Chem Catalysis ( IF 11.5 ) Pub Date : 2023-02-26 , DOI: 10.1016/j.checat.2023.100532 Yuyi Chu , Ergui Luo , Yao Wei , Siyuan Zhu , Xian Wang , Liting Yang , Nanxing Gao , Ying Wang , Zheng Jiang , Changpeng Liu , Junjie Ge , Wei Xing
Metal-nitrogen-carbon materials are the most promising platinum replacement catalysts for oxygen reduction reaction. However, lacking an efficient approach to improve durability—i.e., to cope with the attack by in situ formed radicals, leaching of central ions, etc.—has limited these catalysts from widespread application. Herein we present a novel, dual-metal, single-atom catalyst design (Fe,Ce-N-C) to confront the formidable deactivation issue of the best-performing yet unstable Fe-N-C catalysts. Cerium single sites are revealed as efficient chemical catalysts to catalyze the H2O2 disproportionation into O2, leading to increased 4e selectivity. Moreover, rather than Fe single sites that catalyze the formation of reactive ·OH and ·OOH species, these cerium single sites act proactively to eliminate in situ-generated radicals. The final Fe,Ce-N-C catalyst represents excellent durability exceeding that of Fe-N-C. This work opens a new path to alleviate the degradation of Fe-N-C catalysts in an acidic medium.
中文翻译:
双单原子催化剂设计通过自由基清除构建坚固的氧还原电极
金属-氮-碳材料是最有前途的氧还原反应铂替代催化剂。然而,缺乏有效的方法来提高耐久性——即应对原位形成的自由基的攻击、中心离子的浸出等——限制了这些催化剂的广泛应用。在这里,我们提出了一种新颖的双金属单原子催化剂设计(Fe,Ce-NC),以应对性能最佳但不稳定的 Fe-NC 催化剂的巨大失活问题。铈单中心被揭示为有效的化学催化剂来催化 H 2 O 2歧化成 O 2,导致 4e 选择性增加。此外,与催化反应性·OH 和·OOH 物质形成的 Fe 单点不同,这些铈单点主动消除原位生成的自由基。最终的 Fe,Ce-NC 催化剂表现出超过 Fe-NC 的出色耐久性。这项工作为减轻 Fe-NC 催化剂在酸性介质中的降解开辟了一条新途径。