Abstract:In this work, the reaction mechanism for the conversion of CO2 and H2 to methanol has been researched by density functional theory (DFT). The production of methanol from CO2 and H2 is catalyzed by a univocal bifunctional pincer-type complex trans-RuH2(CO)(dpa) (dpa = bis-(2-diphenylphosphinoethyl)amine). The reaction mechanism includes three continuous catalytic processes: (1) CO2 is converted to formic acid; (2) formic acid is converted to formaldehyde and water; (3) formaldehyde is converted to methanol. By computing the catalytic processes, we have shown that the rate-limiting step in the whole process is the direct cleavage of H2. The calculated largest free energy barrier is 21.6 kcal/mol. However, with the help of water, the free energy barrier can be lowered to 12.7 kcal/mol, which suggests viability of trans-RuH2(CO)(dpa) as a catalyst for the direct conversion of CO2 and H2 to methanol.Keywords: CO2 hydrogenation; formic acid; formaldehyde; methanol; trans-RuH2(CO)(dpa); density functional theory
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