具有缺陷结构的UiO-66-SO3H-X催化CO2和CH3OH合成DMC研究

张奥森; 张忠琪; 沈英杰; 王培贤; 王自庆; 王贺云; 熊新阳; 田芳芳

doi:10.12434/j.issn.2097-2547.20240263

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具有缺陷结构的UiO-66-SO₃H-X催化CO₂和CH₃OH合成DMC研究

- 具有缺陷结构的UiO-66-SO₃H-X催化CO₂和CH₃OH合成DMC研究
- Study on catalytic performances of UiO-66-SO₃H-X with defective structure for synthesis of DMC from CO₂ and CH₃OH
- 低碳化学与化工 2025: 1-11.
- 作者机构：
  
  1.石河子大学化学化工学院，新疆石河子 832003
  2.新疆天业（集团）有限公司，新疆石河子 832003
- 作者简介：
  
  张奥森（1998—），硕士研究生，研究方向金属有机框架材料开发及催化性能，E-mail：1206443868@qq.com。
  王贺云（1975—），博士，教授，研究方向功能高分子材料，E-mail：whyun@shzu.edu.cn。
- 基金信息：
  
  兵团指导性计划项目(2023ZD072;2023ZD074)
- DOI：10.12434/j.issn.2097-2547.20240263
  中图分类号： TQ225.52
- 网络出版日期：2025-01-09，
  
  收稿日期：2024-06-15，
  
  修回日期：2024-07-23，
- 稿件说明：
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张奥森,张忠琪,沈英杰等.具有缺陷结构的UiO-66-SO₃H-X催化CO₂和CH₃OH合成DMC研究[J].低碳化学与化工,

ZHANG Aosen,ZHANG Zhongqi,SHEN Yingjie,et al.Study on catalytic performances of UiO-66-SO₃H-X with defective structure for synthesis of DMC from CO₂ and CH₃OH[J].Low-carbon Chemistry and Chemical Engineering,
张奥森,张忠琪,沈英杰等.具有缺陷结构的UiO-66-SO₃H-X催化CO₂和CH₃OH合成DMC研究[J].低碳化学与化工, DOI：10.12434/j.issn.2097-2547.20240263.

ZHANG Aosen,ZHANG Zhongqi,SHEN Yingjie,et al.Study on catalytic performances of UiO-66-SO₃H-X with defective structure for synthesis of DMC from CO₂ and CH₃OH[J].Low-carbon Chemistry and Chemical Engineering, DOI：10.12434/j.issn.2097-2547.20240263.

摘要

大量排放造成全球变暖引起了广泛关注，如何减少CO

排放并将其转化为高附加值化学品已成为研究热点。以2-巯基苯甲酸（MBA）和对苯二甲酸（H

BDC）作为配体，合成了一系列UiO-66-SH-X，然后利用H

氧化制备了UiO-66-SO

H-X（X =

(MBA):(

BDC) +

(MBA))）催化剂。研究了X对UiO-66-SO

H-X催化剂物理化学性质、催化性能和重复使用性的影响。结果表明，UiO-66-SO

H-X具有良好的晶体结构，随着X增大，UiO-66-SO

H-X比表面积和平均孔径迅速减小。与UiO-66相比，UiO-66-SO

H-X催化性能更优，其中UiO-66-SO

H-0.3催化性能最优。在温度140 ℃、CO

压力3.5 MPa和反应时间8 h条件下，DMC收率为0.92%，较UiO-66提高2.83倍。UiO-66-SO

H-0.3具有良好的水热稳定性，经过3次循环测试后，活性比为92.6%。

Abstract

The global warming caused by large amount of CO

emissions has attracted wide attention. How to reduce CO

emissions and transform them into high value-added chemicals has become a research hotspot. A series of UiO-66-SH-X were synthesized using 2-mercaptobenzoic acid (MBA) and terylene acid (H

BDC) as ligands

and then UiO-66-SO

H-X catalysts (X =

(MBA):(

BDC) +

(MBA)) ) were prepared by H

oxidation. The effects of X on the physical and chemical properties

catalytic performance and reusability of UiO-66-SO

H-X were studied. The results show that UiO-66-SO

H-X has great crystal structure. The

specific surface area and average pore size of UiO-66-SO

H-X decrease rapidly with the increase of X. Compared with UiO-66

UiO-66-SO

H-X has better catalytic performance and UiO-66-SO

H-0.3 shows the best catalytic performance. Under the condition of temperature of 140 ℃

pressure of 3.5 MPa and reaction time of 8 h

the yield of DMC is 0.92%

which is 2.83 times higher than that of UiO-66. UiO-66-SO

H-0.3 has great hydrothermal stability

and the activity ratio can remain 92.6% after three catalytic reaction cycles.

关键词

CO2碳酸二甲酯UiO-66连接体缺陷酸性位点

Keywords

carbon dioxidedimethyl carbonateUiO-66linker defectacid site

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