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氧化还原诱导的具有丰富氧空位的 MnO 在整体式铜泡沫上的生长用于增强甲苯燃烧。

Redox-Induced Growth of MnO with Rich Oxygen Vacancies over Monolithic Copper Foam for Boosting Toluene Combustion.

机构信息

State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210023, China.

出版信息

Environ Sci Technol. 2023 Jun 20;57(24):9096-9104. doi: 10.1021/acs.est.3c02103. Epub 2023 Jun 8.

Abstract

Catalytic combustion has been known to be an effective technique in volatile organic compound (VOC) abatement. Developing monolithic catalysts with high activity at low temperatures is vital yet challenging in industrial applications. Herein, monolithic MnO-O/CF catalysts were fabricated via the growth of KCuFe(CN) (CuFePBA, a family of metal-organic frames) over copper foam (CF) followed by a redox-etching route. The as-synthesized monolith MnO-O-0.04/CF catalyst displays a superior low-temperature activity (T = 215 °C) and robust durability for toluene elimination even in the presence of 5 vol % water. Experimental results reveal that the CuFePBA template not only guides the growth of δ-MnO with high loading over CF but also acts as a source of dopant to create more oxygen vacancies and weaken the strength of the Mn-O bond, which considerably improves the oxygen activation ability of δ-MnO and consequently boosts the low-temperature catalytic activity of the monolith MnO-O-0.04/CF toward toluene oxidation. In addition, the reaction intermediate and proposed mechanism in the MnO-O-0.04/CF mediated catalytic oxidation process were investigated. This study provides new insights into the development of highly active monolithic catalysts for the low-temperature oxidation of VOCs.

摘要

催化燃烧已被证明是一种有效去除挥发性有机化合物 (VOC) 的技术。在工业应用中,开发在低温下具有高活性的整体式催化剂至关重要,但极具挑战性。在此,通过在泡沫铜 (CF) 上生长 KCuFe(CN) (CuFePBA,一种金属有机骨架),然后进行氧化还原刻蚀路线,制备了整体式 MnO-O/CF 催化剂。所合成的整体式 MnO-O-0.04/CF 催化剂在甲苯消除反应中表现出优异的低温活性 (T = 215°C) 和稳健的耐久性,即使在存在 5 vol%水的情况下也是如此。实验结果表明,CuFePBA 模板不仅引导了高负载量的 δ-MnO 在 CF 上的 生长,而且还作为掺杂剂的来源,创造了更多的氧空位并削弱了 Mn-O 键的强度,这极大地提高了 δ-MnO 的氧活化能力,并因此提高了整体式 MnO-O-0.04/CF 对甲苯氧化的低温催化活性。此外,还研究了 MnO-O-0.04/CF 介导的催化氧化过程中的反应中间体和提出的反应机制。本研究为开发用于低温氧化 VOCs 的高活性整体式催化剂提供了新的见解。

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