Citation: Ruizhi Duan, Xiaomei Wang, Panwang Zhou, Yang Liu, Can Li. The role of hydroxyl species in the alkaline hydrogen evolution reaction over transition metal surfaces[J]. Acta Physico-Chimica Sinica, ;2025, 41(9): 100111. doi: 10.1016/j.actphy.2025.100111 shu

The role of hydroxyl species in the alkaline hydrogen evolution reaction over transition metal surfaces

Ruizhi Duan ^{1, 2} ,
Xiaomei Wang ^{1, 3} ,
Panwang Zhou ² ,
Yang Liu ² ,
Can Li ^{1, 2,,}

1.
Key Laboratory of Advanced Catalysis, Gansu Province, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000, Gansu Province, China
2.
State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian National Laboratory for Clean Energy, Dalian 116023, Liaoning Province, China
3.
School of Materials Science and Engineering, Lanzhou Jiaotong University, Lanzhou 730000, Gansu Province, China

Corresponding author: Can Li, canli@dicp.ac.cn
Received Date: 26 March 2025
Revised Date: 16 May 2025
Accepted Date: 2 June 2025

Fund Project: the Fundamental Research Centre of Artificial Photosynthesis FReCAPthe National Key Research and Development Program of China 2021YFB4000300the National Natural Science Foundation of China 22102065the National Natural Science Foundation of China 22088102the National Natural Science Foundation of China 22372162the Natural Science Foundation of Gansu Province for Youth project, China 24JRRA281

Understanding the activity-determining factors governing the alkaline hydrogen evolution reaction (HER) on transition metal catalysts is indispensable for water electrolysis with renewable energy. However, it remains a critical challenge. Although hydroxyl adsorption has been proposed to influence alkaline HER performance, its exact mechanistic role and quantitative correlations remain elusive. Here, we systematically investigate the alkaline HER on ten transition metal surfaces using density functional theory (DFT), revealing that hydroxyl adsorption critically modulates both pathway selection and reaction energy barrier. However, hydroxyl adsorption energy alone cannot fully explain the anomalous activity of certain catalysts, especially Pt. To address this, we introduce a multi-parameter coupled descriptor (ECS) that integrates electron occupancy (E), adsorption configuration (C), and surface crystallographic (S), enabling a qualitative evaluation of catalytic activity. This descriptor successfully elucidates previously unexplained activity trends and demonstrates a good correlation with over 10 experimental datasets, including those involving single-atom alloy (SAA) catalysts, indicating its robustness beyond pure metals. Our findings provide a descriptor based on the key species of hydroxyl for rational catalyst design and screening, and offer a fundamental framework for advancing the development of high-performance alkaline HER catalysts.
- Alkaline water splitting,
- Hydroxyl species,
- Electrocatalysis,
- Transition metal catalysts,
- Structure-activity relationship
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