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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”！
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题目：MOF derived hierarchical α-Bi2O3-BiVO4-CuFe2O4 multijunction heterostructure with conjugated S-scheme charge mobilization: Photocatalytic decontamination study, toxicity assessment and mechanistic elucidation
作者：Swagat Kumar Nayak, Sibun Kumar Pradhan, Saumyaranjan Panda, Ranjit Bariki, B.G. Mishra*
摘要：A series of hierarchical α-Bi2O3-BiVO4-CuFe2O4 multijunction heterostructure was designed by integrating one-pot MOF derived Bi2O3-BiVO4 microrods with CuFe2O4 nanosheets. The MOF-derived route afforded Bi2O3-BiVO4 with interconnecting porous architecture. Comprehensive investigations revealed preservation of crystalline phases, optimal light harvesting ability, higher lifetime, large electrochemically active surface area and improved charge dynamics. The heterostructure efficiently performed the photo-degradation of potentially toxic and mutagenic mesotrione (MTE) herbicide with rates 6-12 times greater than the parent semiconductors. The photo-degraded end products displayed profoundly less acute toxicity, bioaccumulation factor and mutagenic nature than parent MTE as analyzed by QSAR protocol. The heterostructure was equally effective for complete photo-inactivation of E. coli bacteria within 60 min of irradiation. SEM, AFM height profile and confocal microscopic investigation provided crucial information about the photo-inactivation process. A conjugated S-scheme electron transfer mechanism was proposed based on detailed band structure analysis to elucidate the improved activity of the multijunction photocatalyst.
期刊信息：Appl. Catal. B: Environ.
DOI：10.1016/j.apcatb.2024.124534
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题目：In situ anchoring of bimetal (Cu, Fe) sulfides featured by sulfur vacancy and phosphorus doping within porous carbon nanocubes derived from Prussian blue analogs to activate peroxymonosulfate for the efficient degradation of organic pollutants
作者：Jiaqi Chang, Simeng Xia, Zhou Shi, Hanxuan Zeng, Haojie Zhang*, Lin Deng*
摘要：In this work, Prussian blue analogues (CuFe-PBA) derived copper-iron sulfides/N-doped porous carbon composite (CuFe-NC-SP-x) was prepared as an effective peroxymonosulfate (PMS) activator to degrade sulfadiazine (SDZ). A strategy that kills two birds with one stone was proposed to construct CuFe-NC-SP-x, i.e., S-etched CuFe-PBA (CuFe-PBA-S) was annealed with NaH2PO2 in N2 atmosphere to simultaneously introduce sulfur vacancy (Sv) and phosphorus doping. 40 μM SDZ was completely removed by CuFe-NC-SP-2/PMS in 20 min (0.2 g/L catalyst and 0.5 mM PMS). The kobs value obtained by CuFe-NC-SP-2 (0.48 min−1) was nearly 33 and 17 times higher than that of CuFe-PBA (0.014 min−1) and CuFe-PBA-S (0.028 min−1), respectively. Quenching tests, electron paramagnetic resonance (EPR) analysis indicated that PMS activation in the system involved radical pathway (26.1 % ·OH and 22.7 % SO4·–) and non-radical pathway (17.8 % 1O2 and 33.4 % electron transfer process). ·OH, SO4·– and 1O2 were mainly produced by S enhanced metal sites for PMS activation. The synergistic effect of Sv and P doping enabled the powerful electron transfer mechanism. Electrochemical tests and DFT calculations demonstrated that Sv existing in CuFe-NC-SP-x improved the electron donor ability and increased the adsorption energy toward PMS, and phosphorus doping accelerated the electron transport from SDZ to PMS. This work not only provides a novel strategy to synthesize a high effective PMS activator by introducing Sv and phosphorous doing in one step, but also manages to comprehensively understand the electron transfer activation mechanisms of PMS facilitated by Sv and phosphorous doping.
期刊信息：Chem. Eng. J.
DOI:10.1016/j.cej.2024.155252
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题目：ZIF-67-natural sponge derived macroarchitectures as efficient catalytic converters for 4-nitrophenol removal
作者：Chaohai Wang, Zheng Lv, Jianmian Deng, Taiyang Cao, Minjun Kim*, Haiyan Kang, Junning Wang, Rongfu Peng, Xinfeng Zhu, Yanli Mao*
摘要：Sulfate radical-based advanced oxidation processes (SR-AOPs) is a very efficient wastewater treatment technology and has great potential for environmental remediation. However, finding efficient catalysts for activation of peroxomonosulfate (PMS) is still challenge. In this work, we synthesized a ZIF-67-coated natural sponge composite (ZS) using the in-situ growth method, and the material obtained after carbonization (ZSC) was used to activate PMS for better removal of 4-nitrophenol (4-NP). Natural sponges as carriers for loaded MOF materials can better stimulate the ability of composites to activate PMS, for example: (1) Prevents deactivation of MOF particles due to the occurrence of aggregation; (2) Solves the problems caused by the powder characteristics of the MOF particles themselves, prevents secondary contamination, and is easy to recycle; (3) Limit the risk of loss of MOF particles. The removal efficiency of ZSC-activated PMS for 4-NP (10 ppm) was remarkable at 99 %. Natural sponges as carriers, are taken from the natural environment, which is more affinity with the environment, reduces the risk of pollution and highlights the sustainability of the material. This study proposes a green and sustainable material for the removal of 4-NP to provide technical support for water ecological management.
