Hollow core-shell structured TS-1@S-1 as an efficient catalyst for alkene epoxidation.

Hollow core-shell structured TS-1@S-1 as an efficient catalyst for alkene epoxidation.
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DOI:
10.1039/c9ra07893b
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发表时间:
2019-11-19
期刊:
影响因子:
3.9
通讯作者:
Liu, Y.
Liu, Y.
中科院分区:
化学3区
文献类型:
--
作者:
Wang, J.;Chen, Z.;Yu, Y.;Tang, Z.;Shen, K.;Wang, R.;Liu, H.;Huang, X.;Liu, Y.

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首次成功制备了空心核壳结构的TS-1@S-1沸石(HCS-TS),在烯烃环氧化反应中表现出优异的活性。结合TEM、UV-vis、UV-Raman、吡啶-IR、固态MAS NMR、XPS等表征,空心核壳结构TS-1@S-1沸石催化性能的提高归功于新形成的优越活性位点:HCS-TS中的缺陷Ti(OSi)3(OH)物种和未煅烧HCS-TS(HCS-TSP)中的六配位钛活性物种。有趣的是,样品中的这两种不同的钛活性物质可以通过煅烧或不在同一合成过程中构建。详细研究了可能的形成机制;表明第一步对TS-1的空心处理有利于样品中新的优越活性位点的构建,并且在第二步合成过程中TPAOH和TEOS对这些活性位点的形成存在协同作用。该策略对于提高TS-1的催化性能是可行的,适合工业规模合成TS-1。由于不同钛活性中心的形成,成功合成了具有高催化性能的空心核壳结构TS-1@S-1。
Hollow core–shell structured TS-1@S-1 zeolite (HCS-TS) was prepared successfully for the first time, which exhibited excellent activity in the epoxidation of alkenes. Combining TEM, UV-vis, UV-Raman, pyridine-IR, solid-state MAS NMR, XPS and so on characterization, the improvement in the catalytic performance of hollow core–shell structured TS-1@S-1 zeolite was credited to the newly formed superior active sites: defective Ti(OSi)3(OH) species in HCS-TS and six-coordinated titanium active species in uncalcined HCS-TS (HCS-TSP). Interestingly, these two different titanium active species in the samples could be constructed through calcination or not in the same synthesis process. A possible formation mechanism was investigated in detail; it indicated that the hollowing treatment of TS-1 in the first step was conducive to the construction of the new superior active sites in the samples, and there was a synergistic effect on the formation of these active sites between TPAOH and TEOS in the second step of the synthesis process. This strategy is feasible to enhance the catalytic performance of TS-1, and is suitable for the synthesis of TS-1 on an industrial scale. Hollow core–shell structured TS-1@S-1 with high catalytic performance was synthesized successfully owing to the formation of different titanium active centers.
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