Operando Identification of Dual Active Sites in Ca2IrO4Nanocrystals with Yttrium Substitutions Boosting Acidic Oxygen Evolution Reaction

Yuying Liu, Liang Cai*, Qianqian Ji, Chao Wang, Ziyi Liu, Liyang Lv, Bing Tang, Hengli Duan, Fengchun Hu, Huijuan Wang, Na Li*, Zhihu Sun, Wensheng Yan*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

9 Scopus citations

Abstract

Non-noble metal substitutions of the iridium sites in iridium-based complex oxides while boosting acidic oxygen evolution reaction (OER) is a promising method for developing efficient electrocatalysts, but this remains a huge challenge. Herein, we report yttrium substitution of iridium in Ca2IrO4(Ca2YxIr1-xO4) nanocrystals for the first time, which is demonstrated by detailed structural characterizations using X-ray absorption spectra, X-ray diffraction patterns, and elemental mapping images. The synthesized Ca2Y0.2Ir0.8O4catalyst requires a low overpotential of only 213 mV, achieving an acidic OER current density of 10 mA cm-2, which represents an approximately 203.7-fold improvement in iridium mass activity and 204.4-fold improvement in turnover frequency in comparison to that of IrO2at 1.5 V vs RHE, respectively. Systematic characterizations of electronic structures reveal the synergistic effects between high-valence iridium sites and increased lattice oxygen concentration induced by Y3+substitutions, which greatly enhance the intrinsic OER activity of Ca2Y0.2Ir0.8O4. Operando X-ray absorption spectra and Raman spectra reveal the iridium and yttrium dual active sites during acidic OER. Our results provide a method for designing dual active sites in iridium-based complex oxides for highly active acidic OER electrocatalysts.

Original languageEnglish (US)
Pages (from-to)3798-3806
Number of pages9
JournalACS Energy Letters
Volume7
Issue number11
DOIs
StatePublished - Nov 11 2022

ASJC Scopus subject areas

  • Chemistry (miscellaneous)
  • Renewable Energy, Sustainability and the Environment
  • Fuel Technology
  • Energy Engineering and Power Technology
  • Materials Chemistry

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