二甲醚羰基化丝光沸石成型催化剂黏结剂的研究

黄守莹; 熊雄; 贺培; 王建豪; 李媖; 刘宏开; 吕静; 马新宾

doi:10.11949/0438-1157.20200609

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二甲醚羰基化丝光沸石成型催化剂黏结剂的研究

催化、动力学与反应器 | 更新时间：2025-11-25

- 二甲醚羰基化丝光沸石成型催化剂黏结剂的研究
- Study on binder of extruded mordenite catalyst for dimethyl ether carbonylation
- 化工学报 2020年71卷第10期页码：4642-4651
- 作者机构：
  
  天津大学化工学院，绿色合成与转化教育部重点实验室，天津化学化工协同创新中心，天津 300072
- 作者简介：
  
  黄守莹（1985—），女，博士，副教授，huangsy@tju.edu.cn
  马新宾（1968—），男，博士，教授，xbma@tju.edu.cn
- 基金信息：
  
  国家自然科学基金项目(21978209;21325626)
- DOI：10.11949/0438-1157.20200609
  中图分类号： TQ203.2
- 收稿：2020-05-18，
  
  修回：2020-07-15，
  
  纸质出版：2020-10-05
- 稿件说明：
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黄守莹, 熊雄, 贺培, 王建豪, 李媖, 刘宏开, 吕静, 马新宾. 二甲醚羰基化丝光沸石成型催化剂黏结剂的研究[J]. 化工学报, 2020, 71(10): 4642-4651

HUANG Shouying, XIONG Xiong, HE Pei, WANG Jianhao, LI Ying, LIU Hongkai, LYU Jing, MA Xinbin. Study on binder of extruded mordenite catalyst for dimethyl ether carbonylation[J]. CIESC Journal, 2020, 71(10): 4642-4651
黄守莹, 熊雄, 贺培, 王建豪, 李媖, 刘宏开, 吕静, 马新宾. 二甲醚羰基化丝光沸石成型催化剂黏结剂的研究[J]. 化工学报, 2020, 71(10): 4642-4651 DOI： 10.11949/0438-1157.20200609.

HUANG Shouying, XIONG Xiong, HE Pei, WANG Jianhao, LI Ying, LIU Hongkai, LYU Jing, MA Xinbin. Study on binder of extruded mordenite catalyst for dimethyl ether carbonylation[J]. CIESC Journal, 2020, 71(10): 4642-4651 DOI： 10.11949/0438-1157.20200609.

摘要

二甲醚（DME）羰基化制乙酸甲酯（MA），MA加氢合成乙醇工艺是一种新颖、绿色且经济的乙醇合成路线，催化剂成型对实现该工艺工业化具有重要意义。本论文选用拟薄水铝石及硅溶胶为黏结剂，对丝光沸石分子筛（MOR）进行挤条成型，制备了一系列不同黏结剂种类与含量的成型MOR催化剂。通过强度测试以及Weibull函数统计分析，探究了黏结剂对成型MOR的强度以及强度可靠性的影响；X射线衍射、N

物理吸附、NH

程序升温脱附、吡啶吸附原位红外等表征结合活性评价，探究了黏结剂对MOR的物理结构、酸性以及催化性能的作用。结果表明：黏结剂的引入不会影响MOR的晶体结构，且以拟薄水铝石为黏结剂时，催化剂力学性能及DME羰基化催化性能最佳。通过建立MA时空收率、TOF与微孔比表面积之间的定量关系，确定黏结剂不影响MOR内单位活性位点催化能力，产物时空收率与催化剂微孔比表面积呈线性正相关。

Abstract

The carbonylation of dimethyl ether (DME) to produce methyl acetate (MA) and the hydrogenation of MA to ethanol is a novel

green and economical ethanol synthesis route. The formation of the catalyst is of great significance to the industrialization of this process. In this paper

pseudo-boehmite and silica sol are used as binders

and mordenite molecular sieve (MOR) is extruded to prepare a series of molded MOR catalysts with different binder types and contents. By using strength evaluation and Weibull distribution analysis

we investigated the mechanical stability and reliability of the extruded MOR. Afterwards

XRD

-physisorption

-TPD and IR spectra of pyridine adsorption were employed to explore the influence of binder on textural properties

acidity and catalytic performance. The results showed that the crystal structure of MOR was maintained after addition of binder. When the pseudo-boehmite was used as a binder

the catalyst showed the best mechanical property and catalytic activity. By establishing the quantitative relationships among the yield

TOF and structure parameter

it is found that the space time yield of MA was linearly related to the specific surface area of micropores. Meanwhile

the almost constant TOF indicated that the binders did not affect the catalytic capacity of each activesites in MOR for carbonylation of dimethyl ether.

关键词

Keywords

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