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Decrypting the Influence of Axial Coordination on the Electronic Microenvironment of Co-N_(5)Site for Enhanced Electrocatalytic Reaction

引用

CCS Chemistry 2023年第8期5卷 1876-1887页

作者： Bingyu Huang Senhe Huang Chenbao Lu Longbin Li Judan Chen Ting Hu Dirk Lützenkirchen-Hecht Kai Yuan Xiaodong Zhuang Yiwang Chen Institute of Polymers and Energy Chemistry(IPEC) College of Chemistry and Chemical EngineeringNanchang UniversityNanchang 330031 The meso-Entropy Matter Lab School of Chemistry and Chemical EngineeringShanghai Jiao Tong UniversityShanghai 200240 School of Materials Science and Engineering Nanchang UniversityNanchang 330031 Faculty of Mathematics and Natural Sciences-Physics Department Bergische Universität WuppertalWuppertal D-42119 Institute of Advanced Scientific Research(iASR) Key Lab of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of EducationJiangxi Normal UniversityNanchang 330022

Metal porphyrins are star molecules that possess welldefined coordination metal centers for versatile catalytic ***,most previous work has focused on the correlations between in-plane symmetric configuration of metal-N_(4)sites and their catalytic *** the catalytic contribution of additional axial coordination to such symmetric configuration remains a *** calculations revealed that axially anchoring an extra pyridine on the tetra-coordinated cobalt porphyrin(Co-N4)to construct penta-coordinated cobalt porphyrin(Co-N_(5))renders cobalt a higher electron density,thereby favoring the rate-determining O_(2)adsorption/activation and reducing the oxygen electroreduction ***,a well-defined Co-N_(5)site is rationally introduced into the azo-linked polymer framework for a fundamental structure-catalytic performance correlation ***-prepared Co-N_(5)catalyst exhibits a 26 mV positive shift in half-wave potential compared with the pyridine-free Co-N_(4)counterpart,discloses a markedly higher power density(141.4 mW cm^(−2)),and possesses better long-term durability(over 160 h cycles)in a Zn-air ***,such a Co-N_(5)catalyst also showcases potential applications for CO_(2)reduction with high CO_(2)-to-CO conversion faradic efficiency and better selectivity than the Co-N_(4)counterpart because coordination of the fifth pyridine evokes electronic localization that suppresses a competitive side *** work proves the positive electrocatalytic contribution of axial penta-coordination on well-defined metalporphyrin-based catalysts and offers atomic understanding of the structure-performance correlation on single atom catalysts for future catalyst design.

关键词： porphyrin axial coordination pentacoordination structureactivity correlation oxygen reduction reaction

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