Issue 45, 2021

Spin unlocking oxygen evolution reaction on antiperovskite nitrides

Abstract

An efficient and low-cost oxygen evolution reaction (OER) electrocatalyst is key for electrochemical energy conversion and storage technologies. However, there is a lack of a strategy to guide the development of cost-effective antiperovskite nitrides with composition-sensitive function adjustability. Herein, we triggered the low-spin to high-spin transition of Fe3+ in Cu0.5NFe3.5 by partially doping Ni at the Fe sites, enabling Cu0.5NFe3Ni0.5 to significantly accelerate the oxidation of the in situ electrochemically formed amorphous FeNi (oxy)hydroxide redox couple, an initial water oxidation step, as well as subsequent water oxidation. Theoretical calculations indicated that the high-spin Fe3+ induces the formation of a paramagnetic FeNi (oxy)hydroxide catalytic layer on the ferromagnetic Cu0.5NFe3Ni0.5 core to accelerate the OER kinetics, thus Cu0.5NFe3Ni0.5 displays an overpotential of 244 mV at 10 mA cm−2 as an outstanding OER electrocatalyst, outperforming the benchmark IrO2 catalyst. Our findings are expected to unlock the potential of designing ideal antiperovskite-based electrocatalysts with adjustable spin states for use in the energy conversion and storage fields.

Graphical abstract: Spin unlocking oxygen evolution reaction on antiperovskite nitrides

Supplementary files

Article information

Article type
Paper
Submitted
03 Sept. 2021
Accepted
25 Okt. 2021
First published
10 Nov. 2021

J. Mater. Chem. A, 2021,9, 25435-25444

Spin unlocking oxygen evolution reaction on antiperovskite nitrides

H. Tang, D. Yang, M. Lu, S. Kong, Y. Hou, D. Liu, D. Liu, S. Yan, Z. Chen, T. Yu and Z. Zou, J. Mater. Chem. A, 2021, 9, 25435 DOI: 10.1039/D1TA07561F

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