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 g_cat⁻¹ h⁻¹) and CO (728.5 mmol g_cat⁻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 CH_x intermediates into coke. This work demonstrates the meticulous design of non-noble metal catalysts for the light-driven DRM with both high performance and stability.