Comparative catalytic study on butene/isobutane alkylation over LaX and CeX zeolites: The influence of calcination atmosphere
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Comparative catalytic study on butene/isobutane alkylation over LaX and CeX zeolites: The influence of calcination atmosphere
Chinese Journal of Chemical EngineeringVol. 46, Issue 6, Pages: 173-183(2022)
Affiliations:
1. School of Chemical Engineering & Technology, Tianjin University,Tianjin,China,300072
2. Beijing Key Laboratory of Ionic Liquids Clean Process, State Key Laboratory of Multiphase Complex Systems, CAS Key Laboratory of Green Process and Engineering, Institute of Process Engineering, Chinese Academy of Sciences,Beijing,China,100049
3. School of Chemical Engineering, University of Chinese Academy of Sciences,Beijing,China,100049
Author bio:
Funds:
DOI:
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Published:2022
Accepted:
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Zhiqiang Yang, Ruirui Zhang, Honghua Zhang, Hongguo Tang, Ruixia Liu, Suojiang Zhang. 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(6): 173-183.
DOI:
Zhiqiang Yang, Ruirui Zhang, Honghua Zhang, Hongguo Tang, Ruixia Liu, Suojiang Zhang. 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(6): 173-183.DOI:
Comparative catalytic study on butene/isobutane alkylation over LaX and CeX zeolites: The influence of calcination atmosphere
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 i s 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 Brønsted 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 Brønsted acid concentration. In addition
Ce
3+
was found more benefit for the hydride transfer compared with La
3+
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 propos
ed in isobutane alkylation.
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