Ag/SiO_(2)催化草酸酯加氢制乙醇酸甲酯的床层-颗粒双尺度耦合模拟研究  

Bed-particle dual scale coupled simulation on Ag/SiO_(2) catalyzed hydrogenation of oxalate to methyl glycolate

作　　者：何传超 周静红[1] 曹约强 施尧 周兴贵[1] HE Chuanchao;ZHOU Jinghong;CAO Yueqiang;SHI Yao;ZHOU Xinggui(State Key Laboratory of Chemical Engineering,East China University of Science and Technology,Shanghai 200237,China)

机构地区：[1]华东理工大学化学工程联合国家重点实验室,上海200237

出　　处：《化工学报》2025年第2期654-666,共13页CIESC Journal

基　　金：国家自然科学基金项目(22178102,22478106)。

摘　　要：草酸二甲酯(DMO)选择性加氢制乙醇酸甲酯(MG)过程中由于目标产物为串联加氢反应的中间产物,催化剂颗粒尺度以及床层尺度的传递过程对于催化性能具有显著影响,因此颗粒催化剂的结构设计对于其工业应用极为重要。首先通过实验获取了Ag/SiO_(2)催化DMO加氢制MG的动力学方程,在此基础上构建了床层-颗粒双尺度耦合的二维反应器模型,从床层尺度与颗粒尺度描述DMO加氢过程的传递与反应过程,考察了颗粒催化剂内活性组分的宏观分布对其在单管反应器内催化性能的影响。模拟计算结果表明,采用均匀型催化剂的反应器中存在着严重的MG过度加氢问题,采用蛋壳型催化剂则能够有效抑制过度加氢产物乙二醇的生成,提升MG的收率,且能够减少活性组分用量,显著提高DMO加氢制MG工艺的经济效益。研究结果可为DMO加氢制MG工业催化剂的结构设计和制备提供基础知识和指导。The selective hydrogenation of dimethyl oxalate(DMO)to methyl glycolate(MG)involves serial hydrogenation reactions,where transport phenomena within the catalyst pellets and throughout the catalyst bed play a pivotal role in determining catalytic performance.Hence,meticulous structural design of pellet catalysts is imperative for their industrial viability.In this study,the kinetic equations were first derived from experimental data for the DMO hydrogenation to MG using Ag/SiO_(2)catalyst.Subsequently,a comprehensive two-dimensional bed-particle dual-scale model was developed to elucidate the transport and reaction dynamics of DMO hydrogenation at both scales.The impact of the active component distribution inside catalyst pellets on their catalytic performance in a single-tube reactor was investigated.Simulation results show that there is a serious problem of excessive hydrogenation of MG in reactors using uniform catalysts.Using eggshell catalysts can effectively suppress the formation of excessive hydrogenation product ethylene glycol,improve the yield of MG,and can reduce the dosage of active components and significantly improve the economic benefits of the DMO hydrogenation to MG process.These findings offer fundamental insights and practical guidance for the design and fabrication of industrial catalysts tailored for DMO hydrogenation to MG.

关 键 词：草酸二甲酯 加氢 动力学 双尺度模型 蛋壳型催化剂 数值模拟 

分 类 号：TQ203.2[化学工程—有机化工]