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Titanosilicalites (MFI-type): Composition, statistical and local structure, catalytic properties
Microporous and Mesoporous Materials ( IF 4.8 ) Pub Date : 2021-08-19 , DOI: 10.1016/j.micromeso.2021.111377
Galina M. Kuz'micheva 1 , Roman D. Svetogorov 2 , Evgeny V. Khramov 2 , Galina V. Kravchenko 1 , Lev G. Bruk 1 , Zhanna Yu. Pastukhova 1 , Ekaterina B. Мarkova 3 , Anna I. Zhukova 3 , Sofia G. Chuklina 1 , Andrey V. Dorokhov 1
Affiliation  

This article presents the results of a study of three commercial titanosilicalites (TS-1, TS-1N, TS-1G) with general formula [(TixSi12-x)O24] × wH2O (MFI-type) using the X-ray study (XRPD), IR spectroscopy (FT-IR), X-ray absorption spectroscopy (EXAFS/XANES), differential scanning calorimetry (DSC), Brunauer–Emmett–Teller method (BET), UV-VIS spectroscopy. It was established that the samples contain amorphous oxygenous titanium-containing formations, which does not allow the use of quantitative elemental methods of analysis to determine the content of titanium ions in the framework. The full-profile Rietveld method was used to determine the silicate modules (Si/Ti = 53 for TS-1, Si/Ti~47 for TS-1N and TS-1G) and the coordination numbers of titanium: CNTi~5.0, CNTi = 4.5, CNTi>5.0, respectively in the structures of TS-1, TS-1N, TS-1G. The distribution of Ti4+ ions over the sites of the MFI-type structure with the orthorhombic symmetry (space group Pnma, z = 8) were found: T2, T6, T10 for TS-1, T8, T10, T5 (unlikely) for TS-1N (Т10 double positions in sinusoidal channels) and Т2, Т10, Т12, Т9 (unlikely) for TS-1G (Т10 and Т12 double positions in sinusoidal channels). The best indicators of the allyl chloride epoxidation in the epichlorohydrin process at 30 °C were achieved for TS-1N and TS-1G. A higher yield of acetaldehyde was found on the TS-1(75) sample (TS-1 sample annealed at 75 °C for 2 h) at 290 °C (non-oxidative ethanol conversion), and ethylene - on the TS-1G(500) sample (TS-1G annealed at 500 °C for 2 h) at 700 °C (propane conversion). The revealed correlations between the catalytic parameters and the characteristics of the samples studied were discussed.



中文翻译:

Titanosilicalites (MFI-type):成分、统计和局部结构、催化性能

本文介绍了三种具有通式 [(Ti x Si 12-x )O 24 ] ×  w H 2 的商业钛硅酸盐(TS-1、TS-1N、TS-1G)的研究结果O(MFI 型)使用 X 射线研究 (XRPD)、红外光谱 (FT-IR)、X 射线吸收光谱 (EXAFS/XANES)、差示扫描量热法 (DSC)、Brunauer-Emmett-Teller 方法 (BET) ), 紫外可见分光光度计。已确定样品包含无定形含氧含钛地层,这不允许使用定量元素分析方法来确定框架中钛离子的含量。全剖面 Rietveld 方法用于确定硅酸盐模块(TS-1 的 Si/Ti = 53,TS-1N 和 TS-1G 的 Si/Ti~47)和钛的配位数:CNTi~5.0,CNTi = 4.5,CNTi>5.0,分别在TS-1、TS-1N、TS-1G的结构中。Ti 4+的分布发现在具有正交对称性(空间群 Pnma,z = 8)的 MFI 型结构位点上的离子:TS-1 的T2、T6、T10、TS-1N 的T8、T10、T5(不太可能)(Т10正弦通道中的双位置)和Т2、Т10、Т12、 Т9(不太可能)对于 TS-1G(Т10 和 Т12正弦通道中的双重位置)。对于 TS-1N 和 TS-1G,在 30 °C 环氧氯丙烷工艺中烯丙基氯环氧化的最佳指标达到了。在 TS-1(75) 样品(TS-1 样品在 75°C 下退火 2 小时)在 290°C(非氧化乙醇转化)上发现了更高的乙醛收率,在 TS-1G 上发现了乙烯 - (500) 样品(TS-1G 在 500°C 下退火 2 小时)在 700°C(丙烷转化)。讨论了催化参数与所研究样品的特征之间所揭示的相关性。

更新日期:2021-08-21
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