Single Carbon Vacancy Traps Atomic Platinum for Hydrogen Evolution Catalysis

Qin Yang; Hanxuan Liu; Pei Yuan; Yi Jia; Linzhou Zhuang; Hongwei Zhang; Xuecheng Yan; Guihao Liu; Yufei Zhao; Jizi Liu; Shiqiang Wei; Li Song; Qilong Wu; Bingqing Ge; Longzhou Zhang; Kang Wang; Xin Wang; Chun-Ran Chang; Xiangdong Yao

doi:10.1021/jacs.1c10814

Single Carbon Vacancy Traps Atomic Platinum for Hydrogen Evolution Catalysis

J Am Chem Soc. 2022 Feb 9;144(5):2171-2178. doi: 10.1021/jacs.1c10814. Epub 2022 Jan 7.

Authors

Qin Yang^{1

2}, Hanxuan Liu³, Pei Yuan¹, Yi Jia², Linzhou Zhuang⁴, Hongwei Zhang¹, Xuecheng Yan², Guihao Liu⁵, Yufei Zhao⁵, Jizi Liu⁶, Shiqiang Wei⁷, Li Song⁷, Qilong Wu², Bingqing Ge¹, Longzhou Zhang², Kang Wang², Xin Wang⁸, Chun-Ran Chang³, Xiangdong Yao^{2

9}

Affiliations

¹ College of Chemical Engineering, Fuzhou University, Fuzhou 350002, P.R. China.
² School of Environment and Science, Queensland Micro- and Nanotechnology Centre, Griffith University, Nathan, Queensland 4111, Australia.
³ School of Chemical Engineering and Technology, Xi'an Jiao Tong University, Xi'an 710049, P.R. China.
⁴ School of Chemical Engineering, East China University of Science and Technology, Shanghai 200000, P.R. China.
⁵ State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, P.R. China.
⁶ Hebert Gleiter Institute of Nanoscience, School of Materials Science and Engineering, Nanjing University of Science and Technology, Jiangsu 210094, P.R. China.
⁷ National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230029, P.R. China.
⁸ College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, Zhejiang 310014, P.R. China.
⁹ State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, P.R. China.

PMID: 34995077
DOI: 10.1021/jacs.1c10814

Abstract

The coordinated configuration of atomic platinum (Pt) has always been identified as an active site with high intrinsic activity for hydrogen evolution reaction (HER). Herein, we purposely synthesize single vacancies in a carbon matrix (defective graphene) that can trap atomic Pt to form the Pt-C₃ configuration, which gives exceptionally high reactivity for HER in both acidic and alkaline solutions. The intrinsic activity of Pt-C₃ site is valued with a turnover frequency (TOF) of 26.41 s^-1 and mass activity of 26.05 A g^-1 at 100 mV, respectively, which are both nearly 18 times higher than those of commercial 20 wt % Pt/C. It is revealed that the optimal coordination Pt-C₃ has a stronger electron-capture ability and lower Gibbs free energy difference (ΔG), resulting in promoting the reduction of adsorbed H⁺ and the acceleration of H₂ desorption, thus exhibiting the extraordinary HER activity. This work provides a new insight on the unique coordinated configuration of dispersive atomic Pt in defective C matrix for superior HER performance.