synergistically catalytic mechanism.
由于特定的电子再分布和空间邻近性，双原子催化剂（DACs）已被确定为将CO高效光转化为CH的主要研究对象。然而，由于异核原子的随机分布，DACs合成中占主导地位的自下而上策略严重限制了高度有序DACs的发展，这阻碍了催化性能的优化和实际反应机理的探索。在此，提出了一种由上至下的离子切割结构来制备结构明确的DACs，并且由于紧凑的杂原子间距（2-3 Å），成功构建了装饰有CuAu双原子（DAs）的TiO₂（CuAu-DAs-TiO₂）的优异空间邻近性。由于CuAu-DAs-TiO₂的C-C偶联能垒极低，实现了具有卓越可持续性的可观CH产量。我们的发现启发了一种新颖的由上至下策略来制备结构明确的DACs，以推动催化性能的优化和对杂原子协同催化机理的独特推导。
