Single Carbon Vacancy Traps Atomic Platinum for Hydrogen Evolution Catalysis

被引:228
作者
Yang, Qin [1 ,2 ]
Liu, Hanxuan [3 ]
Yuan, Pei [1 ]
Jia, Yi [2 ]
Zhuang, Linzhou [4 ]
Zhang, Hongwei [1 ]
Yan, Xuecheng [2 ]
Liu, Guihao [5 ]
Zhao, Yufei [5 ]
Liu, Jizi [6 ]
Wei, Shiqiang [7 ]
Song, Li [7 ]
Wu, Qilong [2 ]
Ge, Bingqing [1 ]
Zhang, Longzhou [2 ]
Wang, Kang [2 ]
Wang, Xin [8 ]
Chang, Chun-Ran [3 ]
Yao, Xiangdong [2 ,9 ]
机构
[1] Fuzhou Univ, Coll Chem Engn, Fuzhou 350002, Peoples R China
[2] Griffith Univ, Queensland Micro & Nanotechnol Ctr, Sch Environm & Sci, Nathan, Qld 4111, Australia
[3] Xi An Jiao Tong Univ, Sch Chem Engn & Technol, Xian 710049, Peoples R China
[4] East China Univ Sci & Technol, Sch Chem Engn, Shanghai 200000, Peoples R China
[5] Beijing Univ Chem Technol, State Key Lab Chem Resource Engn, Beijing 100029, Peoples R China
[6] Nanjing Univ Sci & Technol, Hebert Gleiter Inst Nanosci, Sch Mat Sci & Engn, Nanjing 210094, Jiangsu, Peoples R China
[7] Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230029, Peoples R China
[8] Zhejiang Univ Technol, Coll Chem Engn, Hangzhou 310014, Zhejiang, Peoples R China
[9] Jilin Univ, Coll Chem, State Key Lab Inorgan Synth & Preparat Chem, Changchun 130012, Peoples R China
基金
澳大利亚研究理事会; 中国国家自然科学基金;
关键词
X-RAY-ABSORPTION; GRAPHENE; SITES;
D O I
10.1021/jacs.1c10814
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
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-C-3 configuration, which gives exceptionally high reactivity for HER in both acidic and alkaline solutions. The intrinsic activity of Pt-C-3 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-C-3 has a stronger electron-capture ability and lower Gibbs free energy difference (Delta G), resulting in promoting the reduction of adsorbed H+ and the acceleration of H-2 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.
引用
收藏
页码:2171 / 2178
页数:8
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