Well-defined N3 C1 -anchored Single-Metal-Sites for Oxygen Reduction Reaction.
Angew Chem Int Ed Engl
; 63(1): e202314833, 2024 Jan 02.
Article
en En
| MEDLINE
| ID: mdl-37994382
N-, 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 N3 C1 -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 0.83â
V vs. RHE, which is much better than that of Por-Co (0.77â
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.
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1
Colección:
01-internacional
Base de datos:
MEDLINE
Idioma:
En
Revista:
Angew Chem Int Ed Engl
Año:
2024
Tipo del documento:
Article
País de afiliación:
China
Pais de publicación:
Alemania