A universal chemical-induced tensile strain tuning strategy to boost oxygen-evolving electrocatalysis on perovskite oxides

Daqin Guan, Jian Zhong, Hengyue Xu, Yu Cheng Huang, Zhiwei Hu, Bin Chen, Yuan Zhang, Meng Ni, Xiaomin Xu, Wei Zhou, Zongping Shao

Research output: Journal article publicationJournal articleAcademic researchpeer-review

Abstract

Exploring effective, facile, and universal tuning strategies to optimize material physicochemical properties and catalysis processes is critical for many sustainable energy systems, but still challenging. Herein, we succeed to introduce tensile strain into various perovskites via a facile thermochemical reduction method, which can greatly improve material performance for the bottleneck oxygen-evolving reaction in water electrolysis. As an ideal proof-of-concept, such a chemical-induced tensile strain turns hydrophobic Ba5Co4.17Fe0.83O14-δ perovskite into the hydrophilic one by modulating its solid-liquid tension, contributing to its beneficial adsorption of important hydroxyl reactants as evidenced by fast operando spectroscopy. Both surface-sensitive and bulk-sensitive absorption spectra show that this strategy introduces oxygen vacancies into the saturated face-sharing Co-O motifs of Ba5Co4.17Fe0.83O14-δ and transforms such local structures into the unsaturated edge-sharing units with positive charges and enlarged electrochemical active areas, creating a molecular-level hydroxyl pool. Theoretical computations reveal that this strategy well reduces the thermodynamic energy barrier for hydroxyl adsorption, lowers the electronic work function, and optimizes the charge/electrostatic potential distribution to facilitate the electron transport between active sites and hydroxyl reactants. Also, this strategy is reliable for other single, double, and Ruddlesden-Popper perovskites. We believe that this finding will enlighten rational material design and in-depth understanding for many potential applications.

Original languageEnglish
Article number011422
JournalApplied Physics Reviews
Volume9
Issue number1
DOIs
Publication statusPublished - 1 Mar 2022

ASJC Scopus subject areas

  • Physics and Astronomy(all)

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