期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 -, 期 -, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202312409
关键词
Bifunctional Active Sites; Oxygen Reduction; S-Block Metal K; S-Orbital Electron Structure; Single Atom
This study reports a novel s-block potassium catalyst with excellent activity and stability for the oxygen reduction reaction under alkaline conditions. The catalyst shows bifunctional active sites and can optimize the free energy of ORR reaction intermediates.
Currently, single-atom catalysts (SACs) research mainly focuses on transition metal atoms as active centers. Due to their delocalized s/p-bands, the s-block main group metal elements are typically regarded as catalytically inert. Herein, an s-block potassium SAC (K-N-C) with K-N4 configuration is reported for the first time, which exhibits excellent oxygen reduction reaction (ORR) activity and stability under alkaline conditions. Specifically, the half-wave potential (E1/2) is up to 0.908 V, and negligible changes in E1/2 are observed after 10,000 cycles. In addition, the K-N-C offers an exceptional power density of 158.1 mW cm-2 and remarkable durability up to 420 h in a Zn-air battery. Density functional theory (DFT) simulations show that K-N-C has bifunctional active K and C sites, can optimize the free energy of ORR reaction intermediates, and adjust the rate-determining steps. The crystal orbital Hamilton population (COHP) results showed that the s orbitals of K played a major role in the adsorption of intermediates, which was different from the d orbitals in transition metals. This work significantly guides the rational design and catalytic mechanism research of s-block SACs with high ORR activity.
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