MOFs基材料用于环境污染控制文献整理（2024.11.03-2024.11.09）

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题目：Metal-organic frameworks based on pyrazolates for the selective and efficient capture of formaldehyde

作者：Nicolas Sadovnik*,  Pengbo Lyu,  Farid Nouar,  Mégane Muschi, Menghao Qin,  Guillaume Maurin,  Christian Serre *&  Marco Daturi *

摘要：Indoor air pollution is one of the major threads in developed countries, notably due to high concentrations of formaldehyde, a harmful molecule difficult to eliminate. Addressing this purification challenge while adhering to the principles of sustainable development requires the use of innovative, advanced sustainable materials. Here we show that by combining state-of-the-art spectroscopic techniques with density-functional theory molecular simulations, we have developed an advantageous mild chemisorption synergistic mechanism using porous metal (III or IV) pyrazole- di-carboxylate based metal-organic framework (MOF) to trap formaldehyde in a reversible manner, without incurring significant energy penalties for regeneration. A straightforward, environmentally friendly, and scalable synthesis protocol was established for the porous, water-stable aluminum pyrazole dicarboxylate known as Al-3.5-PDA or MOF-303, capable of functioning as a highly efficient and reusable filter. It demonstrates selectivity and high storage capacity for formaldehyde under conditions typical of severe indoor use, such as in housing or vehicle cockpits, including varying VOC mixtures and concentrations, humidity, and temperature, without any accidental release. Furthermore, we have successfully regenerated this sorbent using a simple domestic protocol, ensuring the material reusability for at least 10 cycles.

期刊信息：Nat. Commun.

DOI：10.1038/s41467-024-53572-z

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题目：Metal-Organic frameworks (MOFs) for Oxo-Anion removal in wastewater Treatment: Advancements and applications

作者：M. Shahnawaz Khan*, Sidi Zhu, Shing Bor Chen*

摘要：Coordination chemistry has unveiled the significant role of metal–organic frameworks (MOFs) in materials research. Characterized by diverse porous structures formed by metal ion/cluster units and organic linkers, MOFs have gained considerable attention due to their unique coordination structure, high porosity, and extensive surface area, making them invaluable in chemical, biological, and materials science. Their exceptional chemical stability also makes MOFs promising candidates for adsorbing pollutants from wastewater. Metal oxo-anions, identified as significant pollutants by the United States Environmental Protection Agency (USEPA), require efficient water treatment solutions. Traditional methods face challenges and low selectivity, leading to incomplete removal of these substances. MOFs offer a solution through their tunable functionalities, enabling selective adsorption of hazardous oxo-anions like chromium, selenium, and arsenic. Precise engineering of MOFs by incorporating suitable functional groups and metal sites can significantly enhance their adsorption capacity and selectivity, advancing environmental remediation efforts. This comprehensive review explores the critical role of MOFs in addressing environmental challenges, especially water pollution from metal oxo-anions. It highlights innovative strategies for customizing MOF architectures and optimizing their performance for selective oxo-anion removal, contributing to a deeper understanding of MOFs’ potential in achieving environmental sustainability. Additionally, the review investigates the interactions between MOFs and toxic oxo-anions, underlying mechanisms, experimental approaches, and design principles crucial for successful MOF deployment in real-world water treatment applications. By analyzing the multifaceted role of MOFs in mitigating water pollution, this review provides valuable insights that can shape the future of sustainable water management.

期刊信息：Chem. Eng. J.

DOI：10.1016/j.cej.2024.157396

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题目：Eco-friendly synthesized zeolitic imidazolate framework-8 enables one-step cerium recovery from water

作者：Ying Zhou, Shengshou Ma, Purui Lin, Changzhong Liao, Cheng-Wei Kao*, Miaoling Chen, Minhua Su, Kaimin Shih*

