Au@Snβ zeolite as stable and active catalyst for the conversion of glycerol to methyl lactate

IF 6.5 1区化学 Q2 CHEMISTRY, PHYSICAL

Journal of Catalysis Pub Date : 2025-02-01 DOI:10.1016/j.jcat.2024.115913

Shengqiang Zhou , Tianliang Lu , Lipeng Zhou , Xiaomei Yang

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Abstract

Au/Sn-zeolite catalysts showed high activity for selective conversion of glycerol to methyl lactate, but suffered from poor stability under the reaction conditions in our previous report (ACS Catal. 2017, 7, 7274). Encapsulation of Au nanoparticles within zeolite is a promising strategy to enhance their stability in catalytic reaction. Herein, one-pot synthesis of Au@Snβ was achieved by a mercaptosilane-assisted hydrothermal synthesis method. The protocol involves crystallization of Snβ synthesis gels around coordinated Au precursors, resulting in Snβ framework constraining Au coordination complexes. The confinement of small (∼2.89 nm) and uniform Au particles within Snβ was achieved. The bifunctional catalyst composed of oxidative sites (Au) and Lewis acid sites (Sn) gave 77.3 % methyl lactate (MLA) yield from the base-free selective conversion of glycerol (GLY). The TOF value of Au@Snβ was higher than that of Au/Sn-zeolite in our previous report. Moreover, the special structure protects Au nanoparticles from sintering or agglomeration and improves the stability and recyclability in selective oxidation of GLY to MLA.

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Au@Snβ 沸石作为甘油转化为乳酸甲酯的稳定活性催化剂

Au/ sn沸石催化剂在甘油选择性转化为乳酸甲酯方面表现出较高的活性，但在我们之前的报告中，反应条件下稳定性较差（ACS catalal . 2017, 7,7274）。将金纳米颗粒包埋在沸石中是提高其催化稳定性的一种很有前途的方法。本文采用巯基硅烷辅助水热合成法，实现了Au@Snβ的一锅合成。该方案涉及Snβ合成凝胶在配位金前体周围结晶，导致Snβ框架约束Au配位配合物。在Snβ中实现了小的（~ 2.89 nm）和均匀的Au粒子的约束。由氧化位（Au）和路易斯酸位（Sn）组成的双功能催化剂使无碱选择性转化甘油（GLY）的乳酸甲酯（MLA）产率达到77.3 %。Au@Snβ分子筛的TOF值高于我们之前报道的Au/ sn分子筛。此外，特殊的结构保护了金纳米粒子不烧结或团聚，提高了GLY选择性氧化成MLA的稳定性和可回收性。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Journal of Catalysis 工程技术-工程：化工

CiteScore

12.30

自引率

5.50%

发文量

447

审稿时长

31 days

期刊介绍： The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes. The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods. The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.

文献相关原料

公司名称

产品信息

阿拉丁

Methyl glycolate (MGO, 98 %)

阿拉丁

Methyl glycerate (MGLA, 97 %)

阿拉丁

MPTS (98 %)

阿拉丁

Tetraethyl orthosilicate (TEOS, AR)

阿拉丁