Insights on copper,manganese,and Nickel/ZSM-5 catalytic mechanisms for nitric oxides selective reduction with ammonia

作     者：Cheng Liu Running Kang Feng Bin Xiaolin Wei Kwun Nam Hui Saravanan Kasipandi Kwan San Hui 

作者机构：State Key Laboratory of High-Temperature Gas DynamicsInstitute of MechanicsChinese Academy of SciencesBeijing 100190PR China School of Engineering ScienceUniversity of Chinese Academy of SciencesBeijing 100049PR China School of Automobile EngineeringWuhan University of TechnologyWuhan 430070PR China Department of Chemical and Metallurgical EngineeringSchool of Chemical EngineeringAalto UniversityKemistintie 1 P.O.Box 16100Espoo FI-00076Finland Institute of Applied Physics and Materials EngineeringUniversity of MacaoAvenida da UniversidadeTaipaMacaoPR China School of EngineeringFaculty of ScienceUniversity of East AngliaNorwich Research Park NR47TJUnited Kingdom 

出 版 物：《Carbon Resources Conversion》 (碳资源转化（英文）)

年 卷 期：2022年第5卷第1期

页      面：15-25页

核心收录：

学科分类：081704[工学-应用化学] 07[理学] 070304[理学-物理化学(含∶化学物理)] 08[工学] 0817[工学-化学工程与技术] 0703[理学-化学] 

基　　金：the support of National Nature Science Foundation of China(No.51736010) China Scholarship Council(No.202004910623) We sincerely thank Prof.Lv Gang(Tianjin University)for the reasonable suggestions about SCR reaction mechanism,and the Key Projects of Tianjin Natural Science Foundation(19JCZDJC40100) 

主　　题：Selective catalytic reduction Transition metals ZSM-5 Reaction mechanism Kinetics 

摘      要：The elucidation of the selective catalytic reduction mechanisms over state-of-the-art metal-promoted zeolites is essential for nitric oxides removal in automobile and stationary source *** this work,H/ZSM-5 catalysts modified with transition metals,including copper,manganese,and nickel,were prepared by using an incipient wetness impregnation method and were evaluated for the selective reduction of nitric oxides with *** indicate that copper/ZSM-5 exhibits the highest catalytic activity,with90%nitric oxide conversion at a broad operation temperature window(221–445◦C).The nitric oxide conversion profiles of nickel/ZSM-5 shows two peaks that correspond to weak activity among the catalysts;the low-temperature peak(290◦C)was induced by nickel clusters dispersed on the ZSM-5 surface,while the high-temperature peak(460◦C)was assigned to the bulk nickel *** size of granular nickel monoxide crystallites with an exposed(202)plane is 2–30 nm,as confirmed by Scanning electron microscopy,X-ray diffraction,and Transmission electron microscope ***-programmed reductions with hydrogen results testified that the copper and nickel cations,as the main species contributing to selective catalytic reduction,were reduced via Cu^(2+)/Cu^(+)→Cu^(0) and Ni^(2+)→Ni^(0) for copper/ZSM-5 and nickel/ZSM-5,respectively,while for the manganese/ZSM5,the Mn3+species in manganese clusters were reduced to Mn^(2+) by ***,temperatureprogrammed desorption coupled with mass spectrometer(TPD-MS)and in situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)were comprehensively used to reveal the relationship between zeolite structure and catalysts’properties for improving selective catalytic *** results confirm that the ammonia is adsorbed and activated on both Brønsted and Lewis acid *** nitrous oxide desorbs in two stages during nitric oxide-TPD-MS measurements,corresponding to the desorption of nitric