Well‐defined N3C1‐anchored Single‐Metal‐Sites for Oxygen Reduction Reaction

Author:

Huang Senhe1ORCID,Tranca Diana1,Rodríguez‐Hernández Fermin1,Zhang Jichao2,Lu Chenbao13,Zhu Jinhui1,Liang Hai‐Wei4,Zhuang Xiaodong15ORCID

Affiliation:

1. The Soft2D Lab State Key Laboratory of Metal Matrix Composites Shanghai Key Laboratory of Electrical Insulation and Thermal Ageing School of Chemistry and Chemical Engineering Shanghai Jiao Tong University Shanghai 200240 China

2. Shanghai Synchrotron Radiation Facility Zhangjiang Laboratory Shanghai Advanced Research Institute Chinese Academy of Sciences 239, Zhangheng Road Shanghai 201204 China

3. College of Chemistry Zhengzhou University Zhengzhou 450001 Henan China

4. Department of Chemistry University of Science and Technology of China Jinzhai Road 96 Hefei 230026 China

5. Frontiers Science Center for Transformative Molecules Zhang Jiang Institute for Advanced Study Shanghai Jiao Tong University Shanghai 201203 China

Abstract

AbstractN‐, C‐, O‐, S‐coordinated single‐metal‐sites (SMSs) have garnered significant attention due to the potential for significantly enhanced catalytic capabilities resulting from charge redistribution. However, significant challenges persist in the precise design of well‐defined such SMSs, and the fundamental comprehension has long been impeded in case‐by‐case reports using carbon materials as investigation targets. In this work, the well‐defined molecular catalysts with N3C1‐anchored SMSs, i.e., N‐confused metalloporphyrins (NCPor‐Ms), are calculated for their catalytic oxygen reduction activity. Then, NCPor‐Ms with corresponding N4‐anchored SMSs (metalloporphyrins, Por‐Ms), are synthesized for catalytic activity evaluation. Among all, NCPor‐Co reaches the top in established volcano plots. NCPor‐Co also shows the highest half‐wave potential of 0.83 V vs. RHE, which is much better than that of Por‐Co (0.77 V vs. RHE). Electron‐rich, low band gap and regulated d‐band center contribute to the high activity of NCPor‐Co. This study delves into the examination of well‐defined asymmetric SMS molecular catalysts, encompassing both theoretical and experimental facets. It serves as a pioneering step towards enhancing the fundamental comprehension and facilitating the development of high‐performance asymmetric SMS catalysts.

Funder

National Natural Science Foundation of China

Publisher

Wiley

Subject

General Medicine

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