低碳化学与化工2024，Vol.49Issue(6)：45-53,9.DOI:10.12434/j.issn.2097-2547.20230382
有序介孔二氧化硅负载Zn和Zr多功能催化剂催化乙醇转化制丁二烯性能研究
Study on catalytic performance of ordered mesoporous silica loaded Zn and Zr multifunctional catalysts for direct conversion of ethanol to butadiene
摘要
Abstract
Direct conversion of ethanol to butadiene is an effective strategy to reduce dependence on fossil resources and alleviate environmental problems.The development of novel catalysts can increase the production of butadiene.By adjusting the pore structure of mesoporous SiO2 materials,the rapid transfer of ethanol and important intermediates between the host and guest molecules can take place,and the adjustment of the acid-base properties and the synergistic effect of the active centers of catalysts can improve the catalytic performance of catalysts.A series of mesoporous SiO2 loaded Zn and Zr catalysts with different pore structures(ZnZr/SiO2,ZnZr/MCF,ZnZr/SBA-5 and ZnZr/KIT-6)were prepared by a wet impregnation method.The performances of catalysts for direct conversion of ethanol to butadiene were evaluated,and the synergistic effects of each active center of the catalysts and the influence of acid-base properties on the catalytic performance were revealed by various characterization techniques.The characterisation results show that the pore structure can effectively modulate the acid-base properties of the catalysts,and the mesostructured porous foam(MCF)can promote the interaction of Zn species with silanol to form strong Lewis acid sites.ZnZr/KIT-6 catalyst exhibits moderate acid properties because the interactions of Zr species with silanol on KIT-6 form moderate strength Lewis acid sites and KIT-6 inhibits the interaction of Zn species with silica hydroxyls to form strong acidic sites.In ZnZr/KIT-6 catalyst,Zn species mainly exist as ZnO,which is favourable for the dehydrogenation of ethanol to acetaldehyde.Compared to ZnZr/SBA-15 catalyst,ZnZr/KIT-6 catalyst has an increased amount of weak bases and a decreased amount of strong bases with a weaker base strength.Moderate acid and weak base properties are beneficial for the aldol condensation reaction in the direct conversion of ethanol to butadiene,so in the direct conversion of ethanol to butadiene reaction catalysed by ordered mesoporous SiO2 loaded Zn and Zr catalysts,ZnZr/KIT-6 catalyst shows the highest ethanol conversion rate and butadiene selectivity at a temperature of 350℃and a reaction space velocity of 1.23 h-1,which is 91.2%and 53.5%,respectively,and the butadiene space time yield is up to 0.35 g/(g·h).关键词
乙醇/丁二烯/介孔SiO2/ZnZr/KIT-6/羟醛缩合/酸碱性质Key words
ethanol/butadiene/mesoporous SiO2/ZnZr/KIT-6/aldol condensation/acid-base properties分类
化学化工引用本文复制引用
陈翀,李自琴,马盈月,王安,王康洲,高新华,张建利..有序介孔二氧化硅负载Zn和Zr多功能催化剂催化乙醇转化制丁二烯性能研究[J].低碳化学与化工,2024,49(6):45-53,9.基金项目
宁夏大学大学生创新创业训练计划 （）
国家自然科学基金(21968025). （21968025）
