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Efficient and selective CO 2  electroreduction into chemical fuels promises to alleviate environmental pollution and energy crisis, but it relies on catalysts with controllable product selectivity and reaction path. Here, by means of first-principles calculations, we identify six ferroelectric catalysts comprising transition-metal atoms anchored on In 2 Se 3  monolayer, whose catalytic performance can be controlled by ferroelectric switching based on adjusted  d -band center and occupation of supported metal atoms. The polarization dependent activation allows effective control of the limiting potential of CO 2  reduction on TM@In 2 Se 3  (TM = Ni, Pd, Rh, Nb, and Re) as well as the reaction paths and final products on Nb@In 2 Se 3  and Re@In 2 Se 3 . Interestingly, the ferroelectric switching can even reactivate the stuck catalytic CO 2  reduction on Zr@In 2 Se 3 . The fairly low limiting potential and the unique ferroelectric controllable CO 2  catalytic performance on atomically dispersed transition-metals on In 2 Se 3  clearly distinguish them from traditional single atom catalysts, and open an avenue toward improving catalytic activity and selectivity for efficient and controllable electrochemical CO 2  reduction reaction.

Controllable CO2 electrocatalytic reduction via ferroelectric switching on single atom anchored In2Se3 monolayer