Shielding effect-engineered single-crystalline Ti-rich nanosized aggregated TS-1 for 1-hexene epoxidation

IF 3.5 3区工程技术 Q2 ENGINEERING, CHEMICAL AIChE Journal Pub Date : 2024-08-21 DOI:10.1002/aic.18566

Ze Zong, Xuliang Deng, Dong Lin, Yang Xu, Qiuming He, Zhe Ma, De Chen, Chaohe Yang, Xiang Feng

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Abstract

Titanosilicate with H₂O₂ stands out as a highly consequential oxidized catalytic system, prized for its user-friendly operation, mild conditions, and eco-friendly attributes. However, a synthesis strategy for large surface area titanosilicalites approaching the theoretical lowest Si/Ti ratio without extra-framework Ti species remains an ongoing challenge. In this study, we successfully synthesized single-crystalline Ti-rich nanosized aggregated TS-1 by shielding effect with a Si/Ti polymer. This polymer demonstrated effectiveness in restraining TiO₂ species by regulating the proximity of Si/Ti species in Ti-Diol-Si polymers. The polymer not only facilitated the synthesis of single-crystalline Ti-rich TS-1 but also exploited the chain length of PEG, functioning as a shielding cage by hydrogen bonds, to synthesize nanosized aggregated TS-1 (TS-1-PEG400). This TS-1-PEG400 exhibited superior conversion (~60%), selectivity (~90%), and stability in 1-hexene epoxidation. This study not only establishes a synthesis pathway for Ti-rich TS-1 but also holds the potential to enhance related industrial oxidation reactions involving titanosilicates and H₂O₂.

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用于 1- 己烯环氧化的屏蔽效应工程化富钛纳米单晶聚合 TS-1

带有 H2O2 的钛硅酸盐是一种极具影响力的氧化催化系统，因其操作简便、条件温和和生态友好的特性而备受推崇。然而，如何合成大表面积的钛硅酸盐，使其接近理论上的最低硅/钛比，且不含框架外的 Ti 物种，仍然是一个持续的挑战。在本研究中，我们利用硅/钛聚合物的屏蔽效应，成功合成了单晶富钛纳米聚集 TS-1。这种聚合物通过调节 Ti-Diol-Si 聚合物中 Si/Ti 物种的接近程度，有效抑制了 TiO2 物种。这种聚合物不仅有助于合成富含钛的单晶 TS-1，还能利用 PEG 的链长，通过氢键起到屏蔽笼的作用，从而合成纳米级的聚集 TS-1（TS-1-PEG400）。这种 TS-1-PEG400 在 1- 己烯环氧化反应中表现出卓越的转化率（约 60%）、选择性（约 90%）和稳定性。这项研究不仅建立了富钛 TS-1 的合成途径，而且有望增强涉及钛硅酸盐和 H2O2 的相关工业氧化反应。

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来源期刊

AIChE Journal 工程技术-工程：化工

CiteScore

7.10

自引率

10.80%

发文量

411

审稿时长

3.6 months

期刊介绍： The AIChE Journal is the premier research monthly in chemical engineering and related fields. This peer-reviewed and broad-based journal reports on the most important and latest technological advances in core areas of chemical engineering as well as in other relevant engineering disciplines. To keep abreast with the progressive outlook of the profession, the Journal has been expanding the scope of its editorial contents to include such fast developing areas as biotechnology, electrochemical engineering, and environmental engineering. The AIChE Journal is indeed the global communications vehicle for the world-renowned researchers to exchange top-notch research findings with one another. Subscribing to the AIChE Journal is like having immediate access to nine topical journals in the field. Articles are categorized according to the following topical areas: Biomolecular Engineering, Bioengineering, Biochemicals, Biofuels, and Food Inorganic Materials: Synthesis and Processing Particle Technology and Fluidization Process Systems Engineering Reaction Engineering, Kinetics and Catalysis Separations: Materials, Devices and Processes Soft Materials: Synthesis, Processing and Products Thermodynamics and Molecular-Scale Phenomena Transport Phenomena and Fluid Mechanics.