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Efficient and reusable zeolite-immobilized acidic ionic liquids for the synthesis of polyoxymethylene dimethyl ethers
Molecular Catalysis ( IF 3.9 ) Pub Date : 2018-06-15 , DOI: 10.1016/j.mcat.2018.06.012
Heyuan Song , Ruiyun Li , Fuxiang Jin , Zhen Li , Jing Chen

A series of molecular sieve-immobilized Brønsted acidic ionic liquids ([email protected]) was prepared, characterized and utilized as efficient catalysts for the synthesis of polyoxymethylene dimethyl ethers (PODEn or DMMn) from methylal (DMM1) and trioxane (TOX). Combined characterization results from fourier transform infrared (FT-IR) spectroscopy, elemental analysis, thermogravimetry (TG), N2 adsorption-desorption (Brunauer-Emmett-Teller, BET) isotherms, X-ray diffraction (XRD), scanning electron microscopy (SEM) and temperature-programmed desorption of ammonia (NH3-TPD), suggested that the synthesized BAILs were successfully immobilized on the surface of molecular sieves through covalent bonds. Moreover, the catalytic performance tests demonstrated that NaZSM-5 immobilized SO3H-functionalized ionic liquids (ILs) i.e., [email protected], exhibited excellent activity for the acetalation of DMM1 with TOX, compared to the homogeneous catalysis of the precursors ([MIMBs]HSO4) as well as other molecular sieve-supported ILs. The influence of catalyst concentration, molar ratio of DMM1 to HCHO, temperature and reaction duration on the catalytic activity were investigated by employing [NaZSM-5IMBs]HSO4 as the catalyst. It was demonstrated that a superior conversion of formaldehyde (FA) (90.3%) and excellent selectivity for DMM3-8 (53.5%) has been achieved in mild conditions (110 °C, 2.5 MPa for 2 h). Additionally, the catalyst can be effortlessly separated by filtration and reused more than ten times without significant loss of activity.



中文翻译:

高效且可重复使用的固定化沸石的酸性离子液体,用于合成聚甲醛二甲醚

制备了一系列固定在分子筛上的布朗斯台德酸性离子液体([已电子邮件保护]),并表征为由甲基(DMM 1)和三恶烷(TOX)合成聚甲醛二甲醚(PODE n或DMM n)的有效催化剂。)。傅里叶变换红外(FT-IR)光谱,元素分析,热重分析(TG),N 2吸附-解吸(Brunauer-Emmett-Teller,BET)等温线,X射线衍射(XRD),扫描电子显微镜( SEM)和程序升温解吸的氨(NH 3-TPD),表明合成的BAILs通过共价键成功地固定在分子筛表面。此外,催化性能测试表明,与前体的均相催化相比,NaZSM-5固定的SO 3 H-官能化离子液体(ILs),即[受电子邮件保护],对于用TOX进行DMM 1缩醛化显示出优异的活性( [MIMBs] HSO 4)以及其他分子筛支持的IL。[NaZSM-5IMBs] HSO 4研究了催化剂浓度,DMM 1与HCHO的摩尔比,温度和反应时间对催化剂活性的影响。作为催化剂。结果表明,在温和的条件下(110°C,2.5 MPa,2 h),甲醛(FA)的转化率高(90.3%),对DMM 3-8的选择性高(53.5%)。另外,可以通过过滤毫不费力地分离催化剂,并重复使用十次以上,而没有明显的活性损失。

更新日期:2018-06-15
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