Zheng, Yihan; Wang, Yuxin; Li, Ruitao; Yang, Haoran; Dai, Yuanyuan; Niu, Qiang; Lin, Tiejun; Gong, Kun; Zhong, Liangshu

CHINESE JOURNAL OF CATALYSIS

2025, ,

Zheng, Yihan; Wang, Yuxin; Li, Ruitao; Yang, Haoran; Dai, Yuanyuan; Niu, Qiang; Lin, Tiejun; Gong, Kun; Zhong, Liangshu

CO2-free H2 refers to H2 production process without CO2 emission, which is a promising clean energy in the future. Catalytic decomposition of methane (CDM) is a competitive technology to produce CO2-free H2 with large-scale. However, CDM reaction is highly endothermic and is kinetically and thermodynamically unfavorable, which typically requires a harsh reaction temperature above 800 degrees C. In this work, solar-driven photothermal catalytic decomposition of methane was firstly introduced to produce CO2-free H2 relying solely on solar energy as the driving force. A high H2 yield of 204.6 mmol g-1 h-1 was observed over Ni-CeO2 interface under photothermal conditions, along with above 87% reduction in the apparent activation energy (11.2 vs. 87.3 kJ mol-1) when comparing with the traditional thermal catalysis. Further studies suggested that Ni/CeO2 catalyst enhanced optical absorption in visible-infrared region to ensure the heat energy for methane decomposition. The generated electrons and holes participated in the redox process of photo-driven CDM reaction with enhanced separation ability of hot carriers excited by ultraviolet-visible light, which lowered activation energy and improved the photothermal catalytic activity. This work provides a promising photothermal catalytic strategy to produce CO2-free H2 under mild conditions. (c) 2025, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.