Durable and efficient concentrated-solar catalytic methane dry reforming over Ni-based catalysts

Title : Durable and efficient concentrated-solar catalytic methane dry reforming over Ni-based catalysts

Abstract:

Dry reforming of methane (DRM) is a promising technology for converting greenhouse gases (CH₄ and CO₂) into syngas, but it is typically hindered by high energy barriers and rapid catalyst deactivation due to severe coking. This work presents a comprehensive study on designing advanced Ni-based catalysts to overcome these challenges through active site engineering and photothermal catalysis. First, we reveal the non-thermal effects of light on Ni/Ga₂O₃, where light irradiation reverses the electron transfer direction and generates hot electrons, effectively tuning the H₂/CO ratio near unity by suppressing the reverse water-gas shift reaction. Second, moving to single-atom catalysis on NiSA/CeO₂, we demonstrate that light irradiation reinforces the formation of the key anti-coking intermediate (CH₃O*), achieving exceptional stability for over 230 hours at a low temperature of 472 °C. Third, we explore heteroatom doping strategies to stabilize active sites. Praseodymium-modified CeO₂ (Ni/Pr-CeO₂) is found to facilitate direct carbonate cleavage under light, significantly boosting CO yield, while Molybdenum-stabilized Nickel-oxo sites (NiMo/MgO) enable a "hydroxyl-mediated" pathway involving CH₂OH intermediates, further lowering the activation temperature to 465 °C. Finally, we scale up these concepts to a concentrated solar catalytic system using Ni-O₄ coordinated sites on CeO₂(100), achieving ultrahigh conversion (>93%) and light-to-chemical energy conversion efficiency (25.9%) with over 800 hours of durability. These findings collectively provide critical mechanistic insights into C-H/C-O bond activation and offer a multidimensional roadmap for developing sustainable, solar-driven C1 chemistry technologies. The integrated strategy connects catalyst-site design with reactor-level solar heat management, highlighting how oxygen mobility, interfacial coordination, and light-assisted reaction pathways can be combined to suppress carbon deposition while maintaining high syngas productivity.

Keywords: Methane dry reforming; Photothermal catalysis; Nickel catalysts; Single-atom engineering; Concentrated solar energy

Biography:

Zeai Huang is a Researcher at Southwest Petroleum University. His research focuses on solar-driven conversion of CO₂ and natural gas, photothermal catalysis, methane dry reforming, anti-coking catalyst design, operando characterization, and solar-driven natural gas conversion systems.