CO2 hydrogenation to methanol over Cu catalysts supported on La-modified SBA-15: The crucial role of Cu–LaOx interfaces
The direct hydrogenation of CO 2 to methanol has become a very active research field because CO 2 can be prospectively recycled to mitigate greenhouse effect and store clean synthetic fuels. This reaction can be catalyzed by supported Cu catalysts and the catalysts display strong support or promoter effects. Sintering of Cu species accelerates the separation of Cu–oxide interfaces, reduces the active component, and diminishes the methanol selectivity. In this work, we report a Cu catalyst supported on La-modified SBA-15, where the Cu–LaO x interface is generated through the interaction of highly dispersed Cu nanoparticles with LaO x species bedded into the SBA-15 pore wall. The optimized Cu 1 La 0.2 /SBA-15 catalyst can achieve methanol selectivity up to 81.2% with no deterioration in activity over 100 h on stream compared with the La-free catalyst. A thorough study reveals that La species not only significantly improve the CO 2 adsorption but also enhance Cu dispersion to produce well-dispersed active sites. The H/D exchange experiments show that the methanol synthesis displays a strong thermodynamic isotope effect and the Cu–LaO x interface plays a crucial role for the methanol synthesis rate in CO 2 /D 2 feed. In situ DRIFTS studies reveal that *HCOO and *OCH 3 species are the key intermediates formed during the activation of CO 2 and methanol synthesis over the Cu 1 La 0.2 /SBA-15 catalyst.
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