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Cooperativity of adjacent Bronsted acid sites in MFI zeolite channel leads to enhanced polarization and cracking of alkanes

文献类型：期刊论文

作者Guo, Xuefeng2,3; Peng, Luming2,3; Xue, Nianhua2,3; Shen, Jianyi2,3; Yang, Weimin1; Ding, Weiping2,3; Zhao, Li2,3; Shi, Hui5; Song, Chenhai2,3; Chu, Yueying4
刊名JOURNAL OF CATALYSIS
出版日期2017-05-01
卷号349页码:163-174
关键词Cooperative Catalysis Adjacent Bronsted Acid Sites Alkane Adsorption Alkane Cracking Hzsm-5 Solid-state Mas Nmr
DOI10.1016/j.jcat.2016.12.024
文献子类Article
英文摘要The spatial proximity between Bronsted acid sites (BAS) in HZSM-5 zeolites is demonstrated by H-1 double quantum (DO) MAS NMR measurements. This proximity results in more pronounced polarization of adsorbed acetone and alkanes in zeolites, evident from C-13 MAS NMR spectra. The adjacent BAS with synergistic interactions on alkane reactants (propane, n-butane, and n-pentane) cooperatively catalyze alkane cracking at higher turnover rates than on isolated BAS. Apparent activation energies are similar on HZSM-5 catalysts with different concentrations of isolated and adjacent BAS, while apparent activation entropies become less negative at higher BAS concentrations. Kinetic experiments in conjunction with adsorption measurement and DFT calculations prove that cracking rates at these Al-site pairs are mainly due to more positive intrinsic activation entropies, suggesting that the protonation transition state occurs later along the reaction coordinate on adjacent BAS. Adjacent Bronsted acid sites favor cracking over dehydrogenation and favor central cracking over terminal cracking. (C) 2017 Elsevier Inc. All rights reserved.
WOS关键词SOLID-STATE NMR ; DIFFUSE-REFLECTANCE SPECTROSCOPY ; PENTASIL-CONTAINING ZEOLITES ; CO2+ ION SITES ; TO-OLEFINS CONVERSION ; MONOMOLECULAR CRACKING ; AL DISTRIBUTION ; THEORETICAL CALCULATION ; ALUMINUM DISTRIBUTION ; PROBE MOLECULES
WOS研究方向Chemistry ; Engineering
语种英语
WOS记录号WOS:000401217600017
资助机构Natural Science Foundation of China(21103087 ; Natural Science Foundation of China(21103087 ; Natural Science Foundation of Jiangsu Province, China(BK20151380) ; Natural Science Foundation of Jiangsu Province, China(BK20151380) ; Shanghai Research Institute of Petrochemical Technology, Sinopec ; Shanghai Research Institute of Petrochemical Technology, Sinopec ; China Scholarship Council ; China Scholarship Council ; 21273107 ; 21273107 ; 21222302) ; 21222302) ; Natural Science Foundation of China(21103087 ; Natural Science Foundation of China(21103087 ; Natural Science Foundation of Jiangsu Province, China(BK20151380) ; Natural Science Foundation of Jiangsu Province, China(BK20151380) ; Shanghai Research Institute of Petrochemical Technology, Sinopec ; Shanghai Research Institute of Petrochemical Technology, Sinopec ; China Scholarship Council ; China Scholarship Council ; 21273107 ; 21273107 ; 21222302) ; 21222302)
源URL[http://ir.wipm.ac.cn/handle/112942/11305]  
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.Sinopec, Shanghai Res Inst Petrochem Technol, Shanghai 201208, Peoples R China
2.Nanjing Univ, Sch Chem & Chem Engn, Minist Educ, Key Lab Mesoscop Chem, Nanjing 210093, Jiangsu, Peoples R China
3.Nanjing Univ, Sch Chem & Chem Engn, Collaborat Innovat Ctr Chem Life Sci, Nanjing 210093, Jiangsu, Peoples R China
4.Chinese Acad Sci, Wuhan Inst Phys & Math, Wuhan Ctr Magnet Resonance, State Key Lab Magnet Resonance & Atom & Mol Phys, Wuhan 430071, Peoples R China
5.Pacific Northwest Natl Lab, Inst Integrated Catalysis, 902 Battelle Blvd, Richland, WA 99352 USA
推荐引用方式
GB/T 7714		 Guo, Xuefeng,Peng, Luming,Xue, Nianhua,et al. Cooperativity of adjacent Bronsted acid sites in MFI zeolite channel leads to enhanced polarization and cracking of alkanes[J]. JOURNAL OF CATALYSIS,2017,349:163-174.
APA Guo, Xuefeng.,Peng, Luming.,Xue, Nianhua.,Shen, Jianyi.,Yang, Weimin.,...&Wang, Meng.(2017).Cooperativity of adjacent Bronsted acid sites in MFI zeolite channel leads to enhanced polarization and cracking of alkanes.JOURNAL OF CATALYSIS,349,163-174.
MLA Guo, Xuefeng,et al."Cooperativity of adjacent Bronsted acid sites in MFI zeolite channel leads to enhanced polarization and cracking of alkanes".JOURNAL OF CATALYSIS 349(2017):163-174.

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来源：武汉物理与数学研究所

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