摘要：The rapid pace of technology advancement has quickly depleted valuable rare earth elements (REEs), which are critical for the function and performance of electric and electronic components, and there is thus a need for REE extraction from secondary sources rather than from virgin mines. This study presents an approach involving the ball-milling-induced construction of zeolitic imidazolate framework-8 (ZIF-8) that integrates REE extraction and recovery processes. ZIF-8 demonstrates remarkable extraction capacities for various REEs, and notably promotes nanoscaled CeO₂ formation. Ball-milling-prepared ZIF-8 (ZIF-8-BM) effectively concentrates cerium (III) ions (Ce^III), and a purity of 99.34% is achieved by controlling the processing parameters, offering a comprehensive solution for efficient Ce retrieval from wastewater. The superior Ce extraction performance is attributed to the greater numbers of structural defects and surface hydroxyl (–OH) groups and the enhanced phase transformation efficiency. Moreover Ce extraction by ZIF-8-BM is found to be efficient in both low and high Ce concentration ranges. ZIF-8-BM nanoparticles spontaneously oxidize CeIII in solution to insoluble CeO₂, thereby facilitating the efficient extraction and subsequent recovery of cerium from complex matrices. The findings of this study provide an environmentally benign approach for the safe and efficient recovery of REEs from waste streams, supported by a scientifically sound and economically feasible processing strategy.

期刊信息：Chem. Eng. J.

DOI：10.1016/j.cej.2024.157456

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题目：Post-synthetic modification of MOF UiO-66-NH₂ membranes for efficient methanol/organic separation

作者：Langhui Wu , Ye Liang , Bo Zhang , Shenzhen Cong , Shenyi Tang , Kangkang Jiang , Liping Luan , Zhi Wang , Xinlei Liu *

摘要：The separation of MeOH/organic mixtures poses a significant challenge in the chemical industry. In this study, metal-organic framework UiO-66-NH₂ membranes prepared by a secondary solvothermal method were employed for MeOH/DMC, MeOH/Tol and MeOH/MTBE separation. The membrane performance was significantly boosted by post-synthetic modification with oxalyl chloride (OC), succinyl chloride (SC), and salicylaldehyde (SA). The modified UiO-66-NH₂-OC and UiO-66-NH₂-SC membranes displayed simultaneous improvement of the separation factors and MeOH fluxes. The modified UiO-66-NH₂-SA membranes exhibited an order of magnitude enhancement of separation factors, with comparable MeOH fluxes. Specifically, separation factors of 3220 and 28,000 with MeOH fluxes of 1.18 kg m⁻² h⁻¹and 1.03 kg m⁻² h⁻¹ for 5/95 wt% MeOH/Tol and 5/95 wt% MeOH/MTBE separation at 40°C, respectively, were delivered by UiO-66-NH₂-SA membranes. Moreover, the UiO-66-NH₂-SA membranes demonstrated good stability over 120 h's evaluation. This study offers a promising post-synthetic approach and a class of membrane materials for efficient MeOH/organic separation.

期刊信息：J. Membr. Sci.

DOI：10.1016/j.memsci.2024.123475

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题目：Mesoporous N-doped hierarchical porous materials derived from core-shell MOFs: A promising strategy for eliminating sulfamethoxazole using ¹O₂

作者：Ming Ma , Yuxin Lu , Sheng Wang , Shangkun Pei , Chong-Chen Wang , Xiang Li*, Bo Wang*

摘要：Slfamethoxazole (SMX) has been considered as one kind of important micropollutants in water which need to be removed effectively. Developing one kind of material for effectively removing SMX in water is crucial in treatment process. In this study, core–shell structured metal–organic frameworks (MOFs) with increasing shell thickness (5, 10, and 20-ZIF-8@ZIF-67 s) were selected as an ideal platform to develop water-stable hierarchical porous carbons (HPCs) using one-step calcination, showing the dual functionals of both adsorption and catalysis by producing large amount of acitve species (¹O₂). These novel HPCs systematically optimized at increasing temperatures and ratios of two metals. The 10-Co-NHPC-900 at optimal conditions shows highest adsorption capacities and initial adsorption rates, which are 4.56 and 10.35 times higher than those of calcinated ZIF-67 s. The decomposition mechanisms based on PMS were systematically studied by analyzing oxidant consumption, reactive oxygen species and by-products of SMX. In addition, Co ions leached amount of 10-Co-NHPC-900 was 63.6 times lower than that of MOF precursor, indicating that the cobalt-based porous carbon have higher water stabilities. This study offers an efficient approach for reducing micropollutants risk using water-stable hierarchical porous carbons.

