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CLC number: TQ032.4

On-line Access: 2021-02-05

Received: 2020-03-31

Revision Accepted: 2020-07-12

Crosschecked: 2021-01-14

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Citations:  Bibtex RefMan EndNote GB/T7714


Bin-bo Jiang


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Journal of Zhejiang University SCIENCE A 2021 Vol.22 No.2 P.106-115


Modification of acidity in HZSM-5 zeolite for methane-methanol co-reaction

Author(s):  Bing-jie Zhou, Zhi-xiang Xi, Yue Yu, Bin-bo Jiang, Jing-dai Wang, Zu-wei Liao, Zheng-liang Huang, Yong-rong Yang

Affiliation(s):  Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology, Department of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, China; more

Corresponding email(s):   jiangbb@zju.edu.cn

Key Words:  Methane conversion, Methanol, Co-reaction, Acidity, HZSM-5

Bing-jie Zhou, Zhi-xiang Xi, Yue Yu, Bin-bo Jiang, Jing-dai Wang, Zu-wei Liao, Zheng-liang Huang, Yong-rong Yang. Modification of acidity in HZSM-5 zeolite for methane-methanol co-reaction[J]. Journal of Zhejiang University Science A, 2021, 22(2): 106-115.

@article{title="Modification of acidity in HZSM-5 zeolite for methane-methanol co-reaction",
author="Bing-jie Zhou, Zhi-xiang Xi, Yue Yu, Bin-bo Jiang, Jing-dai Wang, Zu-wei Liao, Zheng-liang Huang, Yong-rong Yang",
journal="Journal of Zhejiang University Science A",
publisher="Zhejiang University Press & Springer",

%0 Journal Article
%T Modification of acidity in HZSM-5 zeolite for methane-methanol co-reaction
%A Bing-jie Zhou
%A Zhi-xiang Xi
%A Yue Yu
%A Bin-bo Jiang
%A Jing-dai Wang
%A Zu-wei Liao
%A Zheng-liang Huang
%A Yong-rong Yang
%J Journal of Zhejiang University SCIENCE A
%V 22
%N 2
%P 106-115
%@ 1673-565X
%D 2021
%I Zhejiang University Press & Springer
%DOI 10.1631/jzus.A2000126

T1 - Modification of acidity in HZSM-5 zeolite for methane-methanol co-reaction
A1 - Bing-jie Zhou
A1 - Zhi-xiang Xi
A1 - Yue Yu
A1 - Bin-bo Jiang
A1 - Jing-dai Wang
A1 - Zu-wei Liao
A1 - Zheng-liang Huang
A1 - Yong-rong Yang
J0 - Journal of Zhejiang University Science A
VL - 22
IS - 2
SP - 106
EP - 115
%@ 1673-565X
Y1 - 2021
PB - Zhejiang University Press & Springer
ER -
DOI - 10.1631/jzus.A2000126

A co-reaction of methane with methanol over zeolite catalysts has emerged as a new approach to the long-standing challenge of methane transformation. However, the effect of catalyst acid properties on the co-reaction has been rarely studied. In this study, a series of HZSM-5 zeolites with comparable diffusion abilities and various acidities were synthesized directly through steaming with 100% water vapor at 693 K. The co-reaction of methane and methanol was subsequently evaluated. Brønsted acidity at 0.262 mmol/g was detected to reach the maximum methane conversion of 5.42% at 673 K, which was also the odd point in the relationship between acid concentration and C4 hydrogen transfer index. Moreover, the influence of methanol feed was investigated over parent and steamed ZSM-5 catalyst, with results showing that excessive acid sites or methanol molecules reduce methane conversion. It is proposed that acid sites adsorbed with methanol molecules construct the methane activation sites. Hence, a proper design of zeolite acidity should be achieved to obtain higher methane conversion in the co-reaction process.


创新点:1. 实现了低温下的甲烷活化;2. 通过水蒸气处理单因素调控HZSM-5催化剂的酸性;3. 提出了HZSM-5上甲烷与甲醇的共活化机制.
方法:1. 通过水蒸气处理,得到孔结构和扩散能力差异小而酸性差异显著的系列HZSM-5催化剂(图1-6);2. 通过催化剂性能考评,对比研究不同酸性HZSM-5上的甲醇反应以及甲烷甲醇耦合反应过程(图7);3. 在酸性不同的催化剂上研究甲醇空速对甲烷转化的影响(图9).
结论:1. 在HZSM-5催化剂上,存在最适酸浓度,可使甲烷转化率最高;2. 酸浓度更高的催化剂,其达到最大甲烷转化率所对应的甲醇空速更大;3. 吸附有甲醇分子的酸位点构成了耦合反应中甲烷的活化中心.


Darkslateblue:Affiliate; Royal Blue:Author; Turquoise:Article


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