Atomically-precise dopant-controlled single cluster catalysis for electrochemical nitrogen reduction

Chuanhao Yao, Na Guo, Shibo Xi, Cong-Qiao Xu, Wei Liu, Xiaoxu Zhao, Jing Li, Hanyan Fang, Jie Su, Zhongxin Chen, Huan Yan, Zhizhan Qiu, Pin Lyu, Cheng Chen, Haomin Xu, Xinnan Peng, Xinzhe Li, Bin Liu, Chenliang Su, Stephen J. Pennycook, Cheng-Jun Sun, Jun Li (), Chun Zhang (), Yonghua Du () and Jiong Lu ()
Additional contact information
Chuanhao Yao: National University of Singapore
Na Guo: National University of Singapore
Shibo Xi: Institute of Chemical and Engineering Sciences
Cong-Qiao Xu: Southern University of Science and Technology
Wei Liu: National University of Singapore
Xiaoxu Zhao: National University of Singapore
Jing Li: National University of Singapore
Hanyan Fang: National University of Singapore
Jie Su: National University of Singapore
Zhongxin Chen: National University of Singapore
Huan Yan: National University of Singapore
Zhizhan Qiu: National University of Singapore
Pin Lyu: National University of Singapore
Cheng Chen: National University of Singapore
Haomin Xu: National University of Singapore
Xinnan Peng: National University of Singapore
Xinzhe Li: National University of Singapore
Bin Liu: Nanyang Technological University
Chenliang Su: Shenzhen University
Stephen J. Pennycook: NUS Graduate School for Integrative Sciences and Engineering, National University of Singapore
Cheng-Jun Sun: Argonne National Laboratory
Jun Li: Southern University of Science and Technology
Chun Zhang: National University of Singapore
Yonghua Du: Institute of Chemical and Engineering Sciences
Jiong Lu: National University of Singapore

Nature Communications, 2020, vol. 11, issue 1, 1-10

Abstract: Abstract 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.

Date: 2020
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DOI: 10.1038/s41467-020-18080-w

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