Regulating the Coordination Environment of Ruthenium Cluster Catalysts for the Alkaline Hydrogen Evolution Reaction

Tong Liu; Wei Zhang; Tao Chen; Dong Liu; Linlin Cao; Tao Ding; Xiaokang Liu; Beibei Pang; Sicong Wang; Lan Wang; Qiquan Luo; Tao Yao

doi:10.1021/acs.jpclett.1c01936

Regulating the Coordination Environment of Ruthenium Cluster Catalysts for the Alkaline Hydrogen Evolution Reaction

J Phys Chem Lett. 2021 Aug 26;12(33):8016-8023. doi: 10.1021/acs.jpclett.1c01936. Epub 2021 Aug 17.

Authors

Tong Liu¹, Wei Zhang², Tao Chen^{1

3}, Dong Liu¹, Linlin Cao¹, Tao Ding¹, Xiaokang Liu¹, Beibei Pang¹, Sicong Wang¹, Lan Wang¹, Qiquan Luo⁴, Tao Yao¹

Affiliations

¹ National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230029, China.
² School of Materials, Sun Yat-sen University, Guangzhou 510275, Guangdong, China.
³ School of National Defense Science and Technology, Southwest University of Science and Technology, Mianyang 621010, China.
⁴ Institutes of Physical Science and Information Technology, Anhui University, Hefei 230601, China.

PMID: 34433277
DOI: 10.1021/acs.jpclett.1c01936

Abstract

Exploring high-efficiency catalysts for the electrochemical hydrogen evolution reaction (HER) in alkaline environments is attractive but remains challenging. Here we report a coordination regulation strategy to tune the atomic structure of Ru cluster catalysts supported on Ti₃C₂T_x MXene (Ru-Ti₃C₂T_x) for the HER. We identify that the coordination number (CN) of Ru-Ru could be slightly regulated from 2.1 to 2.8 by adjusting the synthesized temperature so as to achieve an optimal catalytic configuration. The Ru-Ti₃C₂T_x with a CN_Ru-Ru of 2.8 exhibits the best catalytic activity with a low overpotential of 96 mV at 10 mA cm^-2 and a mass activity about 11.5 times greater than the commercial Pt/C catalyst. Density functional theory calculations demonstrated that the small Ru clusters have a stronger covalent interaction with Ti₃C₂T_x support leading to an optimal ΔG_H* value. This work opens up a general avenue to modulate the coordination environment of catalysts for the HER.