期刊
ENERGY & ENVIRONMENTAL SCIENCE
卷 15, 期 6, 页码 2356-2365出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d1ee03610f
关键词
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资金
- National Natural Science Foundation of China [21922811, 21961160742, 21878270, 22178308]
- Zhejiang Provincial Natural Science Foundation of China [LR19B060002]
- Leading Innovative and Entrepreneur Team Introduction Program of Zhejiang [2019R01006]
- Startup Foundation for Hundred-Talent Program of Zhejiang University, National Natural Science Foundation of China [U20A20246]
- Fundamental Research Funds for the Central Universities [CCNU20ZT003]
- Key Laboratory of Marine Materials and Related Technologies, Chinese Academy of Science
- Zhejiang Key Laboratory of Marine Materials and Protective Technologies [2020K10]
- New York State's Center of Excellence in Materials Informatics (CMI) at the University at Buffalo
Designing acid-stable oxygen evolution reaction (OER) electrocatalysts with low noble-metal content is crucial for green hydrogen generation. In this study, a rutile-structured ruthenium-manganese solid solution oxide with oxygen vacancies (Mn0.73Ru0.27O2-delta) was developed using an electron-feeding modulation strategy. The catalyst exhibited optimal electronic structure and enhanced electrical conductivity, leading to low overpotential and improved OER kinetics. The incorporation of Mn components and O vacancies modulated the adsorption and desorption energy barriers, improving the overall OER kinetics.
Designing acid-stable oxygen evolution reaction (OER) electrocatalysts with low noble-metal content to facilitate the sluggish kinetics is crucial for sustaining green hydrogen generation. Herein, we developed a rutile-structured ruthenium-manganese solid solution oxide with oxygen vacancies (Mn0.73Ru0.27O2-delta) by using an electron-feeding modulation strategy to stabilize the catalyst structure and accelerate the OER kinetics. Due to the optimal electronic structure and enhanced electrical conductivity, the Mn0.73Ru0.27O2-delta catalyst displayed a low overpotential of 208 mV to reach 10 mA cm(-2) current density in 0.5 M H2SO4 electrolyte, outperforming the benchmark RuO2 and most previously reported noble-metal based OER catalysts. Experimental characterization verified that the electron transfer occurred from Ru to Mn atoms with the bridging O atom, which was further enhanced with the existence of oxygen vacancies. Therefore, the center Ru active sites in an electron-deficient state is favorable for bonding with active oxygen intermediates. Meanwhile, theoretical calculations revealed that the simultaneous incorporation of Mn components and O vacancies significantly decreased the anti-bonding spin states of Ru's d-orbitals, which modulated the adsorption and desorption energy barriers of elementary reactions on the active Ru sites, thus boosting the overall OER kinetics.
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