4.6 Article

Regulating single-atom Mn sites by precisely axial pyridinic-nitrogen coordination to stabilize the oxygen reduction

Journal

JOURNAL OF ENERGY CHEMISTRY
Volume 80, Issue -, Pages 542-552

Publisher

ELSEVIER
DOI: 10.1016/j.jechem.2023.01.048

Keywords

Single-atom manganese catalyst; Mn-N5 active moiety; Oxygen reduction reaction Coordination; number; Axial pyridinic-nitrogen coordination

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Significantly enhanced oxygen reduction reaction (ORR) activity can be achieved by accurately regulating the coordination number of isolated manganese (Mn) atoms. In this work, an atomically dispersed Mn-N5 catalyst was synthesized by precisely coordinating pyridinic-N into two-dimensional porous nanocarbon sheets, which exhibited outstanding catalytic activity and ultrahigh stability for ORR in zinc-air batteries. This work provides a new strategy for regulating the electronic structure of metal single-atoms and improving the overall ORR performance in energy systems.
Designing single-atom catalysts for oxygen reduction reaction (ORR) are fashionable but challenging to boost the zinc-air battery performance. Significantly enhanced ORR activity by manganese (Mn) single -atom catalysts can be achieved by accurately regulating the coordination number of isolated Mn atoms. Theoretical calculations indicate that the single Mn-N5 sites possess lower free energy barrier and higher oxygen adsorption performance than single Mn-N4 sites to accelerate the ORR kinetics. Target to it, here we synthesize an atomically dispersed Mn-N5 catalyst by precisely axial coordination of pyridinic-N doped into two-dimensional (2D) porous nanocarbon sheets (-3.56 nm thickness), which reveals out-standing catalytic activity and ultrahigh stability for the ORR in zinc-air battery owing to the inhomoge-neous charge distribution of Mn-N5 sites compared to the conventional single-site Mn-N4 catalyst and Pt/ C. This work gives a new strategy for in situ regulating the electronic structure of metal single-atoms and further promoting the overall ORR performance in energy systems.(c) 2023 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved.

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