1-Pentene epoxidation in catalytic microfabricated reactors

1-Pentene epoxidation in catalytic microfabricated reactors
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DOI:
10.1016/j.jcat.2003.11.001
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发表时间:
2004-04
影响因子:
7.3
通讯作者:
Y. Wan;J. Chau;K. Yeung;A. Gavriilidis
Y. Wan;J. Chau;K. Yeung;A. Gavriilidis
中科院分区:
化学1区
文献类型:
--
作者:
Y. Wan;J. Chau;K. Yeung;A. Gavriilidis

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制备了涂有TS-1催化剂的硅玻璃微反应器,并用于过氧化氢环氧化1-戊烯的连续流动反应。为了获得小的晶体尺寸和足够的沸石膜厚度,在沸石生长之前对微通道进行播种是必要的。通过调整合成条件和使用三乙氧基甲基硅烷(TEMS)作为晶体生长抑制剂,进一步减小了晶体尺寸。沸石膜形态和晶体取向对反应器性能没有显示出任何显著影响。然而,发现反应速率随着沸石膜中TS-1晶体尺寸的减小和四面体配位Ti(IV)的量的增加而增加。观察到催化剂失活,由有机化合物的存在和Ti从微孔框架中浸出引起。
Silicon-glass microreactors with TS-1 catalyst wall coatings were fabricated and used for 1-pentene epoxidation with hydrogen peroxide in continuous flow. Seeding of the microchannels before zeolite growth was necessary to obtain a small crystal size and a sufficient zeolite film thickness. Crystal size was further reduced by adjusting synthesis conditions and utilizing triethoxymethylsilane (TEMS) as a crystal growth inhibitor. Zeolite film morphology and crystal orientation did not show any significant effect on reactor performance. However, reaction rate was found to increase with decreasing TS-1 crystal size in the zeolite films and with increasing amount of tetrahedrally coordinated Ti(IV). Catalyst deactivation was observed, caused by the presence of organic compounds and Ti leaching from the microporous framework.