Engineering the Electronic Structure of Submonolayer Pt on Intermetallic Pd3Pb via Charge Transfer Boosts the Hydrogen Evolution Reaction

被引:123
作者
Yao, Yancai [1 ]
Gu, Xiang-Kui [4 ]
He, Dongsheng [5 ]
Li, Zhijun [6 ]
Liu, Wei [7 ]
Xu, Qian [7 ]
Yao, Tao [7 ]
Lin, Yue [1 ]
Wang, Hui-Juan [1 ]
Zhao, Changming [1 ]
Wang, Xiaoqian [1 ]
Yin, Peiqun [1 ]
Li, Hai [8 ,9 ]
Hong, Xun [1 ]
Wei, Shiqiang [7 ]
Li, Wei-Xue [1 ]
Li, Yadong [1 ,2 ,3 ]
Wu, Yuen [1 ]
机构
[1] Univ Sci & Technol China, iChEM Collaborat Innovat Ctr Chem Energy Mat, Hefei Natl Lab Phys Sci Microscale, Dept Chem, Hefei 230026, Anhui, Peoples R China
[2] Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
[3] Tsinghua Univ, Collaborat Innovat Ctr Nanomat Sci & Engn, Beijing 100084, Peoples R China
[4] Wuhan Univ, Sch Power & Mech Engn, Wuhan 430072, Hubei, Peoples R China
[5] Southern Univ Sci & Technol SUSTech, MCPC, Shenzhen 518055, Guangdong, Peoples R China
[6] Northeast Petr Univ, Coll Chem & Chem Engn, Prov Key Lab Oil & Gas Chem Technol, Daqing 163318, Peoples R China
[7] Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230026, Anhui, Peoples R China
[8] Nanjing Univ Technol, KLOFE, Nanjing 211816, Jiangsu, Peoples R China
[9] Nanjing Univ Technol, IAM, Jiangsu Natl Synerget Innovat Ctr Adv Mat SICAM, Nanjing 211816, Jiangsu, Peoples R China
基金
中国国家自然科学基金; 国家重点研发计划;
关键词
SINGLE-CRYSTAL SURFACES; ELECTROCHEMISTRY; CATALYSTS;
D O I
10.1021/jacs.9b09391
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The efficient electrochemical hydrogen evolution reaction (HER) plays a key role in accelerating sustainable H-2 production from water electrolysis, but its large-scale applications are hindered by the high cost of the state-of-the-art Pt catalyst. In this work, submonolayer Pt was controllably deposited on an intermetallic Pd3Pb nanoplate (AL-Pt/Pd3Pb). The atomic efficiency and electronic structure of the active surface Pt layer were largely optimized, greatly enhancing the acidic HER. AL-Pt/Pd3Pb exhibits an outstanding HER activity with an overpotential of only 13.8 mV at 10 mA/cm(2) and a high mass activity of 7834 A/g(Pd+Pt) at -0.05 V, both largely surpassing those of commercial Pt/C (30 mV, 1486 A/g(Pt)). In addition, AL-Pt/Pd3Pb shows excellent stability and robustness. Theoretical calculations show that the improved activity is mainly derived from the charge transfer from Pd3Pb to Pt, resulting in a strong electrostatic interaction that can stabilize the transition state and lower the barrier.
引用
收藏
页码:19964 / 19968
页数:5
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