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负载型金属氧化物上芳烃的催化氧化

The catalytic oxidation of aromatic hydrocarbons over supported metal oxide.

作者信息

Kim Sang Chai

机构信息

Department of Environmental Education, College of Engineering, Mokpo National University, 61 Torim-ri, Chungkye-myon, Muan-gun, Chonnam 534-729, South Korea.

出版信息

J Hazard Mater. 2002 Apr 26;91(1-3):285-99. doi: 10.1016/s0304-3894(01)00396-x.

DOI:10.1016/s0304-3894(01)00396-x
PMID:11900919
Abstract

The catalytic activity of metals (Cu, Mn, Fe, V, Mo, Co, Ni, Zn)/gamma-Al2O3 was investigated to bring about the complete oxidation of benzene, toluene and xylene (BTX). Among them, Cu/gamma-Al2O3 was found to be the most promising catalyst based on activity. X-ray diffraction (XRD), Brunauer Emmett Teller method (BET), electron probe X-ray micro analysis (EPMA) and temperature programmed reduction (TPR) by H2 were used to characterize a series of supported copper catalysts. Increasing the calcination temperature resulted in decreasing the specific surface areas of catalysts and, subsequently, the catalytic activity. Copper loadings on gamma-Al2O3 had a great effect on catalytic activity, and 5 wt.% Cu/gamma-Al2O3 catalyst was observed to be the most active, which might be contributed to the well-dispersed copper surface phase. Using TiO2 (anatase), TiO2 (rutile), SiO2 (I) and SiO2 (II) as support instead of gamma-Al2O3, the activity sequence of 5 wt.% Cu with respect to the support was gamma-Al2O3 > TiO2 (rutile) > TiO2 (anatase)>SiO2 (I) > SiO2 (II), and this appeared to be correlated with the distribution of copper on support rather than with the specific surface area of the catalyst. The smaller particle size of copper, due to its high dispersion on support, had a positive effect on catalytic activity. The activity of 5 wt.% Cu/gamma-Al2O3 with respect to the VOC molecule was observed to follow this sequence: toluene > xylene > benzene. Increasing the reactant concentration exerted an inhibiting effect on the catalytic activity.

摘要

研究了金属(铜、锰、铁、钒、钼、钴、镍、锌)/γ-氧化铝的催化活性,以实现苯、甲苯和二甲苯(BTX)的完全氧化。其中,基于活性发现Cu/γ-氧化铝是最有前景的催化剂。采用X射线衍射(XRD)、布鲁诺尔-埃米特-泰勒法(BET)、电子探针X射线微分析(EPMA)以及氢气程序升温还原(TPR)对一系列负载型铜催化剂进行了表征。提高煅烧温度导致催化剂比表面积减小,进而催化活性降低。γ-氧化铝上的铜负载量对催化活性有很大影响,观察到5 wt.% Cu/γ-氧化铝催化剂活性最高,这可能归因于铜表面相的良好分散。用TiO2(锐钛矿型)、TiO2(金红石型)、SiO2(I)和SiO2(II)代替γ-氧化铝作为载体,5 wt.% Cu相对于载体的活性顺序为γ-氧化铝>TiO2(金红石型)>TiO2(锐钛矿型)>SiO2(I)>SiO2(II),这似乎与铜在载体上的分布有关,而不是与催化剂的比表面积有关。由于铜在载体上的高分散性导致其粒径较小,这对催化活性有积极影响。观察到5 wt.% Cu/γ-氧化铝对VOC分子的活性遵循以下顺序:甲苯>二甲苯>苯。增加反应物浓度对催化活性有抑制作用。

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