Issue 27, 2023

Boosting oxygen evolution reaction performance via metal defect-induced lattice oxygen redox reactions on spinel oxides

Abstract

High-performance and low-cost oxygen evolution reaction (OER) catalysts are essential for sustainable energy-to-hydrogen conversion. Defect engineering has been extensively used to optimize the structure and performance of catalysts. Metal defects have been found to be highly stable relative to oxygen defects in oxygen-rich environments and possess unique electronic structures. However, the formation of metal defects has a high energy cost, and traditional adsorbate evolution mechanism (AEM) catalysts have limited active sites. Here, lattice oxygen-mediated mechanism (LOM) spinel catalysts were successfully fabricated by controllably introducing metal defects to enhance OER efficiency. X-ray absorption spectra indicated that the metal defects induced electron delocalization and redistributed electron density between metal and ligand. Density functional theory calculations revealed that the metal defects elevated the position of the O p-band center, decreased the formation enthalpy of the oxygen defects and altered the adsorption sites, verifying the mechanism switch from the AEM to the LOM. Therefore, the metal defect-enriched ZnFe2O4 exhibited enhanced OER activity, delivering a low overpotential of 236 mV @ 10 mA cm−2 with a small Tafel slope of 67.24 mV dec−1 for the OER in KOH. This work facilitates the development of novel high-performance activated lattice oxygen redox electrocatalysts through cation defect engineering in spinel oxides.

Graphical abstract: Boosting oxygen evolution reaction performance via metal defect-induced lattice oxygen redox reactions on spinel oxides

  • This article is part of the themed collection: #MyFirstJMCA

Supplementary files

Article information

Article type
Paper
Submitted
06 Mar 2023
Accepted
26 Jun 2023
First published
26 Jun 2023

J. Mater. Chem. A, 2023,11, 15044-15053

Boosting oxygen evolution reaction performance via metal defect-induced lattice oxygen redox reactions on spinel oxides

J. Zheng, R. Sun, D. Meng, J. Guo and Z. Wang, J. Mater. Chem. A, 2023, 11, 15044 DOI: 10.1039/D3TA01385E

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