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Catalytic CO 2  conversion to energy carriers and intermediates is of utmost importance to energy and environmental goals. However, the lack of fundamental understanding of the reaction mechanism renders designing a selective catalyst inefficient. Here we show the correlation between the kinetics of product formation and those of surface species conversion during CO 2  reduction over Pd/Al 2 O 3  catalysts. The  operando  transmission FTIR/SSITKA (Fourier transform infrared spectroscopy/steady-state isotopic transient kinetic analysis) experiments demonstrates that the rate-determining step for CO formation is the conversion of adsorbed formate, whereas that for CH 4  formation is the hydrogenation of adsorbed carbonyl. The balance of the hydrogenation kinetics between adsorbed formates and carbonyls governs the selectivities to CH 4  and CO. We apply this knowledge to the catalyst design and achieve high selectivities to desired products.

Controlling selectivities in CO2 reduction through mechanistic understanding