Atomically Dispersed Co-Pyridinic N-C for Superior Oxygen Reduction Reaction
Atomically Dispersed Co-Pyridinic N-C for Superior Oxygen Reduction Reaction
复制标题
原子分散的 Co-吡啶 N-C，可实现出色的氧还原反应
DOI：
10.1002/aenm.202002592
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发表时间：
2020-10-23
影响因子：
27.8
通讯作者：
Wu, Renbing
中科院分区：
文献类型：
--
作者：
Ha, Yuan;Fei, Ben;Wu, Renbing
具有高密度可及活性位点和优化电子结构的工程化过渡金属-氮-碳（TM-N-C）催化剂在电化学氧还原反应（ORR）的背景下具有很大的前景。本文报道了溶菌酶改性的沸石咪唑酯骨架的新改性，其中孤立的Co原子锚定在主导的吡啶-N掺杂的碳（Co-吡啶N-C）上。原子分散的Co允许最大的活性中心暴露，而吡啶N的引入可以大大减少Co中心周围的电子局域化并改善与含氧物种的相互作用，从而降低中间体的能垒并促进有利的四电子ORR途径。由于单原子Co和配位吡啶N的协同效应，Co-吡啶N-C催化剂在碱性和酸性介质中均表现出优异的ORR活性和稳定性，是目前报道的活性最高的Co-N-C催化剂之一。本工作为合理设计TM-N-C催化剂以提高其在ORR中的催化性能开辟了一条途径。
Engineering transition metal-nitrogen-carbon (TM-N-C) catalysts with high-density accessible active sites and optimized electronic structure holds great promise in the context of the electrochemical oxygen reduction reaction (ORR). Herein, a novel modification of a lysozyme-modified zeolitic imidazolate framework with isolated Co atoms anchored on dominated pyridinic-N doped carbon (Co-pyridinic N-C) is reported. The atomically dispersed Co allows the maximum active site exposure while the introduction of pyridinic N can greatly reduce the electron localization around the Co centers and improve the interaction with oxygenated species, and thus lowering the energy barriers of the intermediates and facilitating the favorable four-electron ORR pathway. Owing to the synergistic effects of single-atom Co and coordinated pyridinic N, the Co-pyridinic N-C catalyst exhibits an exceptional ORR activity and remarkable stability in both alkaline and more challenging acidic media, representing one of the most active Co-N-C catalysts reported. This work may open an avenue for the rational design of TM-N-C catalysts to boost their catalytic performance for application in the ORR.