Membrane-free sequential paired electrosynthesis of 1,4-hydroquinone from phenol over a self-supported electrocatalytic electrode

Wei-Ling Zhang, Ya-Jing Li, Yingchun He, Shao Zhang, Haohong Li, Huidong Zheng, Qi-Long Zhu
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Abstract

Sequential paired electrosynthesis capable of the production of organic chemicals through a series of electrochemical reactions that occur consecutively and in pairs are of high significance. Herein, a three-dimensional porous carbon felt-loaded PbO2 electrode (PbO2/CF) with a self-supported nanostructure was fabricated using a double-cathode electrodeposition method, which served as an efficient electrocatalyst enabling the unique sequential paired electrosynthesis of 1,4-hydroquinone (1,4-HQ) from phenol in a membrane-free electrolytic cell. In such an exotic paired electrolysis system, phenol is first oxidized to p-benzoquinone at the anode, which is subsequently reduced to 1,4-HQ at the cathode. The as-obtained PbO2/CF electrode exhibited a remarkable electrochemical performance, achieving impressive conversion and selectivity of 94.5% and 72.1%, respectively, for the conversion of phenol to 1,4-HQ. This exceptional performance can be attributed to the open porous self-supported structure of the PbO2/CF electrode, which improves the active site exposure and substrate adsorption capability and reduces mass and charge transfer resistance. Furthermore, the catalyst electrode well maintained its structure integrity even after 140 hours of long-term use, further highlighting its promising application for the electrosynthesis of 1,4-HQ. Moreover, this sequential paired electrosynthesis strategy can be further extended to other substrates with electron-withdrawing/donating groups over the PbO2/CF electrode. The proof of concept in this innovative sequential paired electrosynthesis could provide a sustainable and efficient way to produce various desired organic compounds.

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在自支撑电催化电极上以苯酚为原料进行无膜顺序配对电合成 1,4-氢醌
通过一系列成对连续发生的电化学反应生产有机化学品的顺序配对电合成具有重要意义。本文采用双阴极电沉积法制备了一种具有自支撑纳米结构的三维多孔碳毡负载 PbO2 电极(PbO2/CF),并将其作为一种高效电催化剂,在无膜电解池中以苯酚为原料进行了独特的 1,4-hydroquinone (1,4-HQ) 顺序配对电合成。在这种奇特的成对电解系统中,苯酚首先在阳极被氧化成对苯醌,然后在阴极被还原成 1,4-HQ。获得的 PbO2/CF 电极表现出卓越的电化学性能,将苯酚转化为 1,4-HQ 的转化率和选择性分别达到 94.5% 和 72.1%,令人印象深刻。这种优异的性能归功于 PbO2/CF 电极的开放式多孔自支撑结构,它改善了活性位点的暴露和底物吸附能力,降低了质量和电荷转移阻力。此外,催化剂电极在长期使用 140 小时后仍能很好地保持其结构完整性,这进一步凸显了其在 1,4-HQ 电合成中的应用前景。此外,这种顺序配对电合成策略还可进一步扩展到 PbO2/CF 电极上其他具有电子吸收/捐献基团的基质。这种创新的序贯配对电合成的概念验证可为生产各种所需有机化合物提供一种可持续的高效方法。
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Industrial Chemistry & Materials
Industrial Chemistry & Materials chemistry, chemical engineering, functional materials, energy, etc.-
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期刊介绍: Industrial Chemistry & Materials (ICM) publishes significant innovative research and major technological breakthroughs in all aspects of industrial chemistry and materials, with a particular focus on the important innovation of low-carbon chemical industry, energy and functional materials. By bringing researchers, engineers, and policymakers into one place, research is inspired, challenges are solved and the applications of science and technology are accelerated. The global editorial and advisory board members are valued experts in the community. With their support, the rigorous editorial practices and dissemination ensures your research is accessible and discoverable on a global scale. Industrial Chemistry & Materials publishes: ● Communications ● Full papers ● Minireviews ● Reviews ● Perspectives ● Comments
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Back cover Membrane-free sequential paired electrosynthesis of 1,4-hydroquinone from phenol over a self-supported electrocatalytic electrode Back cover Toward a low-cost uranium-adsorbing material based on nonwoven fabrics and photografting technology Depolymerization of PET with Ethanol by Homogeneous Iron Catalysts Applied for Exclusive Chemical Recycling of Cloth Waste
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