日用化学工业(中英文)2025,Vol.55Issue(9):1100-1111,12.DOI:10.3969/j.issn.2097-2806.2025.09.003
Al2O3性质诱导Cu-Al体系催化草酸二乙酯加氢合成醇醚酯
The synthesis of alcohol ether esters through the catalytic hydrogenation of diethyl oxalate in the Cu-Al systems induced by Al2O3 properties
摘要
Abstract
The structure-performance relationship of Cu/Al2O3 catalysts in the hydrogenation of diethyl oxalate(DEO)for the synthesis of alcohol ether esters has been investigated by various characterization techniques including XRD,XPS,N2O titration,and 27Al MAS-NMR.The results showed that when the crystal configurations of Al2O3 were the same,increasing the specific surface area could effectively refine the size of copper nanoparticles(Cu NPs),and ultimately improve the conversion of DEO.Meanwhile,the smaller size of γ-Al2O3(HSAl and SBAl)loaded Cu NPs promotes the reaction towards the deep hydrogenation to produce ethanol(EtOH)and ethylene glycol(EG).Besides,the larger size of Cu NPs on the surface of amorphous Al2O3(HTAl and SolAl)resulted in a lower conversion rate,where ethyl glycolate(Egly)is the main product.Despite there are differences in Al3+ionic coordination in Al2O3 with different crystal structures,the experimental data showed that the differences in Al3+ionic coordination did not significantly affect the catalytic performance in the hydrogenation reaction.The formation of alcohol-ether ester chemicals is critically dependent on the interactions between Cu sites and acidic sites.Among them,EG and EtOH were dehydrated to form 2-ethoxyethanol via the SN2 mechanism,while Egly and EtOH were reacted to form ethyl ethoxyacetate(EEA)via the SN2 mechanism.This study provides a theoretical basis for the optimization of the coal-based glycol processes to achieve a diversified product portfolio.关键词
草酸酯加氢/醇醚酯/Cu-Al催化剂/SN2机制Key words
oxalate hydrogenation/alcohol ether esters/Cu-Al catalyst/SN2 mechanism分类
化学化工引用本文复制引用
武鹏,马丽娜,郑昱,罗莉,苏立红,栗俊田..Al2O3性质诱导Cu-Al体系催化草酸二乙酯加氢合成醇醚酯[J].日用化学工业(中英文),2025,55(9):1100-1111,12.基金项目
山西省基础研究计划(202403021212047) (202403021212047)
山西省高等学校科技创新项目(2024L402 ()
2024L405 ()
2023L397) ()