Atomically-precise dopant-controlled single cluster catalysis for electrochemical nitrogen reduction
| Autor: | Pin Lyu, Chun Zhang, Xinzhe Li, Jun Li, Chuanhao Yao, Na Guo, Cheng-Jun Sun, Stephen J. Pennycook, Zhizhan Qiu, Wei Liu, Cong-Qiao Xu, Shibo Xi, Bin Liu, Zhongxin Chen, Huan Yan, Jiong Lu, Chenliang Su, Cheng Chen, Jie Su, Haomin Xu, Jing Li, Xiaoxu Zhao, Xinnan Peng, Hanyan Fang, Yonghua Du |
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| Jazyk: | angličtina |
| Rok vydání: | 2020 |
| Předmět: |
0301 basic medicine
Materials science Catalyst synthesis Science Heteroatom General Physics and Astronomy 02 engineering and technology General Biochemistry Genetics and Molecular Biology Article Catalysis law.invention Bimetal 03 medical and health sciences law Cluster (physics) lcsh:Science HOMO/LUMO Bimetallic strip Heterogeneous catalysis Multidisciplinary Dopant Graphene General Chemistry 021001 nanoscience & nanotechnology 030104 developmental biology Chemical engineering lcsh:Q 0210 nano-technology Electrocatalysis |
| Zdroj: | Nature Communications, Vol 11, Iss 1, Pp 1-10 (2020) Nature Communications |
| ISSN: | 2041-1723 |
| Popis: | The ability to precisely engineer the doping of sub-nanometer bimetallic clusters offers exciting opportunities for tailoring their catalytic performance with atomic accuracy. However, the fabrication of singly dispersed bimetallic cluster catalysts with atomic-level control of dopants has been a long-standing challenge. Herein, we report a strategy for the controllable synthesis of a precisely doped single cluster catalyst consisting of partially ligand-enveloped Au4Pt2 clusters supported on defective graphene. This creates a bimetal single cluster catalyst (Au4Pt2/G) with exceptional activity for electrochemical nitrogen (N2) reduction. Our mechanistic study reveals that each N2 molecule is activated in the confined region between cluster and graphene. The heteroatom dopant plays an indispensable role in the activation of N2 via an enhanced back donation of electrons to the N2 LUMO. Moreover, besides the heteroatom Pt, the catalytic performance of single cluster catalyst can be further tuned by using Pd in place of Pt as the dopant. The fabrication of singly dispersed metal cluster catalysts with atomic-level control of dopants is a long-standing challenge. Here, the authors report a strategy for the synthesis of a precisely doped single cluster catalyst which shows exceptional activity for electrochemical dinitrogen reduction. |
| Databáze: | OpenAIRE |
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