Converting CO2 to liquid fuels, such as formate and methanol, using inexpensive metal catalysts would reduce atmospheric greenhouse gas levels and provide an economical source of renewable energy. In this vein, we have characterized a series of bimetallic catalysts featuring strong Ni→M(III) (M=Al, Ga, In) dative bonds that catalyze CO2 hydrogenation to formate. Detailed thermodynamic studies will be presented that show quantitatively how the supporting metal ion influences each of the three fundamental steps in the catalytic mechanism: (1) H2 binding, (2) H2 heterolysis to form a reactive anionic Ni-H species, and (3) hydride transfer from Ni-H to CO2 to generate formate.

Imparting nobility to first-row metal-hydrides: Unusual anionic Ni-H stabilized by Lewis acidic metal supports and their role in catalytic carbon dioxide hydrogenation

253rd National Meeting (2017)

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