Yang Jingyi, Huang Yike, Qi Haifeng, Zeng Chaobin, Jiang Qike, Cui Yitao, Su Yang, Du Xiaorui, Pan Xiaoli, Liu Xiaoyan, Li Weizhen, Qiao Botao, Wang Aiqin, Zhang Tao
CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China.
University of Chinese Academy of Sciences, Beijing, 100049, China.
Nat Commun. 2022 Jul 22;13(1):4244. doi: 10.1038/s41467-022-31966-1.
Metal-support interaction predominately determines the electronic structure of metal atoms in single-atom catalysts (SACs), largely affecting their catalytic performance. However, directly tuning the metal-support interaction in oxide supported SACs remains challenging. Here, we report a new strategy to subtly regulate the strong covalent metal-support interaction (CMSI) of Pt/CoFeO SACs by a simple water soaking treatment. Detailed studies reveal that the CMSI is weakened by the bonding of H, generated from water dissociation, onto the interface of Pt-O-Fe, resulting in reduced charge transfer from metal to support and leading to an increase of C-H bond activation in CH combustion by more than 50 folds. This strategy is general and can be extended to other CMSI-existed metal-supported catalysts, providing a powerful tool to modulating the catalytic performance of SACs.
金属-载体相互作用在很大程度上决定了单原子催化剂（SACs）中金属原子的电子结构，对其催化性能有很大影响。然而，直接调控氧化物负载型SACs中的金属-载体相互作用仍然具有挑战性。在此，我们报道了一种新策略，通过简单的水浸泡处理来巧妙调节Pt/CoFeO SACs的强共价金属-载体相互作用（CMSI）。详细研究表明，由水离解产生的H键合到Pt-O-Fe界面上会削弱CMSI，导致从金属到载体的电荷转移减少，并使CH燃烧中C-H键活化增加50多倍。该策略具有通用性，可扩展到其他存在CMSI的金属负载型催化剂，为调节SACs的催化性能提供了有力工具。
