低碳化学与化工2026,Vol.51Issue(4):59-69,11.DOI:10.12434/j.issn.2097-2547.20250174
形貌调控TiO2负载Cu催化剂对草酸二甲酯选择性加氢制乙醇酸甲酯的影响
Effects of morphology modulation on TiO2-supported Cu catalysts for selective hydrogenation of dimethyl oxalate to methyl glycolate
摘要
Abstract
As a crucial chemical intermediate,methyl glycolate(MG)has extensive applications in fields such as pharmaceuticals and fine chemicals.The route for preparing MG through the hydrogenation of dimethyl oxalate(DMO)using syngas as the raw material has green development concept and boasts high growth potential.Cu-based catalysts exhibit good catalytic performance in DMO hydrogenation reaction but tend to induce deep hydrogenation.To achieve the synergistic optimization of efficient DMO conversion and selective MG synthesis,TiO2 with different morphologies were prepared as the supports firstly,and then a series of Cu-based catalysts(Cu/TO-Nx)were fabricated via the ultrasonic impregnation method.The obtained supports and catalysts were characterized by SEM,N2 physical adsorption/desorption,XRD and so on,and the catalytic performances of Cu/TO-Nx in DMO hydrogenation to MG were investigated.The results demonstrate that support with nanosheet structure(TO-NF)possesses the highest defect degree and the fewest acidic sites,which are conducive to the uniform dispersion of Cu species and the inhibition of side reactions.The Cu/TO-NF catalyst has the highest proportion(n(Cu0)/n(Cu0+Cu+))of Cu⁰ species at 74.80%,with Cu0 particle size of 5.45 nm,and there exists an electronic interaction between the Cu species and TO-NF.Under the reaction conditions of temperature of 230℃,pressure of 2.5 MPa,weight hourly space velocity of 0.7 h-1 and n(H2)/n(DMO)of 30,the DMO conversion rate,MG selectivity and MG yield of Cu/TO-NF can reach 87.73%,82.38%and 72.27%,respectively.Moreover,the catalytic performance of Cu/TO-NF can remain basically stable after 550 h continuous reaction under the aforementioned conditions.关键词
Cu基催化剂/二氧化钛/草酸二甲酯加氢/乙醇酸甲酯/电子相互作用Key words
Cu-based catalyst/titanium dioxide/dimethyl oxalate hydrogenation/methyl glycolate/electronic interaction分类
化学化工引用本文复制引用
张雨,张旭妍,邵旭浩,艾培培,黄伟..形貌调控TiO2负载Cu催化剂对草酸二甲酯选择性加氢制乙醇酸甲酯的影响[J].低碳化学与化工,2026,51(4):59-69,11.基金项目
国家自然科学基金(22008166) (22008166)
山西省基础研究项目(202403021211029,201901D211047). (202403021211029,201901D211047)