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Pd/silicalite-1: An highly active catalyst for the oxidative removal of toluene

Journal of Environmental Sciences 2022年第6期34卷 209-219页

作者： Linke Wu Jiguang Deng Yuxi Liu Lin Jing Xiaohui Yu Xing Zhang Ruyi Gao Wenbo Pei Xiuqing Hao ali rastegarpanah Hongxing Dai Beijing Key Laboratory for Green Catalysis and Separation Key Laboratory of Beijing on Regional Air Pollution ControlKey Laboratory of Advanced Functional MaterialsEducation Ministry of ChinaLaboratory of Catalysis Chemistry and NanoscienceDepartment of Environmental Chemical EngineeringSchool of Environmental and Chemical EngineeringFaculty of Environment and LifeBeijing University of TechnologyBeijing 100124China

Catalytic combustion is thought as an efficient and economic pathway to remove volatile organic compounds, and its critical issue is the development of high-performance catalytic materials. In this work, we used the in situ synthesis method to prepare the silicalite-1(S-1)-supported Pd nanoparticles(NPs). It is found that the as-prepared catalysts displayed a hexagonal prism morphology and a surface area of 390-440 m^(2)/g. The sample(0.28Pd/S-1-H)derived after reduction at 500°C in 10 vol% H_(2)showed the best catalytic activity for toluene combustion(T50%= 180℃ and T90%= 189℃ at a space velocity of 40,000 m L/(g·hr), turnover frequency(TOFPd) at 160℃ = 3.46 × 10^(-3)sec^(-1), and specific reaction rate at 160℃ = 63.8μmol/(gPd·sec)), with the apparent activation energy(41 k J/mol) obtained over the bestperforming 0.28Pd/S-1-H sample being much lower than those(51-70 k J/mol) obtained over the other samples(0.28Pd/S-1-A derived from calcination at 500℃ in air, 0.26Pd/S-1-im derived from the impregnation route, and 0.27Pd/ZSM-5-H prepared after reduction at 500℃ in 10 vol% H_(2)). Furthermore, the 0.28Pd/S-1-H sample possessed good thermal stability and its partial deactivation due to CO_(2) or H_(2)O introduction was reversible, but SO_(2) addition resulted in an irreversible deactivation. The possible pathways of toluene oxidation over 0.28Pd/S-1-H was toluene → p-methylbenzoquinone → maleic anhydride, benzoic acid, benzaldehyde → carbon dioxide and water. We conclude that the good dispersion of Pd NPs, high adsorption oxygen species concentration, large toluene adsorption capacity, strong acidity,and more Pd~0 species were responsible for the good catalytic performance of 0.28Pd/S-1-H.

关键词： Silicalite-1 Hexagonal prism shape Supported palladium catalyst Volatile organic compound Toluene combustion

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Influence of Adapting P123-PMMA as Templates on Physicochemical Property and Activity of the Ordered Macroporous NiO/CuO Catalysts for CO Oxidation

Influence of Adapting P123-PMMA as Templates on Physicochemi...

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第二十五届大气污染防治技术研讨会

作者： ali rastegarpanah Yuxi Liu Jiguang Deng Lin Jing Hongxing Dai Beijing Key Laboratory for Green Catalysis and Separation Key Laboratory of Beijing on Regional Air Pollution Control Key Laboratory of Advanced Functional MaterialsEducation Ministry of China Laboratory of Catalysis Chemistry and NanoscienceDepartment of Chemistry and Chemical Engineering College of Environmental and Energy Engineering Beijing University of Technology

Most of CO emissions are mainly from the cold start of vehicles and domestic activities [1]. Recently,low-temperature catalytic carbon monoxide oxidation has gained increasing attention in converting toxic CO to harmless CO. Although the catalysts containing gold and platinum group metals(e.g.,Pt,Pd,and Ru [2]) show excellent catalytic performance for CO oxidation,their limited availability and high cost make utilization of these noble metals difficult in commercial requests. In recent years,the transition-metal oxides as heterogeneous catalysts have received more attention [3]. In this work,a series of highly ordered macroporous nickel-copper mixed oxides were prepared using the dual-templating [Pluronic P123 and poly(methyl methacrylate)(PMMA)] method in mixed solution of ethylene glycol and methanol when annealing at 550 οC. Compared to the fabricated samples via the citric acid complexation method as well as poly(methyl methacrylate)(PMMA) colloidal microspheres route,sample by adapting both P123 and PMMA exhibited a much higher catalytic activity for CO oxidation. Over this catalyst,at a carbon monoxide/oxygen volumetric ratio of 2/5 and a space velocity of 60,000 mL/(g h),CO could be completely oxidized lower than 140 °C. The high surface areas,more oxygen adspecies concentration,good low-temperature reducibility,and unique nanovoid structures concluded for its admirable performance.

关键词： Dual-templating method Nickel-copper mixed oxides Macroporous

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