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Metal oxides are archetypal CO 2  reduction reaction electrocatalysts, yet inevitable self-reduction will enhance competitive hydrogen evolution and lower the CO 2  electroreduction selectivity. Herein, we propose a tangible superlattice model of alternating metal oxides and selenide sublayers in which electrons are rapidly exported through the conductive metal selenide layer to protect the active oxide layer from self-reduction. Taking BiCuSeO superlattices as a proof-of-concept, a comprehensive characterization reveals that the active [Bi 2 O 2 ] 2+  sublayers retain oxidation states rather than their self-reduced Bi metal during CO 2  electroreduction because of the rapid electron transfer through the conductive [Cu 2 Se 2 ] 2-  sublayer. Theoretical calculations uncover the high activity over [Bi 2 O 2 ] 2+  sublayers due to the overlaps between the Bi  p  orbitals and O  p  orbitals in the OCHO* intermediate, thus achieving over 90% formate selectivity in a wide potential range from −0.4 to −1.1 V. This work broadens the studying and improving of the CO 2  electroreduction properties of metal oxide systems.

Active and conductive layer stacked superlattices for highly selective CO2 electroreduction