Effective hierarchization of TS-1 and its catalytic performance in cyclohexene epoxidation

Effective hierarchization of TS-1 and its catalytic performance in cyclohexene epoxidation
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DOI:
10.1016/j.micromeso.2016.06.031
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发表时间:
2016-10-01
影响因子:
5.2
通讯作者:
Gora-Marek, Kinga
Gora-Marek, Kinga
中科院分区:
材料科学2区
文献类型:
--
作者:
Tekla, Justyna;Tarach, Karolina A.;Gora-Marek, Kinga

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结果表明,经碱性介质化学处理后,TS-1形成了高度发达的分层结构。通过甲醇对羟基的酯化反应,改性了TS-1表面的疏水性,获得了真正意义上的微/介孔材料。通过XRD和低温氮吸附研究证实了微孔特征的保存。通过吡啶吸附的红外研究和Si-29 MAS NMR研究,提供了介孔钛硅矿酸性性质的详细信息。内部介孔发育良好,且Ti4+原子保持在四面体骨架位置,使得其环己烯分子转化的催化活性比天然微孔TS-1高7倍。最高效的介孔二氧化钛对环氧化物的选择性达到96%。(C) 2016 Elsevier Inc.版权所有。
The presented data showed that the chemical treatment of TS-1 with alkaline medium resulted in the formation of highly developed hierarchical structures. The esterification of the hydroxyl groups by methanol allowed modifying the hydrophobicity of TS-1 surface and obtaining truly micro/mesoporous material. The preservation of microporous characteristics was confirmed by XRD and low temperature nitrogen sorption studies. Detailed information on acidic properties of mesoporous titanosilicalites was delivered by IR studies of pyridine sorption and implicitly from Si-29 MAS NMR investigations. Well developed internal mesoporosity together with the retaining of Ti4+ atoms in tetrahedral framework positions offered 7-fold higher catalytic activity for the conversion of cyclohexene molecules than the native microporous TS-1. The selectivity to epoxide reached the value of 96% for the most efficient mesoporous titanosilicate. (C) 2016 Elsevier Inc. All rights reserved.