Cu-MnO2 催化剂协同去除氮氧化物和甲苯及其相互作用机理

IF 6.7 1区 工程技术 Q2 ENERGY & FUELS Fuel Pub Date : 2024-09-07 DOI:10.1016/j.fuel.2024.133009
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引用次数: 0

摘要

挥发性有机化合物(VOCs)和氮氧化物(NOx)在雾霾和光化学烟雾的形成过程中起着重要作用,对环境和人类健康构成严重威胁。甲苯是一种典型的挥发性有机化合物,经常与氮氧化物共存于各种移动或固定烟气中。然而,目前对它们协同去除的相互影响的了解仍然有限。本研究采用沉淀法制备了 Cu-MnO2 催化剂,该催化剂对氮氧化物和甲苯具有协同去除活性,并对 N2 和 CO2 具有选择性。研究了其相互作用机理,特别是氮氧化物对甲苯吸附和氧化性能的影响。氮氧化物对甲苯的抑制程度随氮氧化物浓度的增加而增加。此外,还发现了氮氧化物对甲苯氧化的多种抑制方式,包括氮氧化物和甲苯在催化剂表面的竞争吸附,突破实验证明了这一点。TPD 和 XPS 表征表明,氮氧化物的加入减少了氧空位,从而削弱了甲苯氧化性能。此外,还进行了原位 DRIFT 表征,发现氮氧化物的添加影响了甲苯的氧化过程。除了苯甲醇、苯甲醛和苯甲酸之外,还出现了亚硝酸盐中间产物,它们的沉积也是甲苯氧化能力下降的原因。这项工作对协同去除氮氧化物和挥发性有机化合物过程中各种成分之间的相互作用机制提供了新的见解。
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Synergistic removal of nitrogen oxides and toluene and their interaction mechanism on Cu-MnO2 catalyst

Volatile organic compounds (VOCs) and nitrogen oxides (NOx) contribute significantly to the formation of haze and photochemical smog, posing substantial threats to both the environment and human health. Toluene, a typical VOCs, often coexists with NOx in various mobile or stationary flue gases. However, the current understanding of the mutual influence of their synergistic removal remains limited. In this work, the Cu-MnO2 catalyst was prepared using the precipitation method, which demonstrated synergistic removal activity for both NOx and toluene, as well as selectivity towards N2 and CO2. The interaction mechanism was investigated, particularly focusing on the effect of NOx on the adsorption and oxidation performance of toluene. The degree to which NOx inhibits toluene increases with NOx concentration. Furthermore, multiple inhibition ways of NOx on toluene oxidation were discovered, including competitive adsorption of NOx and toluene on the catalyst surface, as evidenced by the breakthrough experiments. TPD and XPS characterization indicated that the addition of NOx reduces oxygen vacancies, thereby weakening toluene oxidation performance. In addition, in-situ DRIFT characterization was conducted, and it was found that the addition of NOx affected the oxidation process of toluene. Apart from benzyl alcohol, benzaldehyde, and benzoic acid, intermediate nitrite species also appeared, and their deposition was also the reason for the decrease in toluene oxidation ability. This work provides new insights into the interaction mechanisms between various components in the collaborative removal of NOx and VOCs.

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来源期刊
Fuel
Fuel 工程技术-工程:化工
CiteScore
12.80
自引率
20.30%
发文量
3506
审稿时长
64 days
期刊介绍: The exploration of energy sources remains a critical matter of study. For the past nine decades, fuel has consistently held the forefront in primary research efforts within the field of energy science. This area of investigation encompasses a wide range of subjects, with a particular emphasis on emerging concerns like environmental factors and pollution.
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