摘要
以金属有机骨架UiO-66(Zr)和(NH_(4))_(2)SO_(4)为原料制备了高稳定性固体酸催化剂SUA500,将其用于催化油酸与甲醇的酯化反应生产生物柴油过程,以考察催化活性和稳定性。同时,借助XRD、FTIR、N_(2)吸附-脱附、Py-FTIR和XPS等表征手段分析催化剂理化特性与催化活性之间的内在联系。结果表明,当UiO-66(Zr)与(NH_(4))_(2)SO_(4)质量比为1∶1、活化温度为500℃、研磨时间为40 min和活化时间为4 h时,SUA500的酸量高达11.08 mmol/g,且具有良好的催化活性。具体表现为:在催化剂质量分数6%、甲醇与油酸摩尔比8、反应温度70℃、反应时间2 h时,酯化转化率达到93.62%,多次重复使用后催化活性未出现明显下降;并计算得到SUA500催化酯化反应的活化能为38.21 kJ/mol,指前因子为1144.76 min^(-1)。
A highly stable solid acid catalyst SUA500 is synthesized from MOF-based UiO-66(Zr)and(NH_(4)_(2)SO_(4),which is applied to catalyze the esterification reaction of oleic acid with methanol for biodiesel to investigate its catalytic activity and stability.In the meantime,the physical property and catalytic activity of the catalyst are analyzed by means of XRD,FTIR,N_(2)adsorption and desorption,XPS and Py-FTIR to reveal their inter-relationship.Results indicate that with the mass ratio of UiO-66(Zr)toNH_(4))_(2)SO_(4)of 1∶1 and the activation temperature of 500℃,the grinding time of 40 min and the activation time of 4 h,the acid amount of SUA500 is as high as 11.08 mmol/g,and it has excellent catalytic activity.For specific performance,the esterification conversion of 93.62%is achieved with the catalyst mass fraction of 6%and molar ratio of alcohol to oleic acid of 8 at 70℃for 2 h.No obvious catalytic activity loss is detected during repeated use.The activation energy and pre-exponential factor of catalyzed esterification reaction by SUA500 is 38.21 kJ/mol and 1144.76 min^(-1),respectively.
作者
楚会君
李国宁
李辉
郭敏
李燕
王桂荣
陆万鹏
周守军
于明志
CHU Huijun;LI Guoning;LI Hui;GUO Min;LI Yan;WANG Guirong;LU Wanpeng;ZHOU Shoujun;YU Mingzhi(School of Thermal Engineering,Shandong Jianzhu University,Ji′nan 250101,China;State Grid Shandong Integrated Energy Service Co.,Ltd,Ji′nan 250000,China)
出处
《石油学报(石油加工)》
EI
CAS
CSCD
北大核心
2022年第5期1090-1101,共12页
Acta Petrolei Sinica(Petroleum Processing Section)
基金
国家自然科学基金项目(51806126)
山东省高等学校科技计划(J18KA087)
山东建筑大学博士基金(XNBS1603)资助。