使用新型双金属-有机框架吸附剂协同增强全氟辛酸的捕获

IF 4.1 2区材料科学 Q2 ENGINEERING, CHEMICAL

Particuology Pub Date : 2025-02-01 DOI:10.1016/j.partic.2024.12.009

Heng Lin , Zhouheng Xia , Kunpeng Xue , Xiaojing Zhou , Yifan Yao , Na Ma , Wei Dai

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引用次数: 0

摘要

金属有机骨架（MOF）作为去除全氟辛酸（PFOA）的潜在吸附剂受到了广泛关注。然而，单组分MOF通常在吸附能力、功能和孔隙结构方面存在局限性。因此，我们创新地设计并合成了一种双金属核壳型MOF复合吸附剂MIL-101(Cr)@ZIF-8（一种铬锌双金属MOF， CZDM），该吸附剂对水溶液中PFOA具有优异的吸附去除性能。结果表明，CZDM复合材料具有较高的比表面积（2091 m2/g），孔隙结构为典型的微孔（~ 1.16 nm）和介孔（~ 3.4 nm），这是有效吸附PFOA的关键。SEM和TEM图像显示，CZDM具有均匀的核壳形态，以MIL-101（Cr）为核，ZIF-8为壳，保持了稳定完整的结构。EDX分析进一步证实了Cr和Zn元素的成功掺入。批量实验考察了温度、溶液pH和PFOA浓度对吸附效率的影响。结果表明，CZDM-3吸附剂在较宽的pH范围内具有快速的吸附动力学和良好的PFOA去除效率。CZDM优越的吸附性能是由于双金属活性位点、优化的孔结构、静电相互作用和配位键的协同作用。对PFOA的最大吸附容量达到625.5 mg/g，在60 min内达到平衡，优于一些相关的吸附剂。吸附过程的实验数据符合Langmuir吸附等温线和拟二级动力学模型，表明吸附过程是自发的、吸热的，并且伴随着熵的增加。值得注意的是，即使经过5次循环，CZDM材料对PFOA的去除效率仍然很高。本研究提出了一种新的MOF@MOF合成策略，CZDM在去除水中PFOA方面具有潜在的应用前景。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

Synergistically enhanced capture of perfluorooctanoic acid using a novel dual metal-organic framework adsorbent

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Synergistically enhanced capture of perfluorooctanoic acid using a novel dual metal-organic framework adsorbent

Metal-Organic Framework (MOF) have gained widespread attention as potential adsorbents for the removal of perfluorooctanoic acid (PFOA). However, single-component MOF often exhibit limitations in adsorption capacity, functionality, and pore structure. Hereby, we innovatively designed and synthesized a dual-metal core-shell MOF composite adsorbent, MIL-101(Cr)@ZIF-8 (a chromium-zinc bimetallic MOF, CZDM), which exhibits an excellent adsorption removal performance of PFOA from aqueous solutions. The results showed that the CZDM composite material has a high specific surface area (2091 m²/g), with pore structures exhibiting typical micropores (∼1.16 nm) and mesopores (∼3.4 nm), which are crucial for the efficient adsorption of PFOA. SEM and TEM images revealed that CZDM has a uniform core-shell morphology, with MIL-101(Cr) as the core and ZIF-8 as the shell, maintaining a stable and intact structure. EDX analysis further confirmed the successful incorporation of Cr and Zn elements. Batch experiments evaluated the effects of temperature, solution pH, and PFOA concentration on adsorption efficiency. The results demonstrated that the CZDM-3 adsorbent exhibited rapid adsorption kinetics and good PFOA removal efficiency across a wide pH range. The superior adsorption performance of CZDM is attributed to the synergistic effect of the dual-metal active sites, optimized pore structure, electrostatic interactions, and coordination bonds. The maximum adsorption capacity for PFOA reached 625.5 mg/g, with equilibrium achieved within 60 min, outperforming some related reported adsorbents. The experimental data of the adsorption process fit well with both Langmuir adsorption isotherms and pseudo-second-order kinetics models, indicating that the adsorption process is spontaneous, endothermic, and accompanied by an increase in entropy. Notably, even after five cycles, the CZDM material maintained high removal efficiency toward PFOA. This study advances a new synthesizing strategy of the MOF@MOF, and the CZDM exhibits a potential application in PFOA elimination from water.

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来源期刊

Particuology 工程技术-材料科学：综合

CiteScore

6.70

自引率

2.90%

发文量

1730

审稿时长

32 days

期刊介绍： The word ‘particuology’ was coined to parallel the discipline for the science and technology of particles. Particuology is an interdisciplinary journal that publishes frontier research articles and critical reviews on the discovery, formulation and engineering of particulate materials, processes and systems. It especially welcomes contributions utilising advanced theoretical, modelling and measurement methods to enable the discovery and creation of new particulate materials, and the manufacturing of functional particulate-based products, such as sensors. Papers are handled by Thematic Editors who oversee contributions from specific subject fields. These fields are classified into: Particle Synthesis and Modification; Particle Characterization and Measurement; Granular Systems and Bulk Solids Technology; Fluidization and Particle-Fluid Systems; Aerosols; and Applications of Particle Technology. Key topics concerning the creation and processing of particulates include: -Modelling and simulation of particle formation, collective behaviour of particles and systems for particle production over a broad spectrum of length scales -Mining of experimental data for particle synthesis and surface properties to facilitate the creation of new materials and processes -Particle design and preparation including controlled response and sensing functionalities in formation, delivery systems and biological systems, etc. -Experimental and computational methods for visualization and analysis of particulate system. These topics are broadly relevant to the production of materials, pharmaceuticals and food, and to the conversion of energy resources to fuels and protection of the environment.