La-Modified NiMgAl LDH-Derived Catalysts for Enhanced Low-Temperature CO2 Methanation
摘要
The conversion of CO2 to CH4 under mild conditions is regarded as a crucial pathway for carbon recycling and renewable energy storage, but challenging to achieve. In this work, the low-temperature CO2 methanation performance on the NiMgAl layered double hydroxide-derived catalyst was effectively enhanced by La addition. The catalyst with appropriate La loading (NiMgAl-La0.5) exhibited 93.1% CO2 conversion at 250 °C, which is significantly higher than that on NiMgAl (37.5%). This activity remains stable during a 100-h long-term reaction. Various ex situ and in situ characterizations revealed that La doping promotes Ni nanoparticle dispersion, increases weak basic sites, and introduces abundant oxygen vacancies, thereby enhancing the adsorption and activation of CO2. In situ DRIFTS studies and density functional theory calculations identified a formate-mediated pathway, where La doping accelerates the conversion of carbonate to formate and facilitates C-O bond cleavage. This work potentially guides the design of efficient Ni-based catalysts for CO2 hydrogenation under mild conditions.
Graphical Abstract