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

Ni-based catalysts hold great potential in the light-driven dry reforming of methane (DRM) for syngas production due to their 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 attributed to the coking. Herein, an atomically dispersed Ni-loaded CeO2 (Ni/CeO2) for light-driven DRM is prepared by employing a polyol-mediated doping method to allow the high loading concentration of Ni on the CeO2, which overcomes 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 effects for driving the reaction, while the CeO2 can facilitate 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, and such excellent stability of the presence of enormous Ni-O pairs can prevent the rapid conversion of CHx intermediates into coke. This work demonstrates the meticulous design of non-noble metal catalysts for the lightdriven DRM with both high performance and stability.