Mechanistic ab-initio DFT Study of CO₂ Hydrogenation to olefines on MgH₂(001)
Palavras-chave:
CO2, hydrogenation, olefins, metal hydrides, computational catalysis.Resumo
We present a comprehensive theoretical investigation of CO2 hydrogenation on the MgH2(001) surface, focusing on the unique role of lattice hydrogen as the primary H source. Our findings reveal a distinct reaction pathway involving spontaneous formate (HCOO*) formation upon CO2 adsorption, followed by subsequent hydrogenation to dioxomethylene (H2COO*) and hydroxymethoxy (H2COOH*) intermediates. Under H2-lean conditions, partially hydrogenated C1 intermediates can undergo coupling to form C2 products with selectivity toward olefins. This work provides fundamental insights into hydride-mediated catalysis and establishes a mechanistic framework for rational design of metal hydride catalysts capable of selective CO2 conversion under H2-limited conditions
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