MOFs基材料用于环境污染控制文献整理（2024.9.7-9.13)

文摘 2024-09-16 07:24 土耳其

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为较全面地展示MOFs材料在环境污染控制领域的研究进展并服务于同行，NMTer课题组每周收集整理“MOFs基材料用于环境污染控制”方面的文献资料，通过“MOFs帮助环境”公众号推送。欢迎各位老师和同学关注！同时，欢迎各位老师将您的相关成果在本公众号做专题推送宣传。“赠人玫瑰，手有余香”！

题目：Recent progress on organic metal compound/MOF hybrids: From controllable synthesis to potential catalytic applications

作者：Yahya Absalan*, Mostafa Gholizadeh, Eun-Bi Kim, Sadia Ameen*, Yousheng Wang*,

Yudi Wang*, Hongming He*

摘要：The desire for functional materials with unique and excellent performance has led to many researchers to prepare new composites. Organic–metal compounds (OMCs), including polyoxometalates, coordination complexes, and organometals, belong to a class of organic and inorganic hybrid materials, which have been widely used in a large variety of industries. On the other hand, metal–organic frameworks (MOFs) as crystalline organic–inorganic materials have attracted lots of attentions in various applications. MOFs also can be considered as a polymeric type of OMCs. The rich porous structure and high specific surface area of MOFs provide a good platform to incorporate OMCs as guest species into matrix MOFs. The OMC/MOF hybrids keep their original characteristics and overcome the drawbacks of individual components through synergy and effective combination. In this review, we systematically and comprehensively summarize the development status of relevant fields in recent years, including hybrid methods, synthetic techniques, advanced catalytic applications, conclusion and perspectives. This review can provide a systematic summary for readers and enable them to quickly understand the development status of OMC@MOF hybrids. And it can provide a platform to further consider how to promote the development of this field in the future.

期刊信息：Coord. Chem. Rev.

DOI：10.1016/j.ccr.2024.215972

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题目：Transformation of europium metal-organic framework from 3D via 2D into exfoliating 3D for enzyme immobilization

作者：Ani Vardanyan*, Guojun Zhou, Nayoung Kim, Tetyana M. Budnyak, Vadim G. Kessler, Insung S. Choi, Zhehao Huang & Gulaim A. Seisenbaeva*

摘要：Metal-organic frameworks (MOFs) have emerged as highly promising materials for hosting functional biomolecules. Here, a 1,2,4-benzenetricarboxylate ligand with a flat asymmetric shape is applied to infuse an unusual behavior to a 3D europium MOF (SLU-1). Solvent addition results in the 3D MOF splitting into a 2D one (SLU-2), and in the presence of excess water, gets cross-linked into a different 3D MOF (SLU-3) prone to spontaneous exfoliation. SLU-3 features a combination of highly hydrophilic and hydrophobic spots and serves as an attractive host for incorporating large active species. As a representative demonstration, horseradish peroxidase (HRP) is incorporated into the exfoliated 3D-layered structure by simple mixing, and secured by an outer silica layer in the form of core-shell structures. The resulting HRP-based biocatalyst exhibited enhanced stability and reusability, effectively degrading phenol. This work showcases the potential of reconfigurable MOFs, offering upheld applications through the controlled uptake and retention of biocatalytic agents.

期刊信息：Commun. Mater.

DOI：10.1038/s43246-024-00624-y

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题目：Consolidating CQDs with NiFe-MOF photo-Fenton membranes to effectively treat wastewater containing antibiotics and antibiotic-resistant bacteria

作者：Haiyi Jin, Wangyi Zhou, Zhenyu Guo, Hailiang Xu, Xiaoli Zhong, Tai-Shung Chung, Die Ling Zhao*, Hongjun Lin*

摘要：The escalating presence of antibiotics and antibiotic-resistant bacteria in wastewater poses a pressing threat to both human health and ecosystems. Addressing this challenge requires innovative approaches while photocatalytic membranes emerge as promising solutions because they offer multiple functions to separate and degrade/sterilize antibiotics and antibiotic-resistant bacteria simultaneously. In this study, we for the first time developed in-situ grown Ni-Fe metal–organic framework/carbon quantum dot (NiFe-MOF/CQD) membranes with NiFe-MOF seeds pre-integrated into the substrates. The incorporation of CQDs not only enhances the hydrophilicity and integrity of NiFe-MOF membranes that resulting in both a high water flux of 119.7 L m⁻²h⁻¹ bar⁻¹ and a high antibiotic rejection of 98.1 % to rifampicin, but also promotes the photo-Fenton activity by enhancing the visible light absorption and photoelectrons (e⁻)-holes (h⁺) separation. Therefore, the degradation efficiency of rifampicin in a photo-Fenton system within 100 min by NiFe-MOF/CQD composites (84.9 %) surpasses that of NiFe-MOFs (63.1 %). Additionally, NiFe-MOF/CQDs can effectively inactivate both Gram-negative and Gram-positive bacteria in the photo-Fenton system. The supreme separation performance of NiFe-MOF/CQD membranes and photo-Fenton activity of NiFe-MOF/CQDs underscore the significant potentials of the newly invented photocatalytic membranes in treating wastewater containing antibiotic and antibiotic-resistant bacteria.

