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[1]孙文娟,艾胜兰,薛冶,等.Al-SO3H-SBA-15孔径可控制备及其对醋酸与异丁烯加成酯化的催化性能[J].南京工业大学学报(自然科学版),2017,39(04):30-36.[doi:10.3969/j.issn.1671-7627.2017.04.006]
 SUN Wenjuan,AI Shenglan,XUE Ye,et al.Pore controlled preparation of Al-SO3H-SBA-15 for the addition of acetic acid and isobutylene[J].Journal of NANJING TECH UNIVERSITY(NATURAL SCIENCE EDITION),2017,39(04):30-36.[doi:10.3969/j.issn.1671-7627.2017.04.006]
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Al-SO3H-SBA-15孔径可控制备及其对醋酸与异丁烯加成酯化的催化性能()
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《南京工业大学学报(自然科学版)》[ISSN:1671-7627/CN:32-1670/N]

卷:
39
期数:
2017年04期
页码:
30-36
栏目:
出版日期:
2017-07-20

文章信息/Info

Title:
Pore controlled preparation of Al-SO3H-SBA-15 for the addition of acetic acid and isobutylene
文章编号:
1671-7627(2017)04-0030-07
作者:
孙文娟1艾胜兰1薛冶2汤吉海1陈献1费兆阳1崔咪芬1乔旭1
1.南京工业大学 化工学院,江苏 南京 210009; 2.吉化集团公司 物流中心,吉林 吉林 132022
Author(s):
SUN Wenjuan1AI Shenglan1XUE Ye2TANG Jihai1CHEN Xian1FEI Zhaoyang1CUI Mifen1QIAO Xu1
1.College of Chemical Engineering,Nanjing Tech University,Nanjing 210009,China; 2.Logistic Center,Jilin Chemical Group Company,Jilin 132022,China
关键词:
分子筛 均三甲苯 孔径调控 催化 酯化 醋酸叔丁酯
Keywords:
molecular sieves trimethylbenzene pore regulation catalysis esterification tertiary butyl acetate
分类号:
O642.5
DOI:
10.3969/j.issn.1671-7627.2017.04.006
文献标志码:
A
摘要:
以均三甲苯为调节剂,采用一步共缩合法制备一系列孔径可调(3.71~4.76 nm)、高比表面积、Al掺杂且磺酸嫁接的介孔分子筛SBA-15(x-AS-SBA-15)。通过小角度X线衍射(SAXRD)、N2吸附-脱附、热分析(TG)、NH3程序升温脱附(NH3-TPD)、傅里叶变换红外光谱(FT-IR)、紫外-可见光谱(UV-Vis)和扫描电子显微镜(SEM)等手段对x-AS-SBA-15的结构、酸量等理化性质进行表征。结果表明:x-AS-SBA-15仍然留有六方介孔的相结构,但是随着x值的增大,有序介孔分子筛的孔径减小,有序度有所降低。同时研究了x-AS-SBA-15在醋酸与异丁烯无溶剂加成酯化反应中的催化性能,结果表明:50-AS-SBA-15具有最优的催化活性和产物选择性。50-AS-SBA-15用量为醋酸的5%、反应温度为30 ℃、烯酸摩尔比为3:1时,醋酸转化率为93.5%,醋酸叔丁酯选择性为94.0%。催化剂拥有良好的稳定性,重复利用5次催化活性依旧保持稳定。
Abstract:
The modified SBA-15 materials(x-AS-SBA-15)with Al ions and organo-sulfonic acid were synthesized in a one-pot approach of co-condensing inorganic-organic reagents in the presence of different amounts of trimethylbenzene(TMB).The obtained materials was characterized by small angle X-ray diffraction(SAXRD),N2 adsorption-desorption,thermal analysis(TG),temperature programmed desorption of NH3(NH3-TPD),Fourier transform infrared spectroscopy(FT-IR),ultraviolet-visible spectroscopy(UV-Vis)and scanning electron microscope(SEM)techniques.Results showed that x-AS-SBA-15 had typically mesoporous structure with tunable pore size of 3.71-4.76 nm and huge specific surface area.However the pore size and the specific pore volume decreased with the increase of TMB amount.The activity of x-AS-SBA-15 in the additive reaction of acetic acid with isobutene was investigated.It turned out that the 50-AS-SBA-15 had the best catalytic activity and the product selectivity.The conversion of acetic acid could reach 93.5% with the selectivity of tertiary butyl acetate as high as 94.0% over 50-AS-SBA-15,using a catalyst loading of 5% and isobutene/acetic acid molar ratio of 3:1 under 30 ℃.The 50-AS-SBA-15 catalyst could be reused up to five times without significant loss of catalytic activity.

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备注/Memo

备注/Memo:
收稿日期:2016-05-06
基金项目:国家自然科学基金(21276126); 江苏省“六大人才高峰”(2015-XCL-017); 江苏高校优势学科建设工程
作者简介:孙文娟(1990—),女,山东滨州人,硕士,主要研究方向为绿色化工与原子经济反应; 汤吉海(联系人),教授,E-mail:jhtang@njtech.edu.cn.
引用本文:孙文娟,艾胜兰,薛冶,等.Al-SO3H-SBA-15孔径可控制备及其对醋酸与异丁烯加成酯化的催化性能[J].南京工业大学学报(自然科学版),2017,39(4):30-36..
更新日期/Last Update: 2017-07-31