低碳化学与化工2025,Vol.50Issue(5):49-59,11.DOI:10.12434/j.issn.2097-2547.20240263
具有缺陷结构的UiO-66-SO3H-X催化CO2和CH3OH合成DMC研究
Study on synthesis of DMC from CO2 and CH3OH catalyzed by UiO-66-SO3H-X with defective structure
摘要
Abstract
The global warming caused by large amount of CO2 emissions has attracted wide attention.How to reduce CO2 emissions and transform it 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(H2BDC)as ligands,and then UiO-66-SO3H-X(X=n(MBA)∶(n(H2BDC)+n(MBA)))were prepared by H2O2 oxidation.The effects of n(MBA)∶(n(H2BDC)+n(MBA))on the physical and chemical properties,catalytic performance and reusability of UiO-66-SO3H-X were studied.The results show that UiO-66-SO3H-X has great crystal structure.The specific surface area and average pore size of UiO-66-SO3H-X decrease rapidly with the increase of n(MBA)∶(n(H2BDC)+n(MBA)).Compared with UiO-66,UiO-66-SO3H-X has better catalytic performance and UiO-66-SO3H-0.3 shows the best catalytic performance.Under the condition of temperature of 140 ℃,CO2 pressure of 3.5 MPa,catalyst dosage of 0.1 g 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-SO3H-0.3 has great hydrothermal stability,and the activity ratio(the ratio of DMC yield after three cycles to fresh catalyst DMC yield)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Key words
CO2/dimethyl carbonate/UiO-66/linker defect/acid site分类
化学工程引用本文复制引用
张奥森,张忠琪,沈英杰,王培贤,王自庆,王贺云,熊新阳,田芳芳..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,2025,50(5):49-59,11.基金项目
兵团指导性计划项目(2023ZD072,2023ZD074). (2023ZD072,2023ZD074)