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Host-Guest Interactions and Their Catalytic Consequences in Methanol to Olefins Conversion on Zeolites Studied by C-13-Al-27 Double-Resonance Solid-State NMR Spectroscopy

文献类型：期刊论文

作者Liu, Xiaolong2; Wang, Qiang2; Zhou, Xue2; Qi, Guodong2; Feng, Ningdong2; Xu, Jun2; Meng, Xiangju1; Xiao, Fengshou1; Deng, Feng2; Wang, Chao2
刊名ACS CATALYSIS
出版日期2017-09-01
卷号7期号:9页码:6094-6103
关键词Methanol Conversion Zeolites Mechanism Host-guest Interaction Nmr Spectroscopy
DOI10.1021/acscatal.7b01738
文献子类Article
英文摘要Methanol conversion over zeolites with different topologies (H-ZSM-5, H-SSZ-13, and H-MOR) was studied using solid-state NMR spectroscopy and gas chromatrography mass spectroscopy (GC-MS). Host guest interactions between active hydrocarbon pool (HP) species and zeolite framework (Bronsted acid/base site) were observed, and the supramolecular reaction centers (SMCs) generated by the interactions were unambiguously identified by C-13-Al-37 double-resonance NMR The internuclear spatial interaction/proximity between the C-13 nuclei (associated with HP species) and the Al-27 nuclei (associated with Bronsted acid/base site) was analyzed and compared over the three zeolites. The product shape selectivity of zeolites greatly influences the catalytic performance that can be linked to the nature of HP species and the host guest interactions. Closer spatial proximity and stronger interaction between methylbenzenes (MBs) and Bronsted acid/base sites were observed over H-SSZ-13 and H-MOR zeolites, which facilitate aromatic-based reaction routes and rationalize the higher selectivity to ethene on the two catalysts. This leads to rapid deactivation at high temperature due to coke deposition on the active sites caused by the evolution of active MBs. For H-ZSM-5, the lesser amount of retained MBs and their weaker interactions with the active sites at high temperature cause the aromatic-based reactions to be insignificant and lead to the prevalence of alkene-based and carbocation-involved reactions, which are responsible for the high resistance of H-ZSM-5 to deactivation. In contrast, at lower temperature, the aromatic-based reaction route is favored with the MBs-composed SMCs prevailing. The distribution of the carbonaceous species in deactivated catalysts was revealed by host guest interactions.
WOS关键词TO-HYDROCARBONS REACTION ; PRODUCT SELECTIVITY ; COKE FORMATION ; AROMATIC-HYDROCARBONS ; REACTION-MECHANISM ; SHAPE-SELECTIVITY ; REACTION CENTERS ; MTH REACTION ; H-BETA ; H-ZSM-5
WOS研究方向Chemistry
语种英语
WOS记录号WOS:000410005700060
资助机构National Natural Science Foundation of China(21622311 ; National Natural Science Foundation of China(21622311 ; key program for frontier science of the Chinese Academy of Science(QYZDB-SSW-SLH027) ; key program for frontier science of the Chinese Academy of Science(QYZDB-SSW-SLH027) ; 21473245 ; 21473245 ; 21603265 ; 21603265 ; 21210005) ; 21210005) ; National Natural Science Foundation of China(21622311 ; National Natural Science Foundation of China(21622311 ; key program for frontier science of the Chinese Academy of Science(QYZDB-SSW-SLH027) ; key program for frontier science of the Chinese Academy of Science(QYZDB-SSW-SLH027) ; 21473245 ; 21473245 ; 21603265 ; 21603265 ; 21210005) ; 21210005)
源URL[http://ir.wipm.ac.cn/handle/112942/11405]  
专题武汉物理与数学研究所_磁共振应用研究部
作者单位1.Zhejiang Univ, Dept Chem, Hangzhou 310028, Zhejiang, Peoples R China
2.Chinese Acad Sci, State Key Lab Magnet Resonance & Atom & Mol Phys, Natl Ctr Magnet Resonance Wuhan, Wuhan Inst Phys & Math, Wuhan 430071, Hubei, Peoples R China
推荐引用方式
GB/T 7714		 Liu, Xiaolong,Wang, Qiang,Zhou, Xue,et al. Host-Guest Interactions and Their Catalytic Consequences in Methanol to Olefins Conversion on Zeolites Studied by C-13-Al-27 Double-Resonance Solid-State NMR Spectroscopy[J]. ACS CATALYSIS,2017,7(9):6094-6103.
APA Liu, Xiaolong.,Wang, Qiang.,Zhou, Xue.,Qi, Guodong.,Feng, Ningdong.,...&Wang, Chao.(2017).Host-Guest Interactions and Their Catalytic Consequences in Methanol to Olefins Conversion on Zeolites Studied by C-13-Al-27 Double-Resonance Solid-State NMR Spectroscopy.ACS CATALYSIS,7(9),6094-6103.
MLA Liu, Xiaolong,et al."Host-Guest Interactions and Their Catalytic Consequences in Methanol to Olefins Conversion on Zeolites Studied by C-13-Al-27 Double-Resonance Solid-State NMR Spectroscopy".ACS CATALYSIS 7.9(2017):6094-6103.

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来源：武汉物理与数学研究所

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