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将均相磷钨钼酸材料进行拓扑转变以制备用于碳水化合物转化为烷基甲基糠醛和烷基乙酰丙酸酯的多相固体酸催化剂。

Topotactic transformation of homogeneous phosphotungastomolybdic acid materials to heterogeneous solid acid catalyst for carbohydrate conversion to alkyl methylfurfural and alkyl levulinate.

作者信息

Gupta Dinesh, Mukesh Chandrakant, Pant Kamal K

机构信息

Chemical Engineering, Indian Institute of Technology Delhi New Delhi 110 016 India

出版信息

RSC Adv. 2020 Jan 2;10(2):705-718. doi: 10.1039/c9ra03300a.

DOI:10.1039/c9ra03300a
PMID:35494434
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9048189/
Abstract

The strong interaction of higher transition metal oxides with inorganic non-metals can be promising for generating highly acidic three-dimensional materials by design. A comprehensive controlled acidity of heteropolyacid-like catalyst and interpretation of the microstructure and mechanism of the formation of a versatile heterogeneous solid acid catalyst, HPWMoO has been heterogenized by biomass-derived cystine as organic linkers to control the acidity of as-synthesized materials, which have greater acidity and complexity in separation from the reaction mixture. The new and unique results obtained in catalysis done in biphasic reaction. Cystine binds to the surface of HPWMoO , and the topotactic transition occurred, change the morphology and lattice parameter. We described here a sustainable transformation of highly acidic (0.84 mmol g) heteropoly acid (HPWMoO ) to cystine anchored on the active surface of the heteropoly acid and controlled the acidity (0.63 mmol g) and heterogenized the materials. As synthesized materials have been showing that for the direct formation of alkyl levulinate and furanics intermediate from carbohydrates. HPWMoO and HPWMoO -Cys, act as acidic catalyst, and catalyse the mono- and disaccharides that are dissolved in primary and secondary alcohols to alkyl levulinate (AL) and alkyl methylfurfural at 170 °C under microwave irradiation with glucose as the substrate, AL yield reaches 62% with 84.95% selectivity. The catalyst can be easily recovered by filtration and minimum five times reused after calcination without any substantial change in the product selectivity. The analytical analysis of as-synthesis materials done by NH-TPD, BET, XRD, FESEM, TEM, HRTEM, FTIR, ATR, TGA, DTA to stabilized the morphology and acidity controlled mechanism.

摘要

较高价态过渡金属氧化物与无机非金属的强相互作用有望通过设计生成高酸性三维材料。通过生物质衍生的胱氨酸作为有机连接体对类杂多酸催化剂进行综合酸度控制,并对通用多相固体酸催化剂HPWMoO的微观结构和形成机理进行解释,以控制合成材料的酸度,这些材料具有更高的酸度且在从反应混合物中分离时更复杂。在双相反应催化中获得了新颖独特的结果。胱氨酸与HPWMoO的表面结合,发生了拓扑转变,改变了形态和晶格参数。我们在此描述了一种将高酸性(0.84 mmol g)杂多酸(HPWMoO)可持续转化为锚定在杂多酸活性表面的胱氨酸,并控制酸度(0.63 mmol g)以及使材料多相化的过程。合成的材料已表明可直接从碳水化合物形成乙酰丙酸酯和呋喃类中间体。HPWMoO和HPWMoO - Cys作为酸性催化剂,在170°C微波辐射下,以葡萄糖为底物,催化溶解在伯醇和仲醇中的单糖和二糖生成乙酰丙酸烷基酯(AL)和烷基甲基糠醛,AL产率达到62%,选择性为84.95%。催化剂可通过过滤轻松回收,煅烧后至少可重复使用五次,且产物选择性无任何实质性变化。通过NH-TPD、BET、XRD、FESEM、TEM、HRTEM、FTIR、ATR、TGA、DTA对合成材料进行分析,以确定形态和酸度控制机制。

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