Oxygen Vacancy-Electron Polarons Featured InSnRuO2 Oxides: Orderly and Concerted In-Ov-Ru-O-Sn Substructures for Acidic Water Oxidation

被引：0

作者：

Sun, Yanhui ^{[1
]}

Xiao, Mingyue ^{[1
]}

Liu, Feng ^{[2
]}

Gan, Jun ^{[2
]}

Gao, Shixin ^{[2
]}

Liu, Jingjun ^{[1
]}

机构：

[1] Beijing Key Laboratory of Electrochemical Process and Technology for Materials, Beijing University of Chemical Technology, Beijing,100029, China

[2] Yunnan Precious Metals Lab, Kunming,650100, China

来源：

Advanced Materials | 2024年 / 36卷 / 52期

关键词：

Polymetallic oxides with extraordinary electrons/geometry structure ensembles; trimmed electron bands; and way-out coordination environments; built by an isomorphic substitution strategy; may create unique contributing to concertedly catalyze water oxidation; which is of great significance for proton exchange membrane water electrolysis (PEMWE). Herein; well-defined rutile InSnRuO2 oxides with density-controllable oxygen vacancy (Ov)-free electron polarons are firstly fabricated by in situ isomorphic substitution; using trivalent In species as Ov generators and the adjacent metal ions as electron donors to form orderly and concerted In-Ov-Ru-O-Sn substructures in the tetravalent oxides. For acidic water oxidation; the obtained InSnRuO2 displays an ultralow overpotential of 183 mV (versus RHE) and a mass activity (MA) of 103.02 A mgRu−1; respectively. For a long-term stability test of PEMWE; it can run at a low and unchangeable cell potential (1.56 V) for 200 h at 50 mA cm−2; far exceeding current IrO2||Pt/C assembly in 0.5 m H2SO4. Accelerated degradation testing results of PEMWE with pure water as the electrolyte show no significant increase in voltage even when the voltage is gradually increased from 1 to 5 A cm−2. The remarkably improved performance is associated with the concerted In-Ov-Ru-O-Sn substructures stabilized by the dense Ov-electron polarons; which synergistically activates band structure of oxygen species and adjacent Ru sites and then boosting the oxygen evolution kinetics. More importantly; the self-trapped Ov-electron polaron induces a decrease in the entropy and enthalpy; and efficiently hinder Ru atoms leaching by increasing the lattice atom diffusion energy barrier; achieves long-term stability of the oxide. This work may open a door to design next-generation Ru-based catalysts with polarons to create orderly and asymmetric substructures as active sites for efficient electrocatalysis in PEMWE application. © 2024 Wiley-VCH GmbH;

D O I：

10.1002/adma.202414579

中图分类号：

学科分类号：

摘要：

引用