期刊信息：Chem. Eng. J.

DOI：10.1016/j.cej.2024.155740

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题目：A pH-responsive MOFs@MPN nanocarrier with enhancing antifungal activity for sustainable controlling myclobutanil release

作者：Yushan Hou, Yaowei Zhang, Yanyan Huang, Ailing Zhou, Jiatong Han, Kexin Yang, Yiming Zhao, Jie Zhou, Jing Wang*, Ge Chen, Xiaomin Xu, Donghui Xu*, Jun Lv, Jing Chen, Honghao Lv, Guangyang Liu *

摘要：The pH-responsive metal–organic framework (MOF) nanocarriers for sustainable controlled release of pesticides is promising in agricultural production owing to their long duration, high loading efficiency and antimicrobial activity. In this work, myclobutanil (MYC) was loaded into an Ag-based MOF (Ag-TCPP), and modified with a metal-phenolic network (MPN) via in-situ polymerization to construct a pH-responsive nano-delivery system (Ag-TCPP@MYC@MPN). Ag-TCPP@MYC@MPN presented a disordered nanoflower structure and many active sites with potential enhanced loading activity. The cumulative release rates of nanoparticles at pH 4.96, 7.5, and 8.5 were 52.6 %, 62.6 % and 80.0 %, respectively. Hence, Ag-TCPP@MYC@MPN has slow release rate and pH responsiveness. The antifungal activity of Ag-TCPP@MYC@MPN was significantly enhanced, and the bacteriostatic rate reached 81.8 %. This enhancement may be attributed to the synergistic antibacterial effect between tannic acid and Ag⁺. Safety experiments showed the nanoparticles had no inhibitory effect on the germination of Pakchoi seeds, and the pesticide residues of Ag-TCPP@MYC@MPN did not exceed the food safety standards. This work offers a new potential to develop improved responsive stimulus nanocarriers for sustainable controlled release of MYC.

期刊信息：Chem. Eng. J.

DOI：10.1016/j.cej.2024.155713

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题目：Sustainability and photocatalytic performance of MOFs: Synthesis strategies and structural insights

作者：Zeshan Ali Sandhu, Umme Farwa, Muhammad Danish, Muhammad Asam Raza*, Aqib Talib, Hifza Amjad, Rukhmah Riaz, Abdullah G. Al-Sehemi

摘要：In the pursuit for sustainable and efficient photocatalyst, Metal-organic frameworks (MOFs) have developed as fascinating materials with remarkable potential for photocatalytic applications. Despite numerous research, certain challenges are still remained in their sustainability and catalysis applications. The physicochemical properties of MOFs, impacted their photocatalytic effect, as well as issues related to synthetic approaches. This work aims to address these gaps by investigating the synthetic strategies and structural modifications of MOFs to enhance their photocatalytic excellence. MOFs have attained consideration in the process of striving for a green synthetic method. The use of green synthesis approaches, depicted the use of renewable precursors and clean solvents, is a key factor in the successful development and improvement of MOFs. By employing the combination of advanced synthetic methods, solvothermal and post-synthetic modifications, this work will explore the impacts of these methods on the structural and photocatalytic performance. Such materials possess the facile nature that triggers the invention of devices with inflexible and efficient photocatalytic performance by manipulating light absorption, separation of charges, and catalytic activity. This work focuses on highlighting the most recent updates in the synthesis processes of MOFs, with an eye on their sustainability and possible impact on the structure characteristics, especially with attention to photocatalysis.

期刊信息：J. Cleaner Prod.

