CO2 activation using transition metal(TM) catalysts was investigated. Homogeneous catalysis of the reverse water gas shift reaction was studied.  �-diketiminatometal models L'MI ( L' =C3N2H5-; M = first-row TMs) were considered as potential catalysts. The thermodynamics of reaction pathways were simulated using B3LYP/aug-cc-pVTZ, showing that middle series metal complexes result in more thermodynamically favorable properties; therefore, more detailed thermodynamic and kinetic studies were carried out for Mn, Fe, and Co complexes. Heterogeneous catalysis of CO2 reduction to CO was carried out on Fe, Co, Ni, and Cu surfaces, using the GGA_PBE functional. Reaction barriers were calculated using the climbing image nudged elastic band method. Co and Ni showed more favorable thermodynamics and lower barriers, while Fe tends to overbind CO2.  An important thermodynamic trend was discovered for both homo- and heterogeneous catalysis, as a function of metal: earlier metals tend to have stronger interaction with CO2 than the later metals.

Computational studies on CO<sub>2</sub> activation using transition metal catalysts: In consideration of homogeneous and heterogeneous catalysis

243rd National Meeting (2012)

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Computational studies on CO2 activation using transition metal catalysts: In consideration of homogeneous and heterogeneous catalysis

Computational studies on CO₂ activation using transition metal catalysts: In consideration of homogeneous and heterogeneous catalysis