Architecture Design and Catalytic Activity: Non‐Noble Bimetallic CoFe/fe(3)O(4) Core–Shell Structures for CO(2) Hydrogenation

Non‐noble metal catalysts now play a key role in promoting efficiently and economically catalytic reduction of CO(2) into clean energy, which is an important strategy to ameliorate global warming and resource shortage issues. Here, a non‐noble bimetallic catalyst of CoFe/Fe(3)O(4) nanoparticles is successfully designed with a core–shell structure that is well dispersed on the defect‐rich carbon substrate for the hydrogenation of CO(2) under mild conditions. The catalysts exhibit a high CO(2) conversion activity with the rate of 30% and CO selectivity of 99%, and extremely robust stability without performance decay over 90 h in the reverse water gas shift reaction process. Notably, it is found that the reversible exsolution/dissolution of cobalt in the Fe(3)O(4) shell will lead to a dynamic and reversible deactivation/regeneration of the catalysts, accompanying by shell thickness breathing during the repeated cycles, via atomic structure study of the catalysts at different reaction stages. Combined with density functional theory calculations, the catalytic activity reversible regeneration mechanism is proposed. This work reveals the structure–property relationship for rational structure design of the advanced non‐noble metallic catalyst materials with much improved performance.