Synthesis of Al-containing Sn-beta with tunable brønsted and lewis acidity for conversion of glucose to 5-hydroxymethylfurfural

IF 4.8 3区材料科学 Q1 CHEMISTRY, APPLIED Microporous and Mesoporous Materials Pub Date : 2024-04-26 DOI:10.1016/j.micromeso.2024.113157

Yaxin Nie , Yangyang Ma , Jie Hu , Xiaomei Yang , Lipeng Zhou , Yunlai Su

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Abstract

Sn–Al-Beta zeolites with less silanol defects were synthesized in fluoride media. The effects of the amount of organic template (tetraethylammonium hydroxide, TEAOH), mineralizer (NH₄F), Al and Sn on the synthesis, acidity and catalytic performance were systematically studied. The synthesized Sn–Al-Beta zeolites were characterized by XRD, SEM, ²⁷Al MAS NMR, UV–vis DRS and FT-IR spectroscopy of hydroxy region and pyridine adsorption. The optimum values of n_TEAOH/n_Si and n_F-/n_Si were same (0.3) for synthesizing Sn–Al-Beta with high crystallinity at 140 °C for 7 d. Moreover, decreasing n_F-/n_Si facilitated the incorporation of Al into the framework. The crystallization rate of Sn–Al-Beta is similar with that of Sn-Beta. Sn was promoted to enter the framework with the increase of Al content, while elevating Sn content has no effect on the incorporation of Al into the framework. The catalytic performance of Sn–Al-Beta was investigated for conversion of glucose to 5-hydroxymethylfurfural in water-containing solvent. Sn–Al-Beta synthesized in fluoride media is more stable than the post-synthesized sample.

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合成具有可调布氏酸度和勒维斯酸度的含铝锡β，用于将葡萄糖转化为 5-羟甲基糠醛

在氟化介质中合成了硅醇缺陷较少的 Sn-Al-Beta 沸石。系统研究了有机模板（四乙基氢氧化铵，TEAOH）、矿化剂（NH4F）、Al 和 Sn 的用量对合成、酸度和催化性能的影响。通过 XRD、SEM、27Al MAS NMR、UV-vis DRS 和 FT-IR 光谱分析羟基区和吡啶的吸附情况，对合成的 Sn-Al-Beta 沸石进行了表征。nTEAOH/nSi 和 nF-/nSi 的最佳值（0.3）相同，可在 140 °C 下 7 d 合成高结晶度的 Sn-Al-Beta。Sn-Al-Beta 的结晶速率与 Sn-Beta 相似。随着 Al 含量的增加，Sn 进入框架的速度加快，而 Sn 含量的增加对 Al 进入框架没有影响。研究了 Sn-Al-Beta 在含水溶剂中将葡萄糖转化为 5-羟甲基糠醛的催化性能。在氟介质中合成的 Sn-Al-Beta 比合成后的样品更稳定。

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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.