Selective hydrogenolysis of 5-hydroxymethylfurfural to 5-methylfurfural over Au/TiO2
Selective hydrogenolysis of 5-hydroxymethylfurfural to 5-methylfurfural over Au/TiO2
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DOI：
10.1016/j.apcatb.2023.122893
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发表时间：
2023-05
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通讯作者：
Lin Dong;Jordi Morales‐Vidal;Lili Mu;Licheng Li;N. López;J. Pérez–Ramírez;Zupeng Chen
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文献类型：
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作者：
Lin Dong;Jordi Morales‐Vidal;Lili Mu;Licheng Li;N. López;J. Pérez–Ramírez;Zupeng Chen
5-甲基糠醛（MF）是一种重要的大宗化学品，用作食品添加剂和合成中间体。开辟一条从 5-羟甲基糠醛 (HMF) 高选择性合成 MF 的可持续路线具有重要意义，但也被证明极具挑战性。在此，我们报告了一种通过锐钛矿支撑的金催化剂（Au/a-TiO2）从 HMF 选择性生产 MF 的有效工艺。 HMF氢解过程中，所需的C双键O键得以保留，并且可以以83.1%的高收率获得MF，在间歇和流动操作中均表现出优异的稳定性。实验和理论分析相结合，将 Au/a-TiO2 的优越性能归因于载体中高浓度氧空位驱动的有限 H 进入、反应物低吸附和避免冷凝的协同效应。这项研究强调了一种调整活性物质覆盖范围的新方法，用于将可再生化合物选择性转化为高附加值化学品。
5-Methylfurfural (MF) is a critical commodity chemical used as food additive and synthetic intermediate. Opening a sustainable route towards highly selective synthesis of MF from 5-hydroxymethylfurfural (HMF) is of great significance, but has demonstrated extremely challenging. Herein, we report an efficient process for the selective production of MF from HMF over an anatase-supported gold catalyst (Au/a-TiO2). During the hydrogenolysis of HMF, the desired Cdouble bondO bond is maintained and MF can be obtained in a high yield of 83.1 %, exhibiting excellent stability both in batch and flow operation. A combination of experimental and theoretical analyses attribute the superior performance of Au/a-TiO2to the synergistic effect of limited H access, low adsorption of reactants, and avoiding condensation, driven by the high concentration of oxygen vacancies in the support. This study highlights a novel approach of tailoring the coverage of active species for the selective transformation of renewable compounds into high-value-added chemicals.