生物模型5-羟甲基糠醛的催化电化学氧化,以实现循环塑料经济

IF 23.5 1区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR
Weijin Cao, Changlong Wang, Zhiyan Hou, Yufeng Wu, Didier Astruc
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引用次数: 0

摘要

电化学氧化已成为合成2,5-呋喃二羧酸(FDCA)的关键绿色技术。作为美国能源部优先考虑的生物基平台分子,FDCA作为石油衍生对苯二甲酸的可持续替代品,促进了向循环塑料经济的过渡。传统的5-羟甲基糠醛(HMF)氧化依赖于高温高压条件,能耗大,环境不利。相比之下,电化学氧化可以通过六电子转移过程将羟甲基和乙基有效地转化为羧基,使其成为迅速发展的研究热点。本综述系统地考察了该领域的关键进展。它区分了直接氧化和间接氧化途径:直接氧化维持稳定的催化剂价态,而间接氧化利用氧化还原介质进行电子转移。阐明了电解质pH、组成和底物浓度对产物选择性的调节机制。提出了调节催化性能的策略,包括活性金属类型、尺寸、支撑和配位环境的优化。结合缺陷工程、应变调节和掺杂技术,这些方法显著提高了催化效率和FDCA选择性。此外,将该过程与析氢或CO2还原反应配对可以降低电解电压并提高能量转换效率。通过生命周期评价,分析了技术经济可行性和环境效益。工业化面临的关键挑战包括在碱性条件下抑制非法拉第生物量降解和开发高效反应器。最后,强调了跨学科合作的重要性。未来的工作应优先考虑先进的催化剂设计、精确的反应条件控制和工艺规模优化,以弥合实验室研究与工业生产之间的差距。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Catalytic electrochemical oxidation of a bio-model, 5-hydroxymethyl furfural, toward a circular plastic economy
Electrochemical oxidation has emerged as a pivotal green technology for synthesizing 2,5-furandicarboxylic acid (FDCA). As a bio-based platform molecule prioritized by the U.S. Department of Energy, FDCA serves as a sustainable alternative to petroleum-derived terephthalic acid, facilitating the transition toward a circular plastic economy. Traditional oxidation of 5-hydroxymethylfurfural (HMF) relies on high-temperature and high-pressure conditions, resulting in significant energy consumption and environmental drawbacks. In contrast, electrochemical oxidation enables efficient conversion of hydroxymethyl and aldehyde groups to carboxyl groups through a six-electron transfer process, making it a rapidly growing research focus. This review systematically examines key advancements in the field. It distinguishes between direct and indirect oxidation pathways: direct oxidation maintains stable catalyst valence states, while indirect oxidation employs redox mediators for electron transfer. The regulatory mechanisms of electrolyte pH, composition, and substrate concentration on product selectivity are elucidated. Strategies for modulating catalytic performance are proposed, including active metal type, size, support, and coordination environment optimization. Combined with defect engineering, strain regulation, and doping techniques, these approaches significantly enhance catalytic efficiency and FDCA selectivity. Furthermore, pairing this process with hydrogen evolution or CO2 reduction reactions reduces electrolysis voltage and improves energy conversion efficiency. Through life cycle assessment, the article analyzes techno-economic viability and environmental benefits. Critical challenges for industrialization are identified, including suppressing non-Faradaic biomass degradation under alkaline conditions and developing efficient reactors. Finally, the importance of interdisciplinary collaboration is emphasized. Future efforts should prioritize advanced catalyst design, precise reaction condition control, and process scale-up optimization to bridge the gap between laboratory research and industrial production.
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来源期刊
Coordination Chemistry Reviews
Coordination Chemistry Reviews 化学-无机化学与核化学
CiteScore
34.30
自引率
5.30%
发文量
457
审稿时长
54 days
期刊介绍: Coordination Chemistry Reviews offers rapid publication of review articles on current and significant topics in coordination chemistry, encompassing organometallic, supramolecular, theoretical, and bioinorganic chemistry. It also covers catalysis, materials chemistry, and metal-organic frameworks from a coordination chemistry perspective. Reviews summarize recent developments or discuss specific techniques, welcoming contributions from both established and emerging researchers. The journal releases special issues on timely subjects, including those featuring contributions from specific regions or conferences. Occasional full-length book articles are also featured. Additionally, special volumes cover annual reviews of main group chemistry, transition metal group chemistry, and organometallic chemistry. These comprehensive reviews are vital resources for those engaged in coordination chemistry, further establishing Coordination Chemistry Reviews as a hub for insightful surveys in inorganic and physical inorganic chemistry.
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