Key Laboratory of Environmental Nanotechnology and Health Effects, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China; National Engineering Laboratory for VOCs Pollution Control Material & Technology, Research Center for Environmental Material and Pollution Control Technology, University of Chinese Academy of Sciences, Beijing 101408, China.
National Engineering Laboratory for VOCs Pollution Control Material & Technology, Research Center for Environmental Material and Pollution Control Technology, University of Chinese Academy of Sciences, Beijing 101408, China.
J Environ Sci (China). 2020 Oct;96:55-63. doi: 10.1016/j.jes.2020.03.015. Epub 2020 May 6.
In this work, a series of Cu-ZSM-5 catalysts with different SiO/AlO ratios (25, 50, 100 and 200) were synthesized and investigated in n-butylamine catalytic degradation. The n-butylamine can be completely catalytic degradation at 350°C over all Cu-ZSM-5 catalysts. Moreover, Cu-ZSM-5 (25) exhibited the highest selectivity to N, exceeding 90% at 350°C. These samples were investigated in detail by several characterizations to illuminate the dependence of the catalytic performance on redox properties, Cu species, and acidity. The characterization results proved that the redox properties and chemisorption oxygen primarily affect n-butylamine conversion. N selectivity was impacted by the Brønsted acidity and the isolated Cu species. Meanwhile, the surface acid sites over Cu-ZSM-5 catalysts could influence the formation of Cu species. Furthermore, in situ diffuse reflectance infrared Fourier transform spectra was adopted to explore the reaction mechanism. The Cu-ZSM-5 catalysts are the most prospective catalysts for nitrogen-containing volatile organic compounds removal, and the results in this study could provide new insights into catalysts design for VOC catalytic oxidation.
在这项工作中，合成了一系列具有不同 SiO/AlO 比（25、50、100 和 200）的 Cu-ZSM-5 催化剂，并研究了其在正丁胺催化降解中的应用。所有 Cu-ZSM-5 催化剂均能在 350°C 下完全催化降解正丁胺。此外，Cu-ZSM-5（25）在 350°C 时对 N 的选择性最高，超过 90%。通过多种表征方法对这些样品进行了详细研究，以阐明催化性能对氧化还原性能、Cu 物种和酸度的依赖关系。表征结果证明，氧化还原性能和化学吸附氧主要影响正丁胺的转化率。Brønsted 酸度和孤立的 Cu 物种影响 N 的选择性。同时，Cu-ZSM-5 催化剂表面的酸位会影响 Cu 物种的形成。此外，还采用原位漫反射红外傅里叶变换光谱法探究了反应机理。Cu-ZSM-5 催化剂是最有前途的用于去除含氮挥发性有机化合物的催化剂，本研究的结果可为 VOC 催化氧化催化剂的设计提供新的思路。
