Abstract
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.