期刊
JOURNAL OF MATERIALS CHEMISTRY A
卷 9, 期 48, 页码 27468-27484出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d1ta07293e
关键词
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资金
- ARC LIEF project [LE 110100223]
- Australian Research Council (Centre of Excellence for Electromaterials Science) [CE140100012]
- Australian Research Council (Future Fellowship) [FT200100317]
- Australian Renewable Energy Agency (Renewable Hydrogen for Export project) [2018/RND008 AS008]
- MNRE Government of India (NCPRE-Phase II, IIT Bombay)
- Early Career Research Award, Science and Engineering Research Board, Government of India [ECR/2016/000550]
- IITB-Monash Academy
In this study, antimony-metal oxides were synthesized and used as electrodes in water electrolysis reactions. Cobalt-antimony and manganese-antimony oxides showed good performance at room temperature, while the ruthenium-antimony system demonstrated exceptional stability at high temperatures.
Proton-exchange membrane water electrolysers provide many advantages for the energy-efficient production of H-2, but the current technology relies on high loadings of expensive iridium at the anodes, which are often unstable in operation. To address this, the present work scrutinises the properties of antimony-metal (Co, Mn, Ni, Fe, Ru) oxides synthesised as flat thin film electrodes by a solution-based method for water electrooxidation in 0.5 M H2SO4. Among the noble-metal-free catalysts, cobalt-antimony and manganese-antimony oxides demonstrate robust performance under ambient conditions, but slowly lose activity at elevated temperatures. A distinctive feature of the ruthenium-antimony system is its outstanding stability demonstrated herein through up to 8 day-long tests at 80 +/- 1 degrees C, during which the reaction rate of 10 mA cm(-2) was maintained at a stable overpotential of 0.34 +/- 0.01 V. The S-number for this catalyst is on par with those for the high-performance benchmark Ir-based systems. Density functional theory analysis and detailed physical characterisation reveal that this high stability is supported by the enhanced hybridisation of the oxygen p- and metal d-orbitals induced by antimony and can arise from two distinct structural scenarios: either formation of an antimonate phase, or nanoscale intermixing of metal and antimony oxide crystallites.
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