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使用由生物质衍生配体构建的镍金属有机框架从塑料废料中选择性电催化生产甲酸。

Selective Electrocatalytic Production of Formic Acid from Plastic Waste Using a Nickel Metal-Organic Framework Constructed from a Biomass-Derived Ligand.

作者信息

Das Satarupa, Zhang Ting, Clarkson Guy J, Walker Marc, Qian Xufang, Long Xia, Zhao Yixin, Walton Richard I

机构信息

Department of Chemistry, University of Warwick, Gibbet Hill Road, Coventry, CV4 7AL, UK.

School of Environmental Science and Engineering, Frontiers Science Center for Transformative Molecules, Shanghai Jiao Tong University, Shanghai, 200240, China.

出版信息

ChemSusChem. 2025 Apr 14;18(8):e202402319. doi: 10.1002/cssc.202402319. Epub 2024 Dec 12.

Abstract

A novel nickel-based metal organic framework (MOF) Ni(FDC)(CHOH)(HO) (UOW-6) utilizing biomass-derived 2,5-furan dicarboxylate (FDC) as a ligand is reported as an electrocatalyst for anodic ethylene glycol (EG) oxidation with cathodic hydrogen evolution. The MOF structure was analyzed using single crystal X-ray-diffraction, thermogravimetric analysis (TGA) and thermodiffractometry, to establish its structure and verify phase purity. The material was dropcast on carbon fiber paper as a catalyst, and by using a three-electrode system, UOW-6 requires only 1.47 V to attain a current density of 50 mA cm. During oxidation of the EG, UOW-6 shows unprecedented selectivity towards formic acid with a Faradaic efficiency of 94 % and remarkable stability over 20 days. The combination of electrochemical measurements and in situ Raman confirmed in situ formed NiOOH at the surface of UOW-6 as the catalytically active sites for EG oxidation. This work not only presents a pioneering application of FDC-based MOFs for polyethylene terephthalate (PET) upcycling but also underscores the potential of electrocatalysis in advancing sustainable plastic valorization strategies.

摘要

报道了一种新型镍基金属有机框架(MOF)Ni(FDC)(CHOH)(HO)(UOW-6),它利用生物质衍生的2,5-呋喃二甲酸酯(FDC)作为配体,作为用于阳极乙二醇(EG)氧化和阴极析氢的电催化剂。使用单晶X射线衍射、热重分析(TGA)和热衍射法对MOF结构进行了分析,以确定其结构并验证相纯度。将该材料滴铸在碳纤维纸上作为催化剂,通过使用三电极系统,UOW-6仅需1.47 V即可达到50 mA cm的电流密度。在EG氧化过程中,UOW-6对甲酸表现出前所未有的选择性,法拉第效率为94%,并且在20多天内具有显著的稳定性。电化学测量和原位拉曼光谱相结合证实,UOW-6表面原位形成的NiOOH是EG氧化的催化活性位点。这项工作不仅展示了基于FDC的MOF在聚对苯二甲酸乙二酯(PET)升级循环方面的开创性应用,还强调了电催化在推进可持续塑料增值策略方面的潜力。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/9ea5/11997925/5ded4721db89/CSSC-18-e202402319-g001.jpg

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