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将聚对苯二甲酸乙二酯废料绿色转化为定制用于催化还原4-硝基苯酚的功能化铜-金属有机框架材料。

Green valorization of PET waste into functionalized Cu-MOF tailored to catalytic reduction of 4-nitrophenol.

作者信息

Ebrahimi Farshchi Mahdi, Madadian Bozorg Negar, Ehsani Atefeh, Aghdasinia Hassan, Chen Zhijie, Rostamnia Sadegh, Ni Bing-Jie

机构信息

Department of Chemical Engineering, Faculty of Chemical and Petroleum Engineering, University of Tabriz, 51666-16471 Tabriz, Iran.

Department of Chemical Engineering, Faculty of Chemical and Petroleum Engineering, University of Tabriz, 51666-16471 Tabriz, Iran.

出版信息

J Environ Manage. 2023 Nov 1;345:118842. doi: 10.1016/j.jenvman.2023.118842. Epub 2023 Aug 22.

Abstract

Metal-organic frameworks (MOFs) are attractive functional materials due to their high surface area, high porosity, and flexible compositions. However, the high precursor cost and complex synthetic processes hinder their large-scale applications. Herein, a novel green approach has been developed toward the synthesis of Cu-based MOF by a solvent-free mechano-synthesis method and utilizing consumed polyethylene terephthalate (PET)-derived benzenedicarboxylate (BDC) as the linker. The as-prepared CuBDC and aminated CuBDC (CuBDC-NH) act as green catalysts for the reduction of deleterious 4-nitrophenol (4-NP) into the value-added 4-aminophenol (4-AP). Compared with CuBDC, CuBDC-NH shows increased adsorption capability and reduction efficiency. The mechanism and thermodynamic studies suggest that the adsorption of 4-NP on CuBDC-NH is an endothermic, spontaneous, favorable, and physical adsorption process. Furthermore, CuBDC-NH can expedite the reduction of 4-NP by participating in an adsorptive catalytic process. With the CuBDC-NH catalyst, the catalytic normalized kinetic rate of 4-NP was achieved 11.28 mol/min. mg, outperforming state-of-the-art catalysts, and a complete reduction occur in 5 min for a concentrated effluent (200-ppm 4-NP). The plastic waste-derived MOF-mediated catalytic valorization of organic pollutants demonstrated here opens an avenue for the green recycling/utilization of plastic waste, providing meaningful insights into the sustainable management of organic pollutants in wastewater.

摘要

金属有机框架材料(MOFs)因其高比表面积、高孔隙率和灵活的组成而成为有吸引力的功能材料。然而,前驱体成本高和合成过程复杂阻碍了它们的大规模应用。在此,通过无溶剂机械合成方法并利用消耗的聚对苯二甲酸乙二酯(PET)衍生的苯二甲酸(BDC)作为连接体,开发了一种新颖的绿色方法来合成铜基MOF。所制备的CuBDC和胺化CuBDC(CuBDC-NH)作为绿色催化剂,用于将有害的4-硝基苯酚(4-NP)还原为增值的4-氨基苯酚(4-AP)。与CuBDC相比,CuBDC-NH表现出更高的吸附能力和还原效率。机理和热力学研究表明,4-NP在CuBDC-NH上的吸附是一个吸热、自发、有利的物理吸附过程。此外,CuBDC-NH可以通过参与吸附催化过程来加速4-NP的还原。使用CuBDC-NH催化剂,4-NP的催化归一化动力学速率达到11.28 mol/min·mg,优于现有催化剂,对于浓缩废水(200 ppm 4-NP),5分钟内即可完全还原。本文展示的塑料废物衍生的MOF介导的有机污染物催化增值为塑料废物的绿色回收/利用开辟了一条途径,为废水中有机污染物的可持续管理提供了有意义的见解。

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