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The in situ exsolution technique of nanoparticles has brought new opportunities for the utilization of perovskite‐based catalysts in solid oxide cells. However, the lack of control over the structural evolution of host perovskites during the promotion of exsolution has restricted the architectural exploitation of exsolution‐facilitated perovskites. In this study, we strategically broke the long‐standing trade‐off phenomenon between promoted exsolution and suppressed phase transition via B‐site supplement, thus broadening the scope of exsolution‐facilitated perovskite materials. Using carbon dioxide electrolysis as an illustrative case study, we demonstrate that the catalytic activity and stability of perovskites with exsolved nanoparticles (P‐eNs) can be selectively enhanced by regulating the explicit phase of host perovskites, accentuating the critical role of the architectures of perovskite scaffold in catalytic reactions occurring on P‐eNs. The concept demonstrated could potentially pave the way for designing the advanced exsolution‐facilitated P‐eNs materials and unveiling a wide range of catalytic chemistry taking place on P‐eNs. [ABSTRACT FROM AUTHOR]

Perovskites are the promising catalysts for various reactions, yet their structure evolutions and the composition-function relation in the carbon dioxide reduction reaction (CO 2 RR) are not fully explored. In this study, we report that the reconstructed BaBiO 3 (BBO) perovskite is able to facilitate CO 2 -to-formate (FA) conversion by both A- (Ba) and B- (Bi) site elements through the cooperative but distinct catalytic mechanisms. Specifically, the electrochemical reductions of BBO trigger the complete rearrangement of atoms with rapid kinetics at catalytically relevant voltages, giving rise to electricity-induced Bi metallene (eBBO) that efficiently generates FA with high selectivity and partial current densities. Moreover, the reconstructed BBO simultaneously enables Ba2+ release to the electrolyte, and the time-resolved FTIR and in situ Raman analysis collectively reveal that the Ba2+ adsorption enables easier CO 2 adsorption, thereby leading to enhanced CO 2 -to-FA conversion. This work is of direct significance in elucidating the cooperative catalysis between A- and B- site elements in perovskites for room-temperature CO 2 RR. [Display omitted] • Potential-induced reconstructions of BaBiO 3 lead to the in situ generation of bismuthene. • BaBiO 3 derived bismuthene exhibits high activity towards CO 2 -to-Foramte (FA) conversion. • A photoelectrochemical cell was constructed to initiate FA production at a low cell voltage of 2.5 V with high selectivity. • The simultaneous release of A-site element (Ba2+) into the electrolyte promotes the CO 2 adsorption. [ABSTRACT FROM AUTHOR]