期刊信息：Sep. Purif. Technol.

DOI：10.1016/j.seppur.2024.130092

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题目：ZIF-8-modified multiscale polyurethane/flexible polyurethane nanofiber membrane for multifunctional adsorption of formaldehyde, antibacterial and anti-haze window screen

作者：Weili Shao*, Wanying Han , Liang Zhu , Shengli Zhu , Shiliang Sheng , Yanfei Chen , Pengju Han , Ying Cao*, Hui Xu , Rongwu Wang , Wanli Yue*, Fan Liu

摘要：All kinds of indoor pollutants (such as particulate matter (PM), formaldehyde, and bacteria, among others) can harm people’s health, making the elimination of indoor pollution a hot topic. In this work, multi-scale polyurethane (PU)/flexible polyurethane (FPU) nanofiber membrane modified with ZIF-8 nanoparticles (ZIF-8@MSNs) were designed and prepared by electrospinning for multifunctional formaldehyde adsorption, antibacterial and anti-fog window screen. The results demonstrated that the multiscale nanofibers (MSNs) modified by zif-8 have excellent filtration performance (filtration efficiency: 99.9 %, pressure drop resistance: 84 Pa) and durability, and better hydrophobic performance (contact angle: 148°) compared with MSNs, while the ZIF-8@MSNs window screen exhibited good light transmittance (79 %) and high air permeability (99.2 mm s⁻¹). It is worth mentioning that the ZIF-8@MSNs exhibited good formaldehyde adsorption properties (up to 95.2 %) and excellent antibacterial properties (under light conditions, the sterilization rates of Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus) reached 99.996 % and 99.993 %, respectively).Consequently, the multifunctional material developed herein, which adsorbs formaldehyde, exhibits antibacterial action, and has anti-haze characteristics, provides a new strategy for indoor air purification applications.

期刊信息：Sep. Purif. Technol.

DOI：10.1016/j.seppur.2024.130345

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题目：Fabrication and incorporation of MIL-53(Fe)-zwitterionic brushes into PVDF thin film composite membranes for enhancing heavy metal/dye rejection from aqueous body

作者：Nethravathi Prabhakar, Arun M. Isloor* , Ramin Farnood , Ahmad Fauzi Ismail.

摘要：The bioaccumulation of heavy metal ions is a serious concern for researchers. The dyes and heavy metal ions also aquatic life impacting the biodiversity adversely. Synthesis of novel MIL-53(Fe)-PSBMA particles, and its incorporation into PVDF-based thin-film composite membranes is the crux of this work. Firstly, H₂N-MIL-53(Fe) was synthesized by metal displacement reaction which was then modified into MIL-53(Fe)-PSBMA brushes. The brushes were synthesized by atom transfer radical polymerization method. The amine groups of the NH₂-MIL-53(Fe) help connecting the MOF to the polymeric moiety. The as-synthesized material and the fabricated TFCs were characterized by BET, FTIR, XRD, XPS, TGA, AFM, FE-SEM, zeta potential, and DLS particle sizer. The presence of sulphur groups on the XPS spectrum of modified MOF ensured the successful polymer grafting on it. Zwitterionic moieties have both positive and negative charges within a single molecule which gave a resultant zeta potential of −13.1 mV for the brushes. A pure water flux of 26.32 Lm⁻² h⁻¹ and 97.33 %, 95.19 %, 82.06 %, and 78.47 % rejections for Pb²⁺, Hg²⁺, As³⁺, Cd²⁺ ions and 96.23 % and 94.04 % rejection for 100 ppm reactive black-5 and sunset yellow dyes respectively were obtained for the optimized membrane having 0.035 wt% loading of zwitterionic MOF. This result was attributed to the enhanced membrane hydrophilicity which was also correlated with contact angle and water uptake studies.

期刊信息：Sep. Purif. Technol.

DOI：10.1016/j.seppur.2024.130348

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本期编辑

郭志慧，女，北京建筑大学资源与环境专业2023级硕士研究生。主要研究方向为金属-有机框架材料的设计、制备及其在水环境修复领域的应用。

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