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Highly dispersed Ni–O site on Ni catalysts for efficient and durable light-driven dry reforming of CH4 at ambient conditions

Xia Gao, Shuaikang Sang, Enquan Zhu, Lihua Cai, Chang Liu, Ferdi Karadas, Chao Zhang*, Jingxiang Low*, Yujie Xiong*

https://doi.org/10.1016/j.cjsc.2025.100570

ABSTRACT

Ni-based catalysts hold great potential in the light-driven dry reforming of methane (DRM) for syngas production due to its low cost and comparable catalytic performance to conventional noble-metal catalysts. However, the currently available Ni-based catalysts are confronted with low light-driven DRM efficiency and poor stability, which are attributed to the coking. Herein, we prepared an atomically dispersed Ni-loaded CeO2 (Ni/CeO2) for light-driven DRM. We employ a polyol-mediated doping method to allow the high loading concentration of the Ni on the CeO2, overcoming the conventional atomically dispersed metal problem of low loading content. The atomically dispersed nature of the Ni can induce enormous CH4 activation sites for the reaction and photothermal effect for driving the reaction, while the CeO2 can facilitate the CO2 activation. Therefore, the optimized atomically dispersed Ni-loaded CeO2 demonstrates an excellent light-driven DRM performance for H2 (626.5 mmol gcat-1 h-1) and CO (728.5 mmol gcat-1 h-1) production. More importantly, the optimized sample sustains its DRM performance after 100 h of continuous test. Such an excellent light-driven DRM stability of the presence of the enormous Ni–O pairs can prevent the rapid conversion of CHx intermediates into coke. This work demonstrates the meticulous design of the non-noble metal catalysts for the light-driven DRM with both high performance and stability.

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