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Comparative catalytic study on butene/isobutane alkylation over LaX and CeX zeolites: The influence of calcination atmosphere | |
Yang, Zhiqiang1,2; Zhang, Ruirui2; Zhang, Honghua2; Tang, Hongguo2; Liu, Ruixia2,3; Zhang, Suojiang1,2,3 | |
2022-06-01 | |
Source Publication | CHINESE JOURNAL OF CHEMICAL ENGINEERING
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ISSN | 1004-9541 |
Volume | 46Pages:173-183 |
Abstract | Lanthanum-containing (LaX) and cerium-containing X zeolites (CeX) were prepared by a double-exchange, double-calcination method. By changing the calcination atmospheres between nitrogen and air, the Ce-IV contents in CeX zeolites were adjusted and their impacts on physicochemical properties and catalytic performance in isobutane alkylation were established. The crystallinity of CeX zeolite was found to be negatively correlated with the Ce-IV content. This is believed to be due to the water formed during the oxidation of Ce-III, which facilitates the framework dealumination. As a consequence, calcining in air resulted in a great elimination of strong Bronsted acid sites while under nitrogen protection, this phenomenon was mostly hindered and the sample's acidity was preserved. When tested in a continuously flowed slurry reactor, the catalyst lifetime for isobutane alkylation was found to be linearly related to the strong Bronsted acid concentration. In addition, Ce3+ was found more benefit for the hydride transfer compared with La3+, which is ascribed to the stronger polarization effect on the CH bond of isobutane. Moreover, the decline of hydride transfer activity can be slowed down by the catalytic cracking of the bulky molecules. Based on the product distribution, a new catalytic cycle of dimethylhexanes (DMHs) involving a direct formation of isobutene rather than tert-butyl carbocation was proposed in isobutane alkylation. (C) 2021 Chemical Industry and Engineering Society of China (CIESC) and Chemical Industry Press (CIP) Published by Elsevier B.V. All rights reserved. |
Keyword | CeX zeolite Calcination atmosphere Isobutane alkylation Bronsted acid Hydride transfer |
DOI | 10.1016/j.cjche.2021.05.041 |
Language | 英语 |
WOS Keyword | ISOBUTANE 2-BUTENE ALKYLATION ; H-EMT ; HYDRIDE TRANSFER ; ION-EXCHANGE ; ACIDITY ; LOCATION ; CATIONS ; CERIUM ; SITES |
Funding Project | National Key Research and Development Program of China[2017YFA0206803] ; National Natural Science Foundation of China[21878315] ; Key Programs of the Chinese Academy of Sciences[KFZD-SW-413] ; Key Programs of Innovation Academy for Green Manufacture, CAS[IAGM2020C17] ; K. C. Wong Education Foundation[GJTD2018-04] ; Major Program of National Natural Science Foundation of China[21890762] |
WOS Research Area | Engineering |
WOS Subject | Engineering, Chemical |
Funding Organization | National Key Research and Development Program of China ; National Natural Science Foundation of China ; Key Programs of the Chinese Academy of Sciences ; Key Programs of Innovation Academy for Green Manufacture, CAS ; K. C. Wong Education Foundation ; Major Program of National Natural Science Foundation of China |
WOS ID | WOS:000806832500005 |
Publisher | CHEMICAL INDUSTRY PRESS CO LTD |
Citation statistics | |
Document Type | 期刊论文 |
Identifier | http://ir.ipe.ac.cn/handle/122111/53734 |
Collection | 中国科学院过程工程研究所 |
Corresponding Author | Liu, Ruixia; Zhang, Suojiang |
Affiliation | 1.Tianjin Univ, Sch Chem Engn & Technol, Tianjin 300072, Peoples R China 2.Chinese Acad Sci, CAS Key Lab Green Proc & Engn, State Key Lab Multiphase Complex Syst, Beijing Key Lab Ionic Liquids Clean Proc,Inst Pro, Beijing 100049, Peoples R China 3.Univ Chinese Acad Sci, Sch Chem Engn, Beijing 100049, Peoples R China |
Recommended Citation GB/T 7714 | Yang, Zhiqiang,Zhang, Ruirui,Zhang, Honghua,et al. Comparative catalytic study on butene/isobutane alkylation over LaX and CeX zeolites: The influence of calcination atmosphere[J]. CHINESE JOURNAL OF CHEMICAL ENGINEERING,2022,46:173-183. |
APA | Yang, Zhiqiang,Zhang, Ruirui,Zhang, Honghua,Tang, Hongguo,Liu, Ruixia,&Zhang, Suojiang.(2022).Comparative catalytic study on butene/isobutane alkylation over LaX and CeX zeolites: The influence of calcination atmosphere.CHINESE JOURNAL OF CHEMICAL ENGINEERING,46,173-183. |
MLA | Yang, Zhiqiang,et al."Comparative catalytic study on butene/isobutane alkylation over LaX and CeX zeolites: The influence of calcination atmosphere".CHINESE JOURNAL OF CHEMICAL ENGINEERING 46(2022):173-183. |
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