Insight into the catalytic oxidation of toluene over M/ZSM-5 (M=Cu, Mn, Fe, Ce, Ti) catalysts

Q3 Energy

燃料化学学报 Pub Date : 2023-06-01 DOI:10.1016/S1872-5813(22)60069-0

Xin-yu PENG , Li-jun LIU , Bo-xiong SHEN , Yao BIAN , Li-chao SU

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引用次数: 0

Abstract

A series of metal oxide catalysts were prepared by impregnating Cu, Mn, Fe, Ce and Ti on ZSM-5 molecular sieve. The physicochemical properties of the catalysts were characterized by SEM, XRD, N₂ adsorption/desorption, XPS, H₂-TPR, and the catalytic oxidation of toluene was investigated. The results showed that Cu/ZSM-5 had rough surface, uniform distribution of metal, good pore structure, superior low-temperature reducibility and abundant adsorbed oxygen species. Cu/ZSM-5 with 5% loading exhibited excellent catalytic activity for toluene oxidation and the best sulfur resistance performance, with t₉₀ (GHSV=24000 h⁻¹) being 224 °C in SO₂ environment. In-situ DRIFTS experiments revealed that the degradation path of toluene was as follows: toluene was first adsorbed on the surface of the catalyst to form adsorbed toluene, then it was converted into benzaldehyde and benzoic acid successively on the catalyst. And small molecule organics such as maleic acid and carboxylic acid were formed through ring opening reaction, and finally was oxidized to CO₂ and H₂O.

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M/ZSM-5 (M=Cu, Mn, Fe, Ce, Ti)催化剂催化氧化甲苯的研究

通过在ZSM-5分子筛上浸渍Cu、Mn、Fe、Ce和Ti，制备了一系列金属氧化物催化剂。采用SEM、XRD、N2吸附/脱附、XPS、H2-TPR等手段对催化剂的理化性质进行了表征，并对甲苯的催化氧化进行了研究。结果表明，Cu/ZSM-5表面粗糙，金属分布均匀，孔隙结构良好，低温还原性好，吸附的氧种类丰富。负载5%的Cu/ZSM-5在SO2环境下的t90 (GHSV=24000 h−1)为224℃，具有优异的甲苯氧化催化活性和最佳的抗硫性能。原位DRIFTS实验表明，甲苯的降解路径为:甲苯首先吸附在催化剂表面形成吸附甲苯，然后在催化剂上依次转化为苯甲醛和苯甲酸。通过开环反应形成马来酸、羧酸等小分子有机物，最终氧化为CO2和H2O。

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来源期刊

燃料化学学报 Chemical Engineering-Chemical Engineering (all)

CiteScore

2.80

自引率

0.00%

发文量

5825

期刊介绍： Journal of Fuel Chemistry and Technology (Ranliao Huaxue Xuebao) is a Chinese Academy of Sciences(CAS) journal started in 1956, sponsored by the Chinese Chemical Society and the Institute of Coal Chemistry, Chinese Academy of Sciences(CAS). The journal is published bimonthly by Science Press in China and widely distributed in about 20 countries. Journal of Fuel Chemistry and Technology publishes reports of both basic and applied research in the chemistry and chemical engineering of many energy sources, including that involved in the nature, processing and utilization of coal, petroleum, oil shale, natural gas, biomass and synfuels, as well as related subjects of increasing interest such as C1 chemistry, pollutions control and new catalytic materials. Types of publications include original research articles, short communications, research notes and reviews. Both domestic and international contributors are welcome. Manuscripts written in Chinese or English will be accepted. Additional English titles, abstracts and key words should be included in Chinese manuscripts. All manuscripts are subject to critical review by the editorial committee, which is composed of about 10 foreign and 50 Chinese experts in fuel science. Journal of Fuel Chemistry and Technology has been a source of primary research work in fuel chemistry as a Chinese core scientific periodical.