应用化学 ›› 2019, Vol. 36 ›› Issue (11): 1294-1300.DOI: 10.11944/j.issn.1000-0518.2019.11.190081

• 研究论文 • 上一篇    下一篇

CTAB-P123辅助制备有序介孔KF/Al-Ce-SBA-15固体碱及其催化性能

刘宁(),刘水林,伍素云,唐新德,吴智,李爱阳()   

  1. 湖南工学院材料与化学工程学院,新型建筑材料研究院 湖南 衡阳 421002
  • 收稿日期:2019-04-01 接受日期:2019-07-09 出版日期:2019-11-01 发布日期:2019-11-05
  • 通讯作者: 刘宁
  • 基金资助:
    国家自然科学基金青年项目(51802093)湖南省自然科学基金(2019JJ60026,2019JJ50107)湖南省教育厅优秀青年项目(18B465)“功能金属有机材料”湖南省普通高等学校重点实验室(GN18K01)湖南省应用特色学科材料科学与工程学科(湘教通[2018]469号)资助

CTAB-P123-Assisted Synthesis of Orderly Mesoporous KF/Al-Ce-SBA-15 Solid Base and Its Catalytic Application

LIU Ning(),LIU Shuilin,WU Suyun,TANG Xinde,WU Zhi,LI Aiyang()   

  1. Department of Materials and Chemical Engineering,New Building Materials Academy,Hunan Institute of Technology,Hengyang,Hunan 421002,China
  • Received:2019-04-01 Accepted:2019-07-09 Published:2019-11-01 Online:2019-11-05
  • Contact: LIU Ning
  • Supported by:
    Supported by the National Natural Science Foundation of China(No. 51802093), the Hunan Provincial Natural Science Foundation of China(No.2019JJ60026, No.2019JJ50107), the Foundation of Hunan Educational Committee(No.18B465), the Key Laboratory of Functional Organometallic Materials of Hengyang Normal University(No.GN18K01), and the Characteristic Application Discipline of Material Science and Engineering in Hunan(No.Xiang-Jiao-Tong[2018]369)

摘要:

为了缩短有序介孔氧化硅(SBA-15)基固体碱催化剂的工艺流程,制备长程有序介孔固体碱,本文以十六烷基三甲基溴化胺(CTAB)-三嵌段表面活性剂P123为模板剂,以KF为改性剂,两步法合成有序介孔KF/Al-Ce-SBA-15(KF/ACS)固体碱催化剂,采用小角X射线衍射(小角XRD)、N2吸附-脱附曲线、透射电子显微镜(TEM)、扫描电子显微镜(SEM)、CO2程序升温脱附(CO2-TPD)等手段,对催化剂的结构与性能进行表征,并研究了其在合成丙二醇甲醚(PM)中的催化性能。 当n(Al)/n(Ce)=0.12,KF的质量分数为10%时,KF/ACS催化剂不仅能够保持长程有序介孔结构,并且显示出强碱性能。 在催化甲醇与环氧丙烷(PO)合成PM的反应中,PM的收率达到92.0%,1-甲氧基-2-丙醇(PPM)选择性达到96.1%以上,并能有效抑制二丙二醇甲醚等副产物。

关键词: 十六烷基三甲基溴化胺, 三嵌段表面活性剂P123, 介孔固体碱, SBA-15, Al-Ce复合物

Abstract:

The orderly mesoporous KF/Al-Ce-SBA-15(KF/ACS) solid bases were successfully prepared with cetyltrimethylammonium bromide(CATB)- poly(ethylene oxide)/poly(propylene oxide)/poly(ethylene oxide) triblock copolymer (P123) as the dual-template and KF as the modifier in two steps. The structure and property of the obtained catalysts were characterized by X-ray diffraction (XRD), N2 adsorption-desorption, transmission electron microscopy (TEM), scanning electron microscopy (SEM) and CO2-temperature programmed desorption (TPD). The results illustrated that the KF/ACS catalysts possess both an ordered mesostructure and superbasicity when the introduced Al/Ce atomic ratio is 0.12 and the loading amounts(mass fraction) of KF is 10%. The catalytic activity of the prepared materials was evaluated in the ring-opening reaction of propylene oxide (PO) with methanol. It shows excellent catalytic performance exhibiting 92.0% yield of propylene glycol monomethyl ether (PM) and 96.1% selectivity to 1-methoxy-2-propanol (PPM) and the by-products of dipropylene glycol methyl ether was effectively inhibited.

Key words: cetyltrimethylammonium bromide, triblock copolymer P123, mesoporous solid bases, SBA-15, Al-Ce mixed oxides