S_(2)O_(8)^(2-)/ZnCe_(x)Al_(2-x)O_(4)制备及催化合成乙酸正丁酯  

Preparation and catalytic activity of S_(2)O_(8)^(2-)/ZnCe_(x)Al_(2-x)O_(4) for n-butyl acetate synthesis

作　　者：田志茗[1] 刘雨佳[1] TIAN Zhi-ming;LIU Yu-jia(College of Chemistry and Chemical Engineering,Qiqihar University,Heilongjiang Qiqihar 161006,China)

机构地区：[1]齐齐哈尔大学化学与化学工程学院,黑龙江齐齐哈尔161006

出　　处：《齐齐哈尔大学学报（自然科学版）》2021年第6期70-74,共5页Journal of Qiqihar University(Natural Science Edition)

基　　金：黑龙江省自然科学基金面上资助项目(B2015014);黑龙江省教育厅基本科研业务专项课题(135209219)。

摘　　要：采用水热法制备Ce掺杂尖晶石ZnCe_(x)Al_(2-x)O_(4),通过(NH_(4))_(2)S_(2)O_(8)溶液浸渍法制备了S_(2)O_(8)^(2-)/ZnCe_(x)Al_(2-x)O_(4)固体催化剂。通过XRD、TG-DSC、IR和N_(2)吸附-脱附等手段对催化剂进行表征,实验结果表明,S_(2)O_(8)^(2-)/ZnCe_(x)Al_(2-x)O_(4)仍具有载体的尖晶石结构特征,颗粒堆积后的平均孔径约为2.66 nm,BET表面积为13.59 m^(2)/g。将S_(2)O_(8)^(2-)/ZnCe_(x)Al_(2-x)O_(4)作为催化剂应用于合成乙酸正丁酯,研究表明,采用0.10 mol/L(NH_(4))_(2)S_(2)O_(8)溶液浸渍ZnCe_(0.15)Al_(1.85)O_(4),在600℃温度下焙烧5 h制备的催化剂表现出良好的催化活性,当酸醇摩尔比为1∶1.2、催化剂用量为3%(相当于冰乙酸的质量)、回流状态下反应5 h时,酯化率可达96.3%。Ce-doped spinel was prepared by hydrothermal method.S_(2)O_(8)^(2-)/ZnCe_(x)Al_(2-x)O_(4)catalysts were prepared by(NH_(4))_(2)S_(2)O_(8)solution impregnation and characterized by means of XRD,TG-DSC,IR spectroscopic analysis and N_(2) adsorption techniques.The characterization results show that the S_(2)O_(8)^(2-)/ZnCe_(x)Al_(2-x)O_(4)still has a spinel structure characteristics as the carrier.The average pore size of S_(2)O_(8)^(2-)/ZnCe_(0.15)Al_(1.85O4) is about 2.66 nm after the accumulation of particles.The surface area is 13.59 m^(2)/g.The preparation conditions of S_(2)O_(8)^(2-)/ZnCe_(x)Al_(2-x)O_(4)were investigated by using S_(2)O_(8)^(2-)/ZnCe_(x)Al_(2-x)O_(4)as catalyst for esterification of acetic acid with n-butanol.The experimental results indicated that the catalytic activity related to the preparation conditions of catalysts.The catalyst prepared by impregnating ZnCe_(0.15)Al_(1.85)O_(4)in solution of 0.10 mol/L(NH_(4))_(2)S_(2)O_(8)solution,calcined at 600℃for 5h showed best catalytic activity.The esterification yield was up 96.3%under the conditions of the catalyst dosage 3%,n(acetic acid)∶n(n-butanol)=1∶1.2,and reaction time in refluxing state 5 h.

关 键 词：锌铝尖晶石 铈改性 催化 酯化反应 

分 类 号：O614.24[理学—无机化学]