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用于生物基乙酰丙酸和呋喃类化合物催化转移氢化及酸反应的微孔/介孔LTL衍生材料。

Micro/mesoporous LTL derived materials for catalytic transfer hydrogenation and acid reactions of bio-based levulinic acid and furanics.

作者信息

Antunes Margarida M, Silva Andreia F, Fernandes Auguste, Ribeiro Filipa, Neves Patrícia, Pillinger Martyn, Valente Anabela A

机构信息

Department of Chemistry, CICECO-Aveiro Institute of Materials, University of Aveiro, Aveiro, Portugal.

Centro de Química Estrutural, Instituto Superior Técnico, Universidade de Lisboa, Lisboa, Portugal.

出版信息

Front Chem. 2022 Sep 29;10:1006981. doi: 10.3389/fchem.2022.1006981. eCollection 2022.

DOI:10.3389/fchem.2022.1006981
PMID:36247668
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9558274/
Abstract

The biomass-derived platform chemicals furfural and 5-(hydroxymethyl)furfural (HMF) may be converted to α-angelica lactone (AnL) and levulinic acid (LA). Presently, LA (synthesized from carbohydrates) has several multinational market players. Attractive biobased oxygenated fuel additives, solvents, may be produced from AnL and LA via acid and reduction chemistry, namely alkyl levulinates and γ-valerolactone (GVL). In this work, hierarchical hafnium-containing multifunctional Linde type L (LTL) related zeotypes were prepared via top-down strategies, for the chemical valorization of LA, AnL and HMF via integrated catalytic transfer hydrogenation (CTH) and acid reactions in alcohol medium. This is the first report of CTH applications (in general) of LTL related materials. The influence of the post-synthesis treatments/conditions (desilication, dealumination, solid-state impregnation of Hf or Zr) on the material properties and catalytic performances was studied. AnL and LA were converted to 2-butyl levulinate (2BL) and GVL in high total yields of up to 100%, at 200°C, and GVL/2BL molar ratios up to 10. HMF conversion gave mainly the furanic ethers 5-(-butoxymethyl)furfural and 2,5-bis(-butoxymethyl)furan (up to 63% total yield, in 2-butanol at 200°C/24 h). Mechanistic, reaction kinetics and material characterization studies indicated that the catalytic results depend on a complex interplay of different factors (material properties, type of substrate). The recovered-reused solids performed steadily.

摘要

生物质衍生的平台化学品糠醛和5-(羟甲基)糠醛(HMF)可转化为α-当归内酯(AnL)和乙酰丙酸(LA)。目前，LA(由碳水化合物合成)有几家跨国市场参与者。有吸引力的生物基含氧燃料添加剂、溶剂可通过酸和还原化学，即烷基乙酰丙酸酯和γ-戊内酯(GVL)，由AnL和LA生产。在这项工作中，通过自上而下的策略制备了分级含铪多功能Linde型L(LTL)相关沸石型材料，用于通过在醇介质中的集成催化转移氢化(CTH)和酸反应对LA、AnL和HMF进行化学增值。这是关于LTL相关材料CTH应用(一般而言)的首次报道。研究了合成后处理/条件(脱硅、脱铝、Hf或Zr的固态浸渍)对材料性能和催化性能的影响。在200°C下，AnL和LA以高达100%的总高收率转化为2-丁基乙酰丙酸酯(2BL)和GVL，GVL/2BL摩尔比高达10。HMF转化主要生成呋喃醚5-(丁氧基甲基)糠醛和2,5-双(丁氧基甲基)呋喃(在200°C/24小时的2-丁醇中，总收率高达63%)。机理、反应动力学和材料表征研究表明，催化结果取决于不同因素(材料性能、底物类型)的复杂相互作用。回收再利用的固体表现稳定。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c673/9558274/1b768678779f/fchem-10-1006981-g012.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c673/9558274/0554d4d27c96/FCHEM_fchem-2022-1006981_wc_sch1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c673/9558274/7c0730f9c714/fchem-10-1006981-g001.jpg
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