La0.4Sr0.6FeO3-δ Perovskite 氧化物纳米粒子中的氧空位对氧进化反应的影响

Geletu Qing, Jingyi Chen
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摘要

氧空位是调整氧进化反应(OER)氧化物催化剂性能的重要因素。然而,如何控制氧空位的浓度,并将其对 OER 的影响与其他因素分离开来,仍然是一项挑战。在这项工作中,我们以特定成分/相态的 La0.4Sr0.6FeO3- d 包晶氧化物为例,采用改进的熔盐合成和臭氧处理方法来定制其纳米颗粒中的氧空位。比较了不同氧空位程度(0 至 25%)的 La0.4Sr0.6FeO3- d 纳米粒子的 OER 性能。OER 反应性随着材料中氧空位的增加而增加,但这种变化是非线性的。另一方面,OER 的稳定性呈双峰分布。完全氧化样品和最缺氧样品的活性降解速度慢于中间的两个样品。结果表明,设计出氧空位催化剂,使其具有最高的 OER 活性和稳定性是可行的。进一步研究氧空位与活性位点的关系将为设计和合成高OER性能的氧化物催化剂提供指导原则。
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Influence of Oxygen Vacancies in La0.4Sr0.6FeO3-δ Perovskite Oxide Nanoparticles for the Oxygen Evolution Reaction
Oxygen vacancies are important factors to tune the performance of oxide catalysts for the oxygen evolution reaction (OER). However, it remains challenging how to control the concentration of the oxygen vacancies and decouple their effects on OER from other factors. In this work, we use a specific composition/phase La0.4Sr0.6FeO3- d perovskite oxide as an example to tailor the oxygen vacancies of their nanoparticulate using a modified molten salt synthesis and ozone treatment. The OER performance of the resulting La0.4Sr0.6FeO3- d nanoparticles with different degree of oxygen vacancies ranging from 0 to 25% are compared. The OER reactivity increases with increased oxygen vacancies in the materials, but the change is nonlinear. The OER stability, on the other hand, has a bimodal distribution. The activities of fully oxidized sample and the most oxygen-deficient sample degrade slower than the two samples in the middle. The results suggest that it is feasible to design catalysts with oxygen vacancy to be the most OER active and stable. Further investigation into the oxygen vacancy – active site relation would offer guiding principle to design and synthesize high OER performance oxide catalysts.
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