Pinpointing the axial ligand effect on platinum single-atom-catalyst towards efficient alkaline hydrogen evolution reaction

Tianyu Zhang, Jing Jin, Junmei Chen, Yingyan Fang, Xu Han, Jiayi Chen, Yaping Li, Yu Wang, Junfeng Liu () and Lei Wang ()
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Tianyu Zhang: Beijing University of Chemical Technology
Jing Jin: Beijing University of Chemical Technology
Junmei Chen: National University of Singapore
Yingyan Fang: Beijing University of Chemical Technology
Xu Han: Beijing University of Chemical Technology
Jiayi Chen: National University of Singapore
Yaping Li: Beijing University of Chemical Technology
Yu Wang: Chinese Academy of Sciences
Junfeng Liu: Beijing University of Chemical Technology
Lei Wang: National University of Singapore

Nature Communications, 2022, vol. 13, issue 1, 1-14

Abstract: Abstract Developing active single-atom-catalyst (SAC) for alkaline hydrogen evolution reaction (HER) is a promising solution to lower the green hydrogen cost. However, the correlations are not clear between the chemical environments around the active-sites and their desired catalytic activity. Here we study a group of SACs prepared by anchoring platinum atoms on NiFe-layered-double-hydroxide. While maintaining the homogeneity of the Pt-SACs, various axial ligands (−F, −Cl, −Br, −I, −OH) are employed via a facile irradiation-impregnation procedure, enabling us to discover definite chemical-environments/performance correlations. Owing to its high first-electron-affinity, chloride chelated Pt-SAC exhibits optimized bindings with hydrogen and hydroxide, which favor the sluggish water dissociation and further promote the alkaline HER. Specifically, it shows high mass-activity of 30.6 A mgPt−1 and turnover frequency of 30.3 H2 s−1 at 100 mV overpotential, which are significantly higher than those of the state-of-the-art Pt-SACs and commercial Pt/C catalyst. Moreover, high energy efficiency of 80% is obtained for the alkaline water electrolyser assembled using the above catalyst under practical-relevant conditions.

Date: 2022
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DOI: 10.1038/s41467-022-34619-5

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