一步合成用于环己烯环氧化反应的分层 Ti-MCM-41/MFI 复合材料

IF 4.8 3区 材料科学 Q1 CHEMISTRY, APPLIED Microporous and Mesoporous Materials Pub Date : 2024-09-03 DOI:10.1016/j.micromeso.2024.113319
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引用次数: 0

摘要

MCM-41/MFI 复合材料的成功一锅合成主要集中在 Al3+ 和 Fe3+ 的三价杂原子上,但关于 Ti-MCM-41/MFI 复合材料的一锅合成几乎没有报道。本研究以十六烷基三甲基溴化铵 CTAB 和硅灰石-1 种子为结构引导剂,以氨水为碱源,采用温度梯度水热策略,报道了 Ti-MCM-41/MFI 复合材料的一锅合成及其在环己烯环氧化反应中作为异相催化剂的应用。系统研究了 Si/Ti 摩尔比、氨水用量和 CTAB 用量对 Ti-MCM-41/MFI 复合材料的形成和性质的影响。此外,还提出了 Ti-MCM-41/MFI 复合材料样品可能的部分转化机制。合成的 Ti-HMZ-50-N3.77-Se0.05 样品具有有序的介孔结构和高含量的框架钛活性中心,具有优异的环己烯环氧化性能,在反应 5 小时内实现了 32.51 % 的环己烯转化率和 61.27 % 的环己烯氧化选择性。
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One-step synthesis of hierarchical Ti-MCM-41/MFI composites for cyclohexene epoxidation reactions

The successful one-pot synthesis of MCM-41/MFI composite is mainly concentrated on the trivalent heteroatom of Al3+ and Fe3+, however there are almost no reports about the one-pot synthesis of Ti-MCM-41/MFI composite. In this work, we reported the one-pot synthesis of Ti-MCM-41/MFI composite with a temperature-gradient hydrothermal strategy using hexadecyl trimethylammonium bromide CTAB and silicalite-1 seed as structure directing agents as well as ammonia solution as alkali source, and its application as heterogeneous catalyst in the cyclohexene epoxidation reactions. The impact of Si/Ti molar ratio and ammonia dosage as well as CTAB amount on the formation and property of Ti-MCM-41/MFI composite were systematically investigated. In addition, a possible partial transformation mechanism of Ti-MCM-41/MFI composite sample was proposed. The synthesized Ti-HMZ-50-N3.77-Se0.05 sample with ordered mesoporous structure and high content of framework titanium active centers revealed the eminent cyclohexene epoxidation performance, achieving a 32.51 % of cyclohexene conversion and a 61.27 % selectivity of cyclohexene oxide within 5 h of reaction.

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来源期刊
Microporous and Mesoporous Materials
Microporous and Mesoporous Materials 化学-材料科学:综合
CiteScore
10.70
自引率
5.80%
发文量
649
审稿时长
26 days
期刊介绍: Microporous and Mesoporous Materials covers novel and significant aspects of porous solids classified as either microporous (pore size up to 2 nm) or mesoporous (pore size 2 to 50 nm). The porosity should have a specific impact on the material properties or application. Typical examples are zeolites and zeolite-like materials, pillared materials, clathrasils and clathrates, carbon molecular sieves, ordered mesoporous materials, organic/inorganic porous hybrid materials, or porous metal oxides. Both natural and synthetic porous materials are within the scope of the journal. Topics which are particularly of interest include: All aspects of natural microporous and mesoporous solids The synthesis of crystalline or amorphous porous materials The physico-chemical characterization of microporous and mesoporous solids, especially spectroscopic and microscopic The modification of microporous and mesoporous solids, for example by ion exchange or solid-state reactions All topics related to diffusion of mobile species in the pores of microporous and mesoporous materials Adsorption (and other separation techniques) using microporous or mesoporous adsorbents Catalysis by microporous and mesoporous materials Host/guest interactions Theoretical chemistry and modelling of host/guest interactions All topics related to the application of microporous and mesoporous materials in industrial catalysis, separation technology, environmental protection, electrochemistry, membranes, sensors, optical devices, etc.
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