Low-temperature catalytic degradation of chlorinated aromatic hydrocarbons over bimetallic Ce-Zr/UiO-66 catalysts
Low-temperature catalytic degradation of chlorinated aromatic hydrocarbons over bimetallic Ce-Zr/UiO-66 catalysts
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双金属 Ce-Zr/UiO-66 催化剂低温催化降解氯化芳烃
DOI：
10.1016/j.cej.2021.128782
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发表时间：
2021-02
影响因子：
15.1
通讯作者：
张海军
中科院分区：
文献类型：
--
作者：
樊芸;张海军
开发低温催化剂对减少工业热过程中氯代芳烃的排放具有重要意义。本文采用溶剂热法制备了Ce-Zr/UiO-66催化剂，并将其用于降解CAHs。粉末X射线衍射、傅里叶变换红外光谱和X射线光电子能谱分析表明，Ce成功地掺入到Zr/UiO-66的晶格中，而没有破坏金属有机骨架的结构。Ce-Zr/UiO-66催化剂对CAHs的降解活性随铈浓度的变化而变化。Ce0.2Zr0.8/UiO-66具有最大的表面积（1502 m2 g −1），在较低的加热温度（100-150 °C）下降解六氯苯的效率最高（>85%），生成的多氯二苯并对二恶英和二苯并呋喃较少。适量的水（5wt%）和氮气气氛有利于提高降解效率。降解产物的分析表明，催化剂上CAHs同时发生了加氢脱氯和氧化反应。
It is of great significance to develop the low-temperature catalysts for the reduction in emission of chlorinated aromatic hydrocarbons (CAHs) from the industrial thermal processes. In this work, the bimetallic Ce-Zr/UiO-66 catalysts were synthesized by a solvothermal method to degrade CAHs. Powder X-ray diffraction, Fourier transform infrared spectra and X-ray photoelectron spectroscopy analyses showed that cerium was successfully incorporated into the lattice of Zr/UiO-66 without destroying the structure of metal–organic frameworks. The activities of Ce-Zr/UiO-66 catalysts for CAHs degradation varied with the concentration of cerium. Ce0.2Zr0.8/UiO-66 with the highest surface area (1502 m2g−1) presented the highest efficiency (>85%) for hexachlorobenzene degradation at low heating temperature (100–150 °C) with less formation of polychlorinated dibenzo-p-dioxins and dibenzofurans. Appropriate amount of water (5 wt%) and nitrogen atmosphere were beneficial to improve degradation efficiency. The degradation products proved that hydrodechlorination and oxidation of CAHs both occurred on the catalysts.
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