DOI：10.1016/j.jclepro.2024.143263

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题目：Synthesis of a novel cost-effective double-ligand Zr-based MOF via an inverted modulator strategy towards enhanced adsorption and photodegradation of tetracycline

作者：Haixia Tong, Ruidong He, Gao Chen, Zhuo Tong, Mingming Dang, Junhua Li, Daoxin Wu*, Dong Qian*

摘要：Developing visible-light response photocatalysts with high activity and adsorption alongside sustainability is vitally important to environmental restoration. Here, we fabricated a novel metal organic framework (MOF) with cost-effective double-ligands (fumaric acid and 2-aminoterephthalic acid as ligand precursors, denoted as MA-MOF) via a facile solvothermal method. Specifically, crystalline [Zr₆O₄(OH)₄(fumarate)₆] (MOF-801) can be only formed with monocarboxylic acids as modulators. Therefore, in the construction of crystalline double-ligand MA-MOF, the absence of monocarboxylic acid modulators successfully prevents the formation of crystalline MOF-801. Instead, the crystalline double-ligand MA-MOF is formed. Properties of MA-MOFs including the surface area, porosity, charge transfer resistance, and energy level position can be adjusted via altering the ratio of ligands. The optimal sample, MA-MOF₂ (prepared with a molar ratio of fumaric acid and 2-aminoterephthalic acid being 2:1), shows a total 94.6% removal of tetracycline via adsorption and photodegradation, far exceeding the corresponding single-ligand counterparts. This work proposes an innovative inverted modulator strategy for constructing double-ligand MOFs.

期刊信息：J. Colloid. Interf. SCI

DOI：10.1016/j.jcis.2024.05.211

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题目：Adsorption and catalytic degradation by CoFe₂O₄ coated on metal–organic framework for the removal of 4-nitrophenol and 2,4-dichlorophenol

作者：Xiaxi Zhang*, Fen Wei*, Sicen Wang*

摘要：4-nitrophenol (4-NP) and 2,4-dichlorophenol (2,4-DCP) contaminated wastewater have attracted attention for their genotoxic and carcinogenic hazards. The magnetic MIL-101/CFO was constructed by synergistically integrating porous/hydrophilic/π-conjugated MIL-101(Cr) and CoFe₂O₄. The nanocomposites markedly accelerated the catalytic reaction activity. The BET characterizations reveal the nanocomposites had a larger specific surface area and pore volume in comparison to the individual CoFe₂O₄. The composite was employed to evaluate the adsorption and peroxymonosulfate (PMS)-activated ability of 4-NP and 2,4-DCP elimination. The adsorption equilibrium could be achieved within 60 min, following the pseudo-second-order kinetic model and the Langmuir isotherm model. The nanocomposites (0.2 g·L⁻¹) achieved exceeding 96 % decomposition efficiencies toward 4-NP and 2,4-DCP (0.1 g·L⁻¹) after 15 min by PMS (5.29 mM) activation. Notably, the reaction system displayed effective catalytic performance across pH 5 − 11 and resistance to the existence of saline ions and humic acid. According to the free radical quenching experiments and electron paramagnetic resonance, the non-radical route dominant by ¹O₂ and few HO• and SO₄^•− were affirmed to participate the reaction. The recyclable MIL-101/CFO/PMS system approached high adsorption and catalysis ability for phenolics remediation in the environmental application.

期刊信息：Sep. Purif. Technol

DOI：10.1016/j.seppur.2024.129458

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题目：Constructing Cu-Mn bimetallic synergistic sites in 2D metal-organic framework nanosheets to induce polarized charge distribution: Electronic structure transformation and evaluation of Fenton-like performance

作者：Sheng Wang, Chi Yuan, Qinyang Lu, Shangkun Pei, Yuxin Lu, Yukai Wu, Xiang Li*, Bo Wang*

摘要：Heterogeneous Fenton-like process based on H₂O₂was an efficient method for the abatement of micropollutants in water. However, the mass transport resistance caused by the limited access between catalytic sites and target chemicals still restrict the decontamination efficiencies. Metal-organic frameworks (MOFs) with uniformed pores and anbundant metal sites shows great potentail in environmental remediation, Here, a novel two-dimensional nanosheet consisting of Cu and Mn bimetallic-oxygen clusters (CuMn-BDC, BDC refers to terephthalic acid organic ligand) was rationally designed and characterized. The introduction of second metal Mn changed the surface electronic distribution and accelerated the electron transfer of pristine Cu-based nanosheet, leading to improved catalytical acticities and removal effeciencies (kSA) for Sulfamethoxazole (SMX). The catalytic activity of CuMn-BDC obtained (5.76 × 10^–⁴) was 3.95 times higher than that of Cu-BDC (1.46 × 10^–⁴), demonstrating that the CuMn-BDC showed higher reaction rates than that of Cu-BDC when same amount of H₂O₂ was added. The interfacial micro-electric fields in bimetallic MOFs increased the interaction of organic pollutants and transfer the electron to activate H₂O₂. Several quenching experiments, electron paramagnetic resonance spectra and theoretical calculations were performed to study the reaction mechanism systematically. Further the powder was fabricated into membrane with higher water stablities. This study shed light on develop efficient 2D-MOFs catalyst for the abatement of micropollutants in water.