期刊信息：Chem. Eng. J.
DOI:10.1016/j.cej.2024.155103
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题目：Highly efficient removal and real-time visual detection of fluoride ions using ratiometric CAU-10-NH2@RhB: Probe design, sensing performance, and practical applications
作者：Ping Ju, Wenhui Lu, Guixue Zhang, Shuping Wang, Anzhang Li, Qingxiang Zhang, Long Jiang, Ensheng Zhang*, Fengli Qu
摘要：The extensive use of fluoride in agriculture, industry, medicine, and daily necessities has raised growing concerns about fluoride residue. To date, real-time visual detection and efficient removal of fluoride ions from water remain greatly desirable. Herein, nano-CAU-10-NH2@RhB is introduced as a ratiometric fluorescent probe and efficient scavenger for the intelligent detection and removal of fluoride ions. CAU-10-NH2@RhB is readily obtained through one-pot synthesis and exhibits high sensitivity and selectivity for real-time fluoride ion detection, with a naked-eye distinguishable color change from pink to blue. A portable device for point-of-care testing was developed based on color hue analysis readout using a smartphone. A quantitative response was achieved across a wide concentration range, with a detection limit of 54.2 nM. Adsorption experiments suggest that nano-CAU-10-NH2@RhB serves as an efficient fluoride ion scavenger, with a fluoride adsorption capacity of 49.3 mg/g. Moreover, the mechanistic study revealed that hydrogen bonds formed between fluoride ions and amino groups of CAU-10-NH2@RhB are crucial for the detection and adsorption of fluoride ions. This analysis platform was also used for point-of-care quantitative visual detection of fluoride ions in food, water, and toothpaste.
期刊信息：J. Hazard. Mater.
DOI:10.1016/j.jhazmat.2024.135659
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题目：Metal organic and covalent organic framework-based QCM sensors for environmental pollutant detection and beyond
作者：Zaynab Golshadi, Mohammad Dinari*, Alexander Knebel, Johannes Lützenkirchen, Bahram Hosseini Monjezi*
摘要：Environmental pollution has become a major global issue, worsened by the rapid growth of industries. Traditional pollutant detection methods often require high operational temperatures and exhibit limited sensitivity and selectivity. Quartz crystal microbalance with dissipation monitoring (QCM-D) sensors have emerged as a promising alternative, offering high sensitivity, affordability, and precise measurements at room temperature. This review explores the integration of metal-organic frameworks (MOFs) and covalent organic frameworks (COFs), into QCM sensors to boost their performance. MOFs, with their high porosity and surface tunability, and COFs, known for their exceptional chemical and thermal stability, are examined for applications such as gas detection, heavy metal sensing, and thin film measurements. Our findings indicate that MOF/COF substrates on QCM electrodes enhance assay efficiency and sensor sensitivity, offering quick responses, good stability, compact size, and nanogram-level detection. Enhancements in porosity, sensitivity, and selectivity, along with integration with other methods, promise significant advancements. We discuss the synthesis methods, properties, and advantages of MOF- and COF-based QCM sensors. Additionally, we address the challenges and future perspectives of these advanced materials in QCM sensor technology, aiming to pave the way for innovative solutions in pollutant detection and environmental safety.
期刊信息：Coord. Chem. Rev
DOI：10.1016/j.ccr.2024.216163
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题目：Interfacial activation of alkaline phosphatase induced by hydrophilic metal-organic frameworks
作者：Dongyan Chen, Yi Xu, Jie Wei, Munetaka Oyama, Quansheng Chen & Xiaomei Chen*
摘要：Encapsulating natural enzymes in metal-organic frameworks (MOFs) can maintain the original biological functions of enzymes in harsh environments. However, the nature of interfacial interactions between a MOF and enzyme is currently unclear, rendering effective regulation of the biocatalytic activity of the enzyme@MOF composite difficult. Differences in the hydrophilicity of MOF carriers are closely related to the conformational changes and catalytic properties of the enzyme. In this study, the catalytic activity, stability, and conformational changes of alkaline phosphatase (ALP) encapsulated in hydrophilic zeolite imidazolate framework-90 (ZIF-90) and hydrophobic ZIF-8 were systematically investigated using experimental methods and molecular dynamics simulations. The results demonstrated that hydrophilic ZIF-90-encapsulated ALP exhibited superior stability and was 2.22-fold more retained catalytically active than hydrophobic ALP@ZIF-8 after 20 cycles of utilization. Moreover, the hydrophilic interface provided by ZIF-90 effectively regulated the structure of ALP to maintain the optimal catalytic conformation of its active center. The practical application of highly bioactive ALP@ZIF-90 was demonstrated by employing it in a self-calibrated colorimetric/fluorescence dual-mode sensing method for the efficient, reliable, and accurate detection of methyl paraoxon. This study provides new insights for improving enzyme immobilization strategies and promoting the rapid development of enzyme@MOF composites for catalytic and sensing applications.
期刊信息：Nano Res.
DOI：10.1007/s12274-024-6929-2
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题目：In-situ synthesis to promote surface reconstruction of metal–organic frameworks for high-performance water/seawater oxidation
作者：Guohao Na, Hongshun Zheng, Mingpeng Chen*, Huachuan Sun, Tong Zhou, Yuewen Wu, Dequan Li, Qingjie Lu