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

Yancai Yao; Xiang-Kui Gu; Dongsheng He; Zhijun Li; Wei Liu; Qian Xu; Tao Yao; Yue Lin; Hui-Juan Wang; Changming Zhao; Xiaoqian Wang; Peiqun Yin; Hai Li; Xun Hong; Shiqiang Wei; Wei-Xue Li; Yadong Li; Yuen Wu

doi:10.1021/jacs.9b09391

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

J Am Chem Soc. 2019 Dec 26;141(51):19964-19968. doi: 10.1021/jacs.9b09391. Epub 2019 Dec 10.

Authors

Yancai Yao¹, Xiang-Kui Gu², Dongsheng He³, Zhijun Li⁴, Wei Liu⁵, Qian Xu⁵, Tao Yao⁵, Yue Lin¹, Hui-Juan Wang¹, Changming Zhao¹, Xiaoqian Wang¹, Peiqun Yin¹, Hai Li⁶, Xun Hong¹, Shiqiang Wei⁵, Wei-Xue Li¹, Yadong Li^{1

7}, Yuen Wu¹

Affiliations

¹ Department of Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials) , University of Science and Technology of China , Hefei 230026 , China.
² School of Power and Mechanical Engineering , Wuhan University , Wuhan 430072 , China.
³ Materials Characterization and Preparation Center (MCPC) , Southern University of Science and Technology (SUSTech) , Shenzhen 518055 , China.
⁴ Provincial Key Laboratory of Oil & Gas Chemical Technology, College of Chemistry and Chemical Engineering , Northeast Petroleum University , Daqing 163318 , China.
⁵ National Synchrotron Radiation Laboratory , University of Science and Technology of China , Hefei 230026 , China.
⁶ Key Laboratory of Flexible Electronics (KLOFE) and Institute of Advanced Materials (IAM), Jiangsu National Synergetic Innovation Center for Advanced Materials (SICAM) , Nanjing Technology University , Nanjing , Jiangsu 211816 , China.
⁷ Department of Chemistry and Collaborative Innovation Center for Nanomaterial Science and Engineering , Tsinghua University , Beijing 100084 , China.

PMID: 31804817
DOI: 10.1021/jacs.9b09391

Abstract

The efficient electrochemical hydrogen evolution reaction (HER) plays a key role in accelerating sustainable H₂ 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/cm² 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.