Ultrarapid and Sustainable Synthesis of Trimetallic-Based MOF (CrNiFe-MOF) from Stainless Steel and Disodium Terephthalate-Derived PET Wastes

材料科学 吸附 金属有机骨架 化学工程 磷酸盐 水溶液中的金属离子 无机化学 金属 核化学 有机化学 冶金 化学 工程类
作者
Khaireddin Boukayouht,Loubna Bazzi,Ayoub Daouli,Guillaume Maurin,Samir El Hankari
出处
期刊:ACS Applied Materials & Interfaces [American Chemical Society]
卷期号:16 (2): 2497-2508 被引量:24
标识
DOI:10.1021/acsami.3c15669
摘要

Designing easy and sustainable strategies for the synthesis of metal–organic frameworks (MOFs) from organic and inorganic wastes with the efficient removal of phosphate from water remains a challenge. The majority of the reported works have utilized costly precursors and nonsoluble ligands for the synthesis of MOFs. Herein, we have developed a low-cost, simple, and sustainable alternative approach using the coprecipitation method in water at room temperature for the synthesis of a new adsorbent-based trimetallic MOF. Poly(ethylene terephthalate) and stainless steel wastes were used as sources of water-soluble disodium terephthalate ligand and three metallic species (chromium, nickel, and iron salts) for the fabrication of trimetallic MOF (CrNiFe-MOF), respectively. The newly developed MOF demonstrates a superior space-time yield of 5760 g m–3 day–1, reaching a level allowing the industrialization production of this sustainable MOF. The scanning electron microscopy and adsorption studies revealed that the developed trimetallic MOF consists of aggregated nanoparticles and the presence of defective as well as mesoporous structures. This MOF showed an enhanced adsorption capacity of phosphate from real eutrophic water samples and higher stability in a range of pHs. The density functional theory calculations evidenced that the phosphate ions preferentially adsorb over H2O toward the metal oxo-trimers, with the adsorption energies increasing from H3PO4 to PO43– species in line with an improvement of the adsorption performance of CrNiFe-MOF when the pH increases, i.e., when HPO42– and PO43– become more predominant. These calculations also supported that the incorporation of Cr metal sites in the oxo-trimer is expected to boost the phosphate affinity of the MOF. Finally, our work provides an easy and eco-friendly approach for MOF designing to enhance phosphate removal from water.
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