期刊信息：Sep. Purif. Technol

DOI：10.1016/j.seppur.2024.129488

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题目：Dual-functional luminescent Zn-MOF@MCHS nanocomposite for TNP detection and copper(II) adsorptive removal

作者：Indu Sharma , Ajay Kumar , Kushal Arya , Sanjay Mehra , Arvind Kumar , Surinder Kumar Mehta , Ramesh Kataria*

摘要：Environmental remediation in the jurisdiction of wastewater treatment is considered a critical global priority. Evidence suggests that mesoporous carbon hollow sphere (MCHS) has been extensively employed for electrochemical applications owing to its distinctive structure and efficient mass or charge transfer abilities. The distinctive amalgamation comprising a high surface area and intrinsic porosity from the metal–organic framework (MOF) and mesoporous spherical carbon shells offer enrichment in active analytical sites. To the extent of our understanding, no sensors have yet been created using a hybrid of MOFs and MCHSs. The current study utilizes in-situ fabricated MCHS and MOF-based novel fluorescent nanocomposite (Zn-MOF@MCHS) for the proficient sensing and adsorptive removal of environmental contaminants. Field emission scanning electron microscopy, High-resolution transmission electron microscopy and several other characterizations were employed to validate the physical attributes of the synthesized nanocomposite. These attributes could be advantageous in enhancing the adsorption and sensing functionalities of a material. The proposed system adaptably detects TNP (2,4,6-trinitrophenol) and Cu(II) ions (Stern-Volmer constants, Ksv = 0.36 × 10⁶ M⁻¹ and 0.83 × 10⁴ M⁻¹ respectively) along with efficient adsorption (99 % removal) of Cu(II) ions featuring a maximum adsorption capacity (q_max) of 523.56 mg/g. The low detection limits i.e., 0.368 µM for Cu(II) ion and 0.301 µM for TNP, demonstrated outstanding selectivity and sensitivity of Zn-MOF@MCHS.

The nanocomposite pertains to a surface area of 18.600 m²/g, adheres to second-order kinetics and exhibits optimal fitting to the Langmuir isotherm model to adsorb Cu(II) ions. X-ray Photoelectron Spectroscopy and zeta-potential analysis diligently scrutinize mechanistic evidence for the sensing and adsorption studies. Through experimental outcomes, the newly proposed nanoscale fluorescent composite showed the potential to serve as a universal platform for detecting and removing metal ions and detecting nitro compounds sensitively.

期刊信息：Sep. Purif. Technol

DOI：10.1016/j.seppur.2024.129538

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题目：Enhanced adsorption of radioactive cesium from nuclear wastewater using ZIF-67 laminated 2D MXene Ti₃C₂

作者：Han Zhang , Yujing Chi , Jiayi Li , Jinsong Peng , Haiyan Song* , Chunxia Chen* , Xuefeng Bai*

摘要：Development of nuclear industry has caused severe water pollution. Adsorptive removal of radionuclides from wastewater has been regarded as effective solution for environment. However, developing adsorbents with high adsorption capacity and selectivity for removal of radionuclides (such as ¹³⁷Cs) is still a challenge. Herein, we adopted an in situ assemble strategy to construct a novel composite, in which zeolitic imidazolate framework (ZIF-67) was grafted into two-dimension (2D) layers of transition metal carbides/nitrides (MXenes) Ti₃C₂, and used it in adsorptive removal of Cs+ from wastewater. Laminated and pillaring effect of ZIF-67 increased interlayer spacing and specific surface area of Ti₃C₂, significantly enhancing Cs⁺ adsorption. MXenes matrix provided the main adsorptive sites and interaction to stabilize Cs⁺, while the hybrid ZIF-67 assisted adsorption. The adsorbent achieved 96.2% removal for 5 mg·L^-1 of Cs⁺ within 6 h, and 50.0 mg·g⁻¹ of maximum adsorption capacity, with good recyclability for 4 times. Ion competition, kinetics and thermodynamics were studied in detail to obtain the behavior of Cs⁺ adsorption. Finally, adsorption mechanism was proposed that [Ti − O] − H⁺ and [Ti − O] groups of 2D Ti₃C₂ were main adsorptive sites to participate in ion exchange and complexation with Cs⁺, respectively, while 2-methylimidazole (2-MI) ligands in ZIF-67 were synergetic adsorption sites.

