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 m2/g.The sample(0.28Pd/S-1-H)derived after reduction at 500℃in 10 vol％H2 showed the best catalytic activity for toluene combustion(T50％=180℃and T90％=189℃at a space velocity of 40,000 mL/(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 kJ/mol)obtained over the best-performing 0.28Pd/S-1-H sample being much lower than those(51-70 kJ/mol)obtained over the other samples(0.28Pd/S-1-A derived from calcination at 500℃in air,0.26Pd/S-1-im de-rived from the impregnation route,and 0.27Pd/ZSM-5-H prepared after reduction at 500℃in 10 vol％H2).Furthermore,the 0.28Pd/S-1-H sample possessed good thermal stability and its partial deactivation due to CO2 or H2O introduction was reversible,but SO2 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,benzalde-hyde → 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 Pd0 species were responsible for the good catalytic performance of 0.28Pd/S-1-H.

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 Control,Key Laboratory of Advanced Functional Materials,Education Ministry of China,Laboratory of Catalysis Chemistry and Nanoscience,Department of Environmental Chemical Engineering,School of Environmental and Chemical Engineering,Faculty of Environment and Life,Beijing University of Technology,Beijing 100124,China

环境科学学报（英文版）

[1]Linke Wu;Jiguang Deng;Yuxi Liu;Lin Jing;Xiaohui Yu;Xing Zhang;Ruyi Gao;Wenbo Pei;Xiuqing Hao;Ali Rastegarpanah;Hongxing Dai-.Pd/silicalite-1:An highly active catalyst for the oxidative removal of toluene)[J].环境科学学报（英文版）,2022(06):209-219

28Pd,TOFPd,26Pd,27Pd,methylbenzoquinone,benzalde

silicalite,An,highly,active,oxidative,removal,toluene,Catalytic,combustion,thought,efficient,economic,remove,volatile,organic,compounds,its,critical,issue,development,performance,catalytic,materials,In,this,work,used,situ,synthesis,method,supported,nanoparticles,NPs,It,found,that,prepared,catalysts,displayed,hexagonal,prism,morphology,surface,area,derived,after,reduction,showed,best,activity,T50,T90,space,velocity,hr,turnover,frequency,sec,specific,reaction,rate,gpd,apparent,energy,kJ,obtained,performing,being,much,lower,than,those,other,samples,from,calcination,air,impregnation,route,ZSM,Furthermore,possessed,good,thermal,stability,partial,deactivation,due,H2O,introduction,was,but,SO2,addition,resulted,irreversible,possible,pathways,oxidation,maleic,anhydride,benzoic,hyde,carbon,dioxide,water,We,conclude,dispersion,adsorption,oxygen,species,concentration,large,capacity,strong,acidity,Pd0,were,responsible

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