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Mn-Ce/ZSM-5 催化三乙胺的选择性氧化。

Selective Oxidation of Triethylamine Catalyzed by Mn-Ce/ZSM-5.

机构信息

School of Chemistry and Chemical Engineering, Nanjing University of Science and Technology, Nanjing 210094, Jiangsu, People's Republic of China.

出版信息

Langmuir. 2023 Jun 6;39(22):7820-7830. doi: 10.1021/acs.langmuir.3c00696. Epub 2023 May 23.

DOI:10.1021/acs.langmuir.3c00696
PMID:37220175
Abstract

The selective catalytic oxidation (SCO) of triethylamine (TEA) to harmless nitrogen (N), carbon dioxide (CO), and water (HO) is of green elimination technology. In this paper, Mn-Ce/ZSM-5 with different proportions of MnO/CeO were studied for the selective catalytic combustion of TEA. The catalysts were characterized by XRD, BET, H-TPR, XPS, and NH-TPD and their catalytic activities were analyzed. The results showed that MnO was the main active component. The addition of a small amount of CeO promotes the generation of high-valence Mn ions, which reduces the reduction temperature of the catalyst and increases the redox capacity of the catalyst. In addition, the synergistic effect between CeO and MnO significantly improves the mobility of reactive oxygen species on the catalyst, thus improving the catalytic performance of the catalyst. The catalytic oxidation performance of TEA over 15Mn5Ce/ZSM-5 is the highest. TEA can be completely converted at 220 °C, and the selectivity for N is up to 80%. The reaction mechanism was studied by in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS).

摘要

三乙胺(TEA)选择性催化氧化(SCO)转化为无害的氮(N)、二氧化碳(CO)和水(HO)是一种绿色消除技术。本文研究了不同 MnO/CeO 比例的 Mn-Ce/ZSM-5 催化剂用于 TEA 的选择性催化燃烧。采用 XRD、BET、H-TPR、XPS 和 NH-TPD 对催化剂进行了表征,并分析了其催化活性。结果表明,MnO 是主要的活性组分。少量 CeO 的添加促进了高价 Mn 离子的生成,降低了催化剂的还原温度,增加了催化剂的氧化还原能力。此外,CeO 和 MnO 之间的协同作用显著提高了催化剂上活性氧物种的迁移率,从而提高了催化剂的催化性能。15Mn5Ce/ZSM-5 上的 TEA 催化氧化性能最高。在 220°C 下可完全转化 TEA,N 的选择性高达 80%。通过原位漫反射红外傅里叶变换光谱(in situ DRIFTS)研究了反应机理。

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