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采用超声能量合成的 CuO/CeO2-ZrO2 纳米催化剂用于湿空气氧化法降解苯酚:物理化学特性表征和催化性能。

Degradation of phenol via wet-air oxidation over CuO/CeO2-ZrO2 nanocatalyst synthesized employing ultrasound energy: physicochemical characterization and catalytic performance.

出版信息

Environ Technol. 2014 May-Jun;35(9-12):1140-9. doi: 10.1080/09593330.2013.863952.

Abstract

Catalytic wet air oxidation (CWAO) of phenol was carried out under atmospheric pressure of oxygen at 160 degrees C in a stirred batch reactor over copper catalysts supported by CeO2-ZrO2. The copper with different loadings were impregnated over the composite support by a sonication process. The catalysts were characterized by X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM), energy dispersive X-ray analysis (EDX), Brunauer-Emmett-Teller (BET) specific surface area and Fourier-transformed infrared analyses. Characteristic peaks attributed to copper were not found in XRD patterns even at high loadings, but based on EDX results, the existence of copper particles was confirmed. It means that sonochemical synthesis method even at high loadings produced small copper particles with low crystallinity and excellent dispersion over the CeO2-ZrO2 composite. FESEM micrographs indicated just slight enhancement in particle size at high loadings of Cu. Blank CWAO experiments illustrated low conversion of phenol using bare CeO2-ZrO2 support. Although some agglomeration of particles was found at high loadings of copper but owning to the fact that almost all ZrO2 particles incorporated into the CeO2 lattice at high contents of Cu, catalyst activity not only did not decrease but also the phenol conversion reached to the higher values. The optimal catalyst loading for phenol degradation was found to be 9 g/l. Complete conversion of phenol was achieved using CuO/CeO2-ZrO2 in 9 g/l catalyst loading with initial phenol concentration of 1000 ppm after 3 h of reaction.

摘要

在搅拌间歇式反应器中,在大气压氧气和 160°C 的条件下,用 CeO2-ZrO2 负载的铜催化剂进行苯酚的催化湿式氧化(CWAO)。通过超声处理过程将不同负载量的铜浸渍在复合载体上。采用 X 射线衍射(XRD)、场发射扫描电子显微镜(FESEM)、能谱分析(EDX)、Brunauer-Emmett-Teller(BET)比表面积和傅里叶变换红外分析对催化剂进行了表征。即使在高负载量下,XRD 图谱中也没有发现归因于铜的特征峰,但根据 EDX 结果,证实了铜颗粒的存在。这意味着,即使在高负载量下,超声化学合成方法也能在 CeO2-ZrO2 复合载体上生成低结晶度和高分散度的小铜颗粒。FESEM 微观照片表明,在高铜负载量下,颗粒尺寸仅略有增加。空白 CWAO 实验表明,使用裸 CeO2-ZrO2 载体时,苯酚的转化率较低。尽管在高铜负载量下发现了一些颗粒团聚,但由于在高 Cu 含量下几乎所有的 ZrO2 颗粒都融入到 CeO2 晶格中,催化剂活性不仅没有降低,而且苯酚转化率达到了更高的值。发现苯酚降解的最佳催化剂负载量为 9 g/l。在初始苯酚浓度为 1000 ppm、催化剂负载量为 9 g/l 的条件下,使用 CuO/CeO2-ZrO2 可在 3 h 内实现苯酚的完全转化。

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