Oxidation of 2,5-bis(hydroxymethyl)furan to 2,5-furandicarboxylic acid with morphology-dependent Au/CeO2 catalysts

IF 4.7 2区 化学 Q2 CHEMISTRY, PHYSICAL Applied Catalysis A: General Pub Date : 2024-08-28 DOI:10.1016/j.apcata.2024.119929
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Abstract

2,5-Furandicarboxylic acid (FDCA), a bio-based diacid with a rigid ring, has a similar structure to petroleum-based terephthalic acid. Its co-polyester with ethylene glycol has excellent performance in terms of thermal and mechanical properties. Herein, an Au/CeO2-rod catalyst with rich oxygen vacancies was developed to achieve the efficient oxidation of 2,5-bis(hydroxymethyl)furan (BHMF) to FDCA with a 92 % yield under mild conditions, with the addition of 4 equivalents of Na2CO3 at 80℃ under 2 MPa O2 for 6 h. The large specific surface area of CeO2-rod is beneficial for better dispersion of Au nanoparticles. Meanwhile, the high activity of Au/CeO2-rod can be attributed to that the rod-shaped CeO2 exposed more active (100) facets, resulting in strong metal-support interaction between Au nanoparticles and CeO2-rod. This could generate more Au species with oxidized state and more oxygen vacancies, thus promoting the reactant adsorption and oxygen activation and enhancing the final oxidation activity. The oxidation of 5-hydroxymethyl-2-furancarboxylic acid to FDCA was determined as the rate-determining step in the oxidation of BHMF over the Au/CeO2 catalyst.

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使用形态依赖性 Au/CeO2 催化剂将 2,5-双(羟甲基)呋喃氧化为 2,5-呋喃二甲酸
2,5-呋喃二甲酸(FDCA)是一种具有硬环的生物基二酸,其结构与石油基对苯二甲酸相似。它与乙二醇的共聚酯具有优异的热性能和机械性能。本文开发了一种富氧空位的 Au/CeO2-rod 催化剂,可在温和条件下将 2,5-双(羟甲基)呋喃 (BHMF) 高效氧化为 FDCA,收率达 92%。CeO2-rod 的大比表面积有利于更好地分散金纳米粒子。同时,Au/CeO2-rod 的高活性可归因于棒状 CeO2 暴露了更多的活性(100)面,从而导致 Au 纳米颗粒与 CeO2-rod 之间产生强烈的金属支撑相互作用。这可以产生更多氧化态的金物种和更多的氧空位,从而促进反应物的吸附和氧活化,提高最终的氧化活性。5-hydroxymethyl-2-furancarboxylic acid 氧化成 FDCA 被确定为 Au/CeO2 催化剂氧化 BHMF 的速率决定步骤。
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来源期刊
Applied Catalysis A: General
Applied Catalysis A: General 化学-环境科学
CiteScore
9.00
自引率
5.50%
发文量
415
审稿时长
24 days
期刊介绍: Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications. Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.
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