Bidirectional S-bridge coordination in the magnetic Au/FeOxSy catalyst for the catalytic oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid†

IF 9.5 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Journal of Materials Chemistry A Pub Date : 2025-03-18 DOI:10.1039/D4TA09277E
Yu Ruan, Shaoyi Wu, Yingxin Lu, Tiefeng Xu, Wenxing Chen and Wangyang Lu
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Abstract

The aerobic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) is a promising approach for producing renewable biodegradable plastics. However, thus far, the development of catalytic oxidation processes operating under mild conditions and the design of highly stable catalysts have been challenging. Herein, the magnetic catalyst Au/FeOxSy was synthesised by doping S into the Fe/Au bimetallic structure. The reaction was conducted in water at 60 °C under air and atmospheric pressure, achieving 100% conversion of HMF and a FDCA yield of 98.5%. The catalytic performance of S-doping Au/FeOx was 4.73 times greater than that of undoped Au/FeOx under the same conditions. Furthermore, the catalyst demonstrated excellent cycling stability, with the FDCA yield maintained above 93% after at least 30 cycles. The introduction of S altered the electronic configuration of Au through the formation of Au–S bonds, thereby enhancing electron mobility and catalytic activity. Additionally, the interaction of S with FeOx led to the formation of Fe–O–S bonds, which fortified the structure of the catalyst and ensured prolonged cycling stability. Thus, this study effectively converted HMF to FDCA under mild conditions through S incorporation, offering a novel approach for preparing metal catalysts and laying a robust foundation for utilising FDCA as a sustainable alternative to terephthalic acid in bio-based polyester production.

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磁性Au/FeOxSy催化剂中双向s桥配位催化5-羟甲基糠醛氧化为2,5-呋喃二羧酸
5-羟甲基糠醛(HMF)的好氧氧化制2,5-呋喃二羧酸(FDCA)是生产可再生生物降解塑料的一种很有前途的方法。然而,到目前为止,在温和条件下的催化氧化过程的开发和高稳定性催化剂的设计一直具有挑战性。本文通过在Fe/Au双金属结构中掺杂S,合成了Au/FeOxSy磁性催化剂。反应在空气和常压下60℃的水中进行,HMF转化率达到100%,FDCA收率为98.5%。在相同条件下,s掺杂Au/FeOx的催化性能是未掺杂Au/FeOx的4.73倍。此外,该催化剂表现出优异的循环稳定性,至少30次循环后,FDCA收率保持在93%以上。S的引入通过形成Au - S键改变了Au的电子构型,从而提高了电子迁移率和催化活性。此外,S与FeOx的相互作用导致Fe-O-S键的形成,强化了催化剂的结构,确保了长时间的循环稳定性。因此,本研究通过S的掺入,在温和条件下有效地将HMF转化为FDCA,为制备金属催化剂提供了一种新的方法,并为FDCA作为对苯二甲酸在生物基聚酯生产中的可持续替代品奠定了坚实的基础。
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来源期刊
Journal of Materials Chemistry A
Journal of Materials Chemistry A CHEMISTRY, PHYSICAL-ENERGY & FUELS
CiteScore
19.50
自引率
5.00%
发文量
1892
审稿时长
1.5 months
期刊介绍: The Journal of Materials Chemistry A, B & C covers a wide range of high-quality studies in the field of materials chemistry, with each section focusing on specific applications of the materials studied. Journal of Materials Chemistry A emphasizes applications in energy and sustainability, including topics such as artificial photosynthesis, batteries, and fuel cells. Journal of Materials Chemistry B focuses on applications in biology and medicine, while Journal of Materials Chemistry C covers applications in optical, magnetic, and electronic devices. Example topic areas within the scope of Journal of Materials Chemistry A include catalysis, green/sustainable materials, sensors, and water treatment, among others.
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