期刊信息：Sep. Purif. Technol

DOI：10.1016/j.seppur.2024.129590

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题目：Enhancing bimetallic redox cycling by Olsalazine-based MOF to achieve efficient removal of ofloxacin

作者：Jiayu Lu , Alu Ouyang , Zixin Wang , Yu Li , Xin Qin , Bo Su , Xuejing Huang , Kefeng Li ,

Jun Luo , Guorong Xu*, Ling Fan*, Ronghua Jin*

摘要：The broad utilization of metal–organic frameworks (MOFs) in advanced oxidation processes (AOPs) for wastewater remediation is impeded by toxic ligands, the challenging recovery of catalysts, and the low cycling efficiency of metal redox pairs. In this study, we fabricated a highly efficient and self-degradable bimetallic catalyst with coordinatively unsaturated metal sites (CUMSs) using non-toxic Olsalazine (Olsa) as a ligand to effectively eliminate the antibiotic ofloxacin (OFL). Under optimal conditions, the OFL removal efficiency approached nearly 100 % within 100 min, with the degradation rate of bimetallic MOFs being 4 times than that of monometallic MOFs. The significant enhancement in catalytic performance of the catalyst was ascribed to its reduced charge transfer resistance (Rct), coordinatively unsaturated metal sites, and accelerated cycling of high valence metal to low valence metal, facilitated by the introduction of bimetallic and reducing non-toxic ligands. Moreover, we investigated the effects of H₂O₂ concentration, catalytic dose, and pH on pollutant degradation. Additionally, results from quenching experiments and electron spin resonance (ESR) tests demonstrated that the three types of free radicals generated during the catalyst activation process played a key role in pollutant degradation.

期刊信息：Sep. Purif. Technol

DOI：10.1016/j.seppur.2024.129521

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题目：Metal–organic framework based photocatalytic membrane for organic wastewater treatment: Preparation, optimization, and applications

作者：Taotao Feng , Bin Wang* , Jiang Li , Tao Wang , Peng Huang , Xiaoyi Xu

摘要：The utilization of photocatalytic membranes represents a sustainable technology that effectively combines the benefits of photocatalysis and membrane separation. These membranes possess the ability to recycle powdered catalysts and mitigate membrane fouling, thereby exhibiting promising applications in the wastewater treatment. Metal–organic frameworks (MOFs) are emerging photocatalysts with favorable physicochemical properties, interfacial compatibility, and tunable performance, making them excellent materials for preparing photocatalytic membranes. In this review, strategies for modifying MOF photocatalysts were discussed to construct photocatalytic membranes with efficient processing performance. Methods for the preparation of MOF-based photocatalytic membranes in recent studies are presented, including crystalline growth, vacuum filtration, electrostatic spinning, and phase inversion. The application of MOF-based photocatalytic membranes in water treatment processes is outlined regarding contaminant removal and mitigation of membrane fouling while analyzing the underlying mechanism. Opportunities and challenges that may arise during further development are discussed to provide a theoretical basis for future research and practical applications of MOF-based photocatalytic membranes.

期刊信息：Sep. Purif. Technol

DOI：10.1016/j.seppur.2024.129540

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题目：Performance evaluation of a dynamic electrooxidation systems with magnetically functionalised UiO-66-NH₂ and Ti/Sb–SnO₂ for methotrexate treatment

作者：Bo Yang, Qiang Bi*, Shiping Zhao, Kun Zhang, Guoping Li, Juanqin Xue*

摘要：Novel conductive MOF magnetic particles Fe₃O₄@UiO-66-NH₂@PANI (FUP) were prepared and combined with Ti/Sb–SnO₂ electrodes to construct a dynamic system with improved electrochemical oxidation efficiency. Electrochemical tests revealed that the Ti/Sb–SnO₂–FUP electrodes showed a high active specific surface area and low charge transfer resistance. Investigation of the effects of parameters such as dynamic particle loading, magnetic separation time, initial concentration, Na₂SO₄ dosage and solution pH on the methotrexate (MTX) degradation rate revealed that the degradation rate reached 97.5%. Electron paramagnetic resonance spectroscopy revealed that the Ti/Sb–SnO₂–FUP electrodes could produce abundant hydroxyl radicals, possibly due to the unique pore structure of UiO-66-NH₂ and the semiconductor structure of aniline. Finally, the decomposition pathway of MTX and ecotoxicity of the intermediates were analysed through LC-MS/MS and Toxicity Estimation Software Tool theoretical calculations combined with genotoxicity experiments. The results showed that Ti/Sb–SnO₂–FUP could effectively reduce the toxicity of the intermediates. In this work, a dynamic electrooxidation system was developed using magnetic Ti/Sb–SnO₂ electrodes coupled with MOFs, providing a new idea to improve the oxidative degradation efficiency of electrooxidation systems.