低碳化学与化工2025，Vol.50Issue(3)：30-38,9.DOI:10.12434/j.issn.2097-2547.20240206
焙烧温度对MOF衍生Cu@C催化剂催化草酸二甲酯加氢制乙二醇性能的影响
Effects of calcination temperatures on performances of MOF-derived Cu@C catalysts for catalytic hydrogenation of dimethyl oxalate to ethylene glycol
摘要
Abstract
Hydrogenation of dimethyl oxalate(DMO)to ethylene glycol(EG)represents a pivotal step in EG production from coal-based syngas.This process is of great significance for replacing traditional petroleum-derived route to produce EG and achieving high value-added conversion of coal.Efficient and stable catalysts for catalytic hydrogenation of DMO to EG are crucial for promoting the further development of coal-based syngas for EG production.Cu-1,3,5-phenyltricarboxylic acid metal organic framework(Cu-BTC MOF)was used as a precursor and calcined under N2 atmosphere at different temperatures to obtain Cu@C-x(x is the calcination temperature)catalysts,and Cu@C-x catalysts were used to catalyze the hydrogenation of DMO to EG.The catalysts were characterized by XRD,SEM,H2-TPR,XPS and N2 physical adsorption/desorption.The effects of calcination temperatures on phase compositions,morphologies,reduction performances surface element compositions and texture properties were also investigated.The results show that calcination temperatures change the interaction between Cu species and the carbon support(Cu-O-C),thereby significantly affecting the Cu particles sizes and n(Cu+)/n(Cu0+Cu+).Thanks to the moderate interaction between Cu species and the carbon support,Cu@C-500 catalyst has the smallest Cu particle size and largest n(Cu+)/n(Cu0+Cu+).Under the reaction conditions of 240 ℃,2.5 MPa,weight hourly space velocity of 0.2 h-1 and n(H2)/n(DMO)of 200,Cu@C-500 catalyst achieves the DMO conversion rate of 100％and EG selectivity of 94.13％,and no deactivation occurs within 250 h.关键词
MOF/Cu催化剂/草酸二甲酯/乙二醇/焙烧温度Key words
MOF/Cu catalyst/dimethyl oxalate/ethylene glycol/calcination temperatures分类
化学工程引用本文复制引用
靳刘艳,赵江涛,张雨,艾培培,黄伟..焙烧温度对MOF衍生Cu@C催化剂催化草酸二甲酯加氢制乙二醇性能的影响[J].低碳化学与化工,2025,50(3):30-38,9.基金项目
国家自然科学基金青年科学基金(22008166) （22008166）
山西省面上青年基金(201901D211047) （201901D211047）
山西省高等学校科技创新项目(2019L0185). （2019L0185）
