Zhang Bo-Wen, Zhu Meng-Nan, Gao Min-Rui, Xi Xiuan, Duan Nanqi, Chen Zhou, Feng Ren-Fei, Zeng Hongbo, Luo Jing-Li
Department of Chemical and Materials Engineering, University of Alberta, Edmonton, AB, T6G 1H9, Canada.
College of Materials Science and Engineering, Shenzhen University, Shenzhen, 518060, P.R. China.
Nat Commun. 2022 Aug 8;13(1):4618. doi: 10.1038/s41467-022-32393-y.
Perovskites with exsolved nanoparticles (P-eNs) have immense potentials for carbon dioxide (CO) reduction in solid oxide electrolysis cell. Despite the recent achievements in promoting the B-site cation exsolution for enhanced catalytic activities, the unsatisfactory stability of P-eNs at high voltages greatly impedes their practical applications and this issue has not been elucidated. In this study, we reveal that the formation of B-site vacancies in perovskite scaffold is the major contributor to the degradation of P-eNs; we then address this issue by fine-regulating the B-site supplement of the reduced SrFeNiMoO using foreign Fe sources, achieving a robust perovskite scaffold and prolonged stability performance. Furthermore, the degradation mechanism from the perspective of structure stability of perovskite has also been proposed to understand the origins of performance deterioration. The B-site supplement endows P-eNs with the capability to become appealing electrocatalysts for CO reduction and more broadly, for other energy storage and conversion systems.
具有析出纳米颗粒的钙钛矿(P-eNs)在固体氧化物电解池中具有巨大的二氧化碳(CO)还原潜力。尽管最近在促进B位阳离子析出以提高催化活性方面取得了进展,但P-eNs在高电压下的稳定性不尽人意,这极大地阻碍了它们的实际应用,而这个问题尚未得到阐明。在本研究中,我们揭示了钙钛矿支架中B位空位的形成是P-eNs降解的主要原因;然后,我们通过使用外来铁源精细调节还原后的SrFeNiMoO的B位补充来解决这个问题,从而实现了坚固的钙钛矿支架和延长的稳定性性能。此外,还从钙钛矿结构稳定性的角度提出了降解机制,以了解性能恶化的根源。B位补充使P-eNs有能力成为用于CO还原以及更广泛地用于其他能量存储和转换系统的有吸引力电催化剂。