A First-Principles-Based Microkinetic Study of CO2 Reduction to CH3OH over In2O3(110)

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High Resolution Image Download MS PowerPoint Slide Methanol synthesis from catalytic recycling of CO 2 is one viable route to produce fuel and a stock chemical from a greenhouse gas. Herein, hydrogenation of CO 2 to CH 3 OH is investigated with density functional theory calculations combined with mean-field microkinetic modeling. The model explores the direct route for CO 2 hydrogenation (HCOOH route) and the competing reverse water-gas shift (RWGS) reaction. The predicted temperature dependence of turnover frequencies, selectivities, and reaction orders are in good agreement with previous experimental results. The formation of methanol at relevant reaction temperatures (470–670 K) is found to be kinetically controlled by H 2 COOH dissociation to H 2 CO + OH, whereas the RWGS reaction is solely controlled by CO 2 hydrogenation to COOH. An analysis of the kinetic behavior reveals that the stabilization of hydrogen adsorption should be one way to improve the catalyst performance.