CO2 hydrogenation on metal oxide catalysts is thought to successively produce formic acid, formaldehyde, and methanol in subsequent proton-coupled electron transfer steps, yet the thermodynamics and kinetics of these catalytic processes on solid-state oxygen carriers remain to be quantified.  A new method for computing enthalpies of reaction and corresponding rate coefficients was proposed, based on computed energies of activation and vibrational frequencies obtained from density functional theory calculations.  This approach was applied to study CO2 hydrogenation on ceria (110) catalysts, and used to accurately predict enthalpies of reaction at finite reaction temperatures.  These enthalpies may then be used to compute energies of activation at finite reaction temperatures, and subsequently, rate coefficients using transition state theory.

Rational design of oxide catalysts for carbon dioxide activation and hydrogenation

248th National Meeting (2014)

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