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Direct amination of isobutylene over zeolite catalysts with various topologies and acidities
Gao, Shangyao1,2; Zhu, Xiangxue1; Li, Xiujie1; Wang, Yuzhong1; Xie, Sujuan1; Du, Songwei3; Chen, Fucun1; Zeng, Peng4; Liu, Shenglin1; Xu, Longya1
关键词Isobutylene Amination Tert-butylamine Zeolite Catalysts Zsm-5
刊名JOURNAL OF ENERGY CHEMISTRY
2017-07-01
DOI10.1016/j.jechem.2017.03.018
26期:4页:776-782
收录类别SCI
文章类型Article
WOS标题词Science & Technology ; Physical Sciences ; Technology
类目[WOS]Chemistry, Applied ; Chemistry, Physical ; Energy & Fuels ; Engineering, Chemical
研究领域[WOS]Chemistry ; Energy & Fuels ; Engineering
关键词[WOS]TERT-BUTYLAMINE ; MOLECULAR-SIEVES ; ALKENES ; CRACKING ; SITES ; TRANSFORMATION ; HYDROCARBONS ; CONVERSION ; ISOBUTENE ; ALKYNES
英文摘要The atomically economic and green chemical reaction of direct amination of isobutylene to tertbutylamine, particularly under the relative mild reaction conditions available for future industrial use, was carried out over zeolite catalysts possessing different topological structures, from one dimensional to three dimensional pore system, and from small 8-member ring pore (MRP) to medium 10 MRP and further to large 12 MRP zeolites, to disclose the relationship between the zeolite properties/topologies and their amination performance systematically under the mild reaction conditions. It was discovered that the pore structure and the acidities of zeolite catalysts played crucial roles in the isobutylene amination process, and suitable pore diameter (larger than 0.5 nm or with large side pockets/cups in the outside surface) and a certain number of mid-strong acid sites are indispensable to catalyze the amination reaction, while too strong acid strength was not conducive to the process of isobutylene amination. Among them, zeolites with topologies of BEA, MFI, MEL, MWW and EUO exhibited good amination performance, with which the isobutylene conversion was higher than 12.61% (> 46.42% of the equilibrium conversion) under the studied mild reaction conditions. Due to the good amination performance and the large adjustable Si/Al-2 ratio range, ZSM-5 was selected to further study the effect of acidity on the amination performance systematically under the mild reaction conditions, and the activity-acidity relationship in the amination process was disclosed: the amination activity (isobutylene conversion) had a linear correlation with the amount of mid-strong B acidity under the studied conditions over ZSM-5 catalyst, which can provide guidance for further developing high-efficient amination catalyst under mild reaction conditions available for future industrial use. (C) 2017 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights reserved.
语种英语
WOS记录号WOS:000412776100027
引用统计
文献类型期刊论文
条目标识符http://cas-ir.dicp.ac.cn/handle/321008/150098
专题中国科学院大连化学物理研究所
作者单位1.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian 116023, Liaoning, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
3.PetroChina Jinzhou Petrochem Co, Jinzhou 121001, Liaoning, Peoples R China
4.China Huanqiu Contracting & Engn Corp, Fushun 113006, Liaoning, Peoples R China
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GB/T 7714
Gao, Shangyao,Zhu, Xiangxue,Li, Xiujie,et al. Direct amination of isobutylene over zeolite catalysts with various topologies and acidities[J]. JOURNAL OF ENERGY CHEMISTRY,2017,26(4):776-782.
APA Gao, Shangyao.,Zhu, Xiangxue.,Li, Xiujie.,Wang, Yuzhong.,Xie, Sujuan.,...&Xu, Longya.(2017).Direct amination of isobutylene over zeolite catalysts with various topologies and acidities.JOURNAL OF ENERGY CHEMISTRY,26(4),776-782.
MLA Gao, Shangyao,et al."Direct amination of isobutylene over zeolite catalysts with various topologies and acidities".JOURNAL OF ENERGY CHEMISTRY 26.4(2017):776-782.
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