Zhang Longzhou, Jia Yi, Liu Hongli, Zhuang Linzhou, Yan Xuecheng, Lang Chengguang, Wang Xin, Yang Dongjiang, Huang Keke, Feng Shouhua, Yao Xiangdong
School of Environment and Science and Queensland Micro- and Nanotechnology Centre, Griffith University, Nathan Campus, Queensland, 4111, Australia.
School of Materials Science and Engineering and Yunnan Key Laboratory for Micro/nano Materials & Technology, Yunnan University, Kunming, Yunnan, 650091, P. R. China.
Angew Chem Int Ed Engl. 2019 Jul 8;58(28):9404-9408. doi: 10.1002/anie.201902107. Epub 2019 Jun 24.
Atomic metal species-based catalysts (AMCs) show remarkable possibilities in various catalytic reactions. The coordination configuration of the metal atoms has been widely recognized as the determining factor to the electronic structure and the catalytic activity. However, the synergistic effect between the adjacent layers of the multilayered AMCs is always neglected. We reported an atomic Co and Pt co-trapped carbon catalyst, which exhibits a ultrahigh activity for HER in the wide range of pH (η =27 and 50 mV in acidic and alkaline media, respectively) with ultralow metal loadings (1.72 and 0.16 wt % for Co and Pt, respectively), which is much superior to the commercial Pt/C. Theoretical analysis reveals that the atomic metals on the inner graphitic layers significantly alter the electronic structure of the outmost layer, thus tailoring the HER activity. This finding arouses a re-thinking of the intrinsic activity origins of AMCs and suggests a new avenue in the structure design of AMCs.
基于原子金属物种的催化剂（AMCs）在各种催化反应中展现出显著的潜力。金属原子的配位构型已被广泛认为是决定电子结构和催化活性的因素。然而，多层AMCs相邻层之间的协同效应一直被忽视。我们报道了一种原子钴和铂共捕获的碳催化剂，该催化剂在宽pH范围内对析氢反应表现出超高活性（在酸性和碱性介质中，过电位分别为27和50 mV），且金属负载量极低（钴和铂的负载量分别为1.72和0.16 wt %），远优于商业Pt/C。理论分析表明，内部石墨层上的原子金属显著改变了最外层的电子结构，从而调整了析氢反应活性。这一发现引发了对AMCs本征活性起源的重新思考，并为AMCs的结构设计提供了一条新途径。
