Chinese Journal of Catalysis

Chinese Journal of Catalysis ›› 2026, Vol. 91: 365-375.DOI: 10.1016/S1872-2067(26)65207-2

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Coordination reconfigured Ni single-atoms for scaled photothermal COx free hydrogen production from ammonia

Yachuan Wanga,1, Runan Leia,1, Wei Wanga,1, Qixuan Wua,1, Kaiwen Kangb,c,1, Dachao Yuand, Zhibo Zhangc, Yuan Tanga,*(), Linjie Gaoa,*(), Yaguang Lia,*(), Jinhua Yea,e,f,*()   

  1. a Research Center for Solar Driven Carbon Neutrality, Engineering Research Center of Zero-carbon Energy Buildings and Measurement Techniques, Ministry of Education, The College of Physics Science and Technology, Institute of Life Science and Green Development, Hebei University, Baoding 071002, Hebei, China
    b State Key Laboratory of Metastable Materials Science and Technology, Yanshan University, Qinhuangdao 066004, Hebei, China
    c School of Materials Science and Engineering, Southwest Jiaotong University, Chengdu 611756, Sichuan, China
    d College of Mechanical and Electrical Engineering, Key Laboratory Intelligent Equipment and New Energy Utilization of Livestock and Poultry Breeding, Hebei Agricultural University, Baoding 071001, Hebei, China
    e Advanced Catalytic Materials Research Center, School of Materials Science and Engineering, Tianjin University, Tianjin 300072, China
    f International Center for Materials Nanoarchitectonics (WPI-MANA), National Institute for Materials Science (NIMS), 1-1 Namiki, Tsukuba, Ibaraki 305-0044, Japan
  • Received:2026-01-15 Accepted:2026-03-19 Online:2026-12-18 Published:2026-10-13
  • About author:1Contributed equally to this work.
  • Supported by:
    National Natural Science Foundation of China(52371220);National Natural Science Foundation of China(U23A20139);Natural Science Foundation of Hebei Province(B2023204034);Natural Science Foundation of Hebei Province(B20232011107);Natural Science Foundation of Hebei Province(2023HBQZYCXY001)

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Abstract:

Ammonia (NH3) decomposition to produce COx free hydrogen is an ideal supply for hydrogen refueling stations with the drawback of giant secondary energy consumption, which limits its application. Herein, we develop a natural sunlight driven photothermal NH3 decomposition system to achieve a hydrogen evolution rate of 298.0 mmol g-cat–1 h–1 with the solar-to-hydrogen efficiency of 16.1%, outperforming all counterparts. The catalytic activity is attributed to the catalyst of Ni single atoms loaded on a cerium-zirconium solid solution (SA Ni/CexZr1–xO2), that the component regulation of CexZr1–xO2 could modulate the Ni–O coordination number and shorten the Ni–O bond length of Ni single atoms to synergistically optimize the dissociative energy barrier of NH3 molecules and the desorption kinetics of NHx intermediates. Under outdoor sunlight illumination, the enlarged photothermal NH3 decomposition system achieves a record hydrogen production rate of 1 kg per day and the corresponding cost is calculated as $3.53 kg–1, significantly lower than the market price of hydrogen from thermocatalytic NH3 decomposition ($4.26 kg–1). This work provides a new strategy for NH3 decomposition in COx free hydrogen energy system with low energy consumption and cost advantage through the synergistic of coordination structure modulation of catalyst and photothermal system.

Key words: Photothermal catalysis, Ammonia, Hydrogen, Solid solution