Universal Catalyst Design Framework for Electrochemical Hydrogen Peroxide Synthesis Facilitated by Local Atomic Environment Descriptors.

Journal: Angewandte Chemie (International ed. in English)
Published Date: Dec 8, 2025

Abstract

A universal design framework for high-performance catalysts remains challenging due to diverse structures and active sites. We developed a framework integrating weighted atom-centered symmetry function (wACSF) descriptors with machine learning, microkinetic modeling, and high-throughput screening. The wACSF descriptors unify geometric and chemical characteristics of active sites across different catalyst families. ML models trained on wACSF accurately predicted adsorption free energies of hydroxyl (ΔGOH *, R2 = 0.84) and oxygen (ΔGO*, R2 = 0.91) for intermetallic alloys, metal oxides, perovskites, and single-atom catalysts in the two-electron water oxidation reaction (2e- WOR). Density functional theory and microkinetic modeling yielded a universal 2e- WOR volcano model that agreed well with experiments. High-throughput screening with ML-predicted ΔGOH* identified LiScO2, which achieved 90% H2O2 Faradaic efficiency at 2.2 V vs. reversible hydrogen electrode (RHE) with 168-hour stability (82%-86% retention). Experimental activity (log(j) = 1.56) matched theoretical predictions (log(j) = 1.28) within 5% deviation at 2.4 V_RHE. This universal framework provides a general paradigm for rational catalyst design and is implemented in the Digital Catalysis Platform (DigCat), enabling efficient discovery across diverse material classes and electrochemical reactions.

Authors

  • Zhijian Liu
    Department of Power Engineering, School of Energy, Power and Mechanical Engineering, North China Electric Power University, Baoding, Hebei, 071003, PR China.
  • Yan Liu
    Department of Clinical Microbiology, Shanghai Tenth People's Hospital, School of Medicine, Tongji University, Shanghai, 200072, People's Republic of China.
  • Yuqi Zhang
    State Key Laboratory of Proteomics, Beijing Proteome Research Center, National Center for Protein Sciences-Beijing (PHOENIX Center), Beijing Institute of Lifeomics, Beijing, China.
  • Yeyu Deng
    School of Chemical and Biomolecule Engineering, The University of Sydney, Sydney, New South Wales, 2006, Australia.
  • Zhong Zheng
    National Research Center of Intelligent Equipment for Agriculture, Beijing 100097, China.
  • Ruth Knibbe
    School of Mechanical and Mining Engineering, The University of Queensland, Brisbane, 4072, Australia.
  • Tianxiang Gao
    Department of Computer Science, University of North Carolina, Chapel Hill, NC, USA.
  • Mingzhe Li
    Independent researcher, [email protected], Leeds, LS29JT, UK.
  • Ziye Wang
    School of Energy and Power Engineering, North China Electric Power University, Baoding, 071003, P.R. China.
  • Bingqian Zhang
    School of Energy and Power Engineering, North China Electric Power University, Baoding, 071003, P.R. China.
  • Xue Jia
    Advanced Institute for Materials Research (WPI-AIMR), Tohoku University, Sendai 980-8577, Japan. Electronic address: [email protected].
  • Di Zhang
    College of Food Science, Fujian Agriculture and Forestry University, Fuzhou 350002, China.
  • Heng Liu
    Yunnan Provincial Key Laboratory of Entomological Biopharmaceutical R&D, College of Pharmacy, Dali University, Dali, Yunnan, PR China; National-Local Joint Engineering Research Center of Entomoceutics, Dali, PR China.
  • Xuqiang Shao
    School of Control and Computer Engineering, North China Electric Power University, Baoding 071003, Hebei, China.
  • Zhengyang Gao
    Department of Power Engineering, School of Energy, Power and Mechanical Engineering, North China Electric Power University, Baoding, 071003, China.
  • Li Wei
    The First Affiliate Hospital of Guangzhou Medical University, Guangzhou, China.
  • Hao Li
    Department of Urology, Tongji Hospital, Tongji Medical College, Huazhong University of Science and Technology, Wuhan, China.
  • Weijie Yang
    Department of Power Engineering, School of Energy, Power and Mechanical Engineering, North China Electric Power University, Baoding, 071003, China.

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