Combined In Situ X-Ray Spectroscopic and Theoretical Study on Trimetal Synergistic Enhancement of Water Oxidation

IF 24.4 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Advanced Energy Materials Pub Date : 2024-12-04 DOI:10.1002/aenm.202404599

Yalei Fan, Xubin Ye, Jing Zhou, Dabiao Lu, Chang-Yang Kuo, Yu-Cheng Huang, Ting-Shan Chan, Chien-Te Chen, Youwen Long, Jian-Qiang Wang, Zhiwei Hu, Linjuan Zhang

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引用次数: 0

Abstract

Electrochemical water-splitting is vital in energy storage and conversion applications. However, the sluggish kinetics of the oxygen evolution reaction (OER) hinders the electrochemical water-splitting. Therefore, developing efficient catalysts and understanding the OER mechanism are highly desirable. This study successfully synthesized a new quadruple perovskite oxide CaCu₃Co₂Ru₂O₁₂ (CCCRO) catalyst exhibiting high OER activity with overpotential 198 mV at 10 mA cm⁻², a Tafel slope of 37 mV dec⁻¹, and long-term operational stability with a current density of 500 mA cm⁻² for >500 h. The in situ X-ray absorption near-edge structure (XANES) indicated that a part of high-spin (HS) Co³⁺ ions and low-spin (LS) Ru⁵⁺ ions transitioned to the tetravalent Co (IV) and hexavalent Ru (VI) valence states under OER. However, the Cu²⁺ valence state remained unchanged. Furthermore, the density functional theory (DFT) calculations reveal that the lattice-oxygen oxidation mechanism (LOM) rather than conventional adsorbate evolution mechanism (AEM) is responsible for high OER activity in Ru (VI)-O-Co (IV) network, and that the Cu(A’)/Co(B)/Ru(B’) three sites synergistically facilitate the OER activity for CCCRO.

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来源期刊

Advanced Energy Materials CHEMISTRY, PHYSICAL-ENERGY & FUELS

CiteScore

41.90

自引率

4.00%

发文量

889

审稿时长

1.4 months

期刊介绍： Established in 2011, Advanced Energy Materials is an international, interdisciplinary, English-language journal that focuses on materials used in energy harvesting, conversion, and storage. It is regarded as a top-quality journal alongside Advanced Materials, Advanced Functional Materials, and Small. With a 2022 Impact Factor of 27.8, Advanced Energy Materials is considered a prime source for the best energy-related research. The journal covers a wide range of topics in energy-related research, including organic and inorganic photovoltaics, batteries and supercapacitors, fuel cells, hydrogen generation and storage, thermoelectrics, water splitting and photocatalysis, solar fuels and thermosolar power, magnetocalorics, and piezoelectronics. The readership of Advanced Energy Materials includes materials scientists, chemists, physicists, and engineers in both academia and industry. The journal is indexed in various databases and collections, such as Advanced Technologies & Aerospace Database, FIZ Karlsruhe, INSPEC (IET), Science Citation Index Expanded, Technology Collection, and Web of Science, among others.