Entropy Enhanced Perovskite Oxide Ceramic for Efficient Electrochemical Reduction of Oxygen to Hydrogen Peroxide

Angew Chem Int Ed Engl. 2022 May 16;61(21):e202200086. doi: 10.1002/anie.202200086. Epub 2022 Mar 23.

Abstract

The electrochemical oxygen reduction reaction (ORR) offers a most promising and efficient route to produce hydrogen peroxide (H2 O2 ), yet the lack of cost-effective and high-performance electrocatalysts have restricted its practical application. Herein, an entropy-enhancement strategy has been employed to enable the low-cost perovskite oxide to effectively catalyze the electrosynthesis of H2 O2 . The optimized Pb(NiWMnNbZrTi)1/6 O3 ceramic is available on a kilogram-scale and displays commendable ORR activity in alkaline media with high selectivity over 91 % across the wide potential range for H2 O2 including an outstanding degradation property for organic dyes through the Fenton process. The exceptional performance of this perovskite oxide is attributed to the entropy stabilization-induced polymorphic transformation assuring the robust structural stability, decreased charge mobility as well as synergistic catalytic effects which we confirm using advanced in situ Raman, transient photovoltage, Rietveld refinement as well as finite elemental analysis.

Keywords: Electrocatalysis; High Entropy; Hydrogen Peroxide; Oxygen Reduction Reaction; Perovskite Oxide Ceramic.