Polyvinylpyrrolidone-Coordinated Single-Site Platinum Catalyst Exhibits High Activity for Hydrogen Evolution Reaction

Can Li; Zheng Chen; Hong Yi; Yi Cao; Lei Du; Yidong Hu; Fanpeng Kong; Richard Kramer Campen; Yunzhi Gao; Chunyu Du; Geping Yin; Igor Ying Zhang; Yujin Tong

doi:10.1002/anie.202005282

Polyvinylpyrrolidone-Coordinated Single-Site Platinum Catalyst Exhibits High Activity for Hydrogen Evolution Reaction

Angew Chem Int Ed Engl. 2020 Sep 7;59(37):15902-15907. doi: 10.1002/anie.202005282. Epub 2020 Jun 29.

Authors

Can Li^{1

2}, Zheng Chen³, Hong Yi⁴, Yi Cao¹, Lei Du¹, Yidong Hu⁵, Fanpeng Kong¹, Richard Kramer Campen^{2

6}, Yunzhi Gao¹, Chunyu Du¹, Geping Yin¹, Igor Ying Zhang³, Yujin Tong^{2

6}

Affiliations

¹ MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, Harbin Institute of Technology, Harbin, 150001, China.
² Fritz Haber Institute of the Max Planck Society, Faradayweg 4-6, 14195, Berlin, Germany.
³ Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Collaborative Innovation Center of Chemistry for Energy Materials, MOE Laboratory for Computational Physical Science, Department of Chemistry, Fudan University, 200433, Shanghai, China.
⁴ College of Chemistry and Molecular Sciences, Wuhan University, Wuhan, 430072, China.
⁵ 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.
⁶ Faculty of Physics, University of Duisburg-Essen, Lotharstraße 1, 47057, Duisburg, Germany.

Abstract

The essence of developing a Pt-based single-atom catalyst (SAC) for hydrogen evolution reaction (HER) is the preparation of well-defined and stable single Pt sites with desired electrocatalytic efficacy. Herein, we report a facile approach to generate uniformly dispersed Pt sites with outstanding HER performance via a photochemical reduction method using polyvinylpyrrolidone (PVP) molecules as the key additive to significantly simplify the synthesis and enhance the catalytic performance. The as-prepared catalyst displays remarkable kinetic activities (20 times higher current density than the commercially available Pt/C) with excellent stability (76.3 % of its initial activity after 5000 cycles) for HER. EXAFS measurements and DFT calculations demonstrate a synergetic effect, where the PVP ligands and the support together modulate the electronic structure of the Pt atoms, which optimize the hydrogen adsorption energy, resulting in a considerably improved HER activity.

Keywords: electrocatalysis; electrochemistry; hydrogen evolution reaction; photochemistry; water splitting.

Abstract

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