富钛骨架无锐钛矿型TS-1沸石的酸调合成

IF 4.7 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials Pub Date : 2025-09-08 DOI:10.1016/j.micromeso.2025.113853

Xiaojing Song , Shuang Liu , Shuang Gao , Zuochao Wang , Hao Zhang

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引用次数: 0

摘要

TS-1沸石被认为是沸石催化的里程碑，需要精密的工程来平衡框架Ti掺入和锐钛矿抑制，以获得卓越的环氧化性能。本文报道了以石胆酸（LCA）为双功能分子筛生长调节剂的一步水热策略合成富钛框架无锐钛矿的TS-1分子筛。时间分辨结晶结合表征揭示了LCA的调控作用，其中LCA通过羧酸盐/羟基介导的Ti- o - si配位延长了TS-1合成的诱导期，在抑制锐钛矿相形成的同时提高了框架Ti的掺入率。优化后的TS-1-0.1LCA在h2o2介导的1-己烯氧化反应中表现出优异的催化性能，对环氧化物的转化率为52%，选择性为97%。此外，TS-1-0.1LCA的TOF值是TS-1-Con的3倍以上（200 h−1 vs 64 h−1）。本研究通过lca导向的配位工程，连接沸石基础化学和工业环氧化工艺，建立了设计高效TS-1催化剂的系统框架。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

Lithocholic acid-modulated synthesis of anatase-free TS-1 zeolite with Ti-rich framework for superior alkene oxidation

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Lithocholic acid-modulated synthesis of anatase-free TS-1 zeolite with Ti-rich framework for superior alkene oxidation

TS-1 zeolite, recognized as milestones in zeolite catalysis, require precision engineering to balance framework Ti incorporation and anatase suppression for superior epoxidation performance. Herein, we report a one-step hydrothermal strategy using lithocholic acid (LCA) as bifunctional zeolite growth regulator to synthesize anatase-free TS-1 zeolite with Ti-rich framework. Time-resolved crystallization combined with characterizations reveals the regulation of LCA, in which LCA extends induction period of TS-1 synthesis through carboxylate/hydroxy-mediated Ti-O-Si coordination, enabling the higher framework Ti incorporation while suppressing anatase phase formation. The optimized TS-1-0.1LCA exhibits exceptional catalytic performance in H₂O₂-mediated 1-hexene oxidation with 52 % of conversion and 97 % of selectivity to epoxides. Besides, the TOF value of TS-1-0.1LCA is over 3-fold (200 h⁻¹ vs 64 h⁻¹) than that of TS-1-Con. This work establishes a systematic framework for designing highly efficient TS-1 catalysts through LCA-directed coordination engineering, bridging fundamental zeolite chemistry and industrial epoxidation processes.

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来源期刊

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.