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Effects of metal and acidic sites on the reaction by-products of butyl acetate oxidation over palladium-based catalysts
Authors:Lin Yue  Chi He  Zhengping Hao  Shunbing Wang and Hailin Wang
Institution:Department of Environmental Nano-materials, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China;Department of Environmental Nano-materials, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China;Department of Environmental Nano-materials, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China;The Administrative Center for China's Agenda 21, Beijing 100038, China;National Urban Environmental Pollution Control Engineering Techniques Research Center, Beijing Municipal Research Institute of Environmental Protection, Beijing 100037, China
Abstract:Catalytic oxidation is widely used in pollution control technology to remove volatile organic compounds. In this study, Pd/ZSM-5 catalysts with different Pd contents and acidic sites were prepared via the impregnation method. All the catalysts were characterized by means of N2 adsorption-desorption, X-ray fluorescence (XRF), H2 temperature programmed reduction (H2-TPR), and NH3 temperature programmed desorption (NH3-TPD). Their catalytic performance was investigated in the oxidation of butyl acetate experiments. The by-products of the reaction were collected in thermal desorption tubes and identified by gas chromatography/mass spectrometry. It was found that the increase of Pd content slightly changed the catalytic activity of butyl acetate oxidation according to the yield of CO2 achieved at 90%, but decreased the cracking by-products, whereas the enhancement of strong acidity over Pd-based catalysts enriched the by-product species. The butyl acetate oxidation process involves a series of reaction steps including protolysis, dehydrogenation, dehydration, cracking, and isomerization. Generally, butyl acetate was cracked to acetic acid and 2-methylpropene and the latter was an intermediate of the other by-products, and the oxidation routes of typical by-products were proposed. Trace amounts of 3-methylpentane, hexane, 2-methylpentane, pentane, and 2-methylbutane originated from isomerization and protolysis reactions.
Keywords:catalytic oxidation  butyl acetate  reaction by-product  Pd/ZSM-5  VOCs
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