评估氧空位对 CaMn1-xFexO3-δ 包晶催化分解 N2O 的作用

IF 4.7 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General Pub Date : 2024-11-18 DOI:10.1016/j.apcata.2024.120026

Ana Serrano-Lotina , Emanuela Mastronardo , Juan M. Coronado

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引用次数: 0

摘要

使用氧化还原过氧化物催化分解 N2O 可以有效地减少这种分子的工业排放。在这里，我们选择了 CaMn1-xFexO3-δ (CMF) 氧化物作为催化剂，以探索氧空位对 N2O 分解的作用，因为这些材料的氧非配位热力学已被详细了解。CMF73 的转化率更高，而且具有良好的稳定性。在存在 N2O 的情况下，温度的变化会促使这种包晶石通过可逆地释放/吸收 O2 来快速调整 δ 值。与此同时，表面空位可参与 N-O 键的断裂，这是产生 N2 和 O2 的再生催化循环的一部分。一个简单的动力学模型显示，根据δ估算的氧空位数量与催化活性之间存在良好的相关性，这也是 CMF73 性能更佳的原因所在。

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Assessing the role of oxygen vacancies on N2O catalytic decomposition over CaMn1-xFexO3-δ perovskites

Catalytic decomposition of N₂O using redox perovskites can efficiently mitigate industrial emissions of this molecule. Here, we have selected the CaMn_1-xFe_xO_3-δ (CMF) oxides as catalysts to explore the role of oxygen vacancies on N₂O decomposition, because for these materials the thermodynamics of oxygen non-stoichiometry is known in detail Perovskites with two levels of Fe-doping, CMF73 (30 % at.) and CMF91 (10 % at.), were prepared and extensively characterized. Higher conversion is obtained over CMF73, which also presents good stability. In the presence of N₂O, variation of temperature prompts this perovskite to quickly adjust the value of δ by reversible release/uptake of O₂. In parallel, surface vacancies can participate in the breaking of the N-O bond, as a part of a regenerative catalytic cycle yielding N₂ and O₂. A simple kinetic model shows good correlation between the number of oxygen vacancies, estimated by δ, and the catalytic activity, explaining the better performance of CMF73.

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来源期刊

Applied Catalysis A: General 化学-环境科学

CiteScore

9.00

自引率

5.50%

发文量

415

审稿时长

24 days

期刊介绍： Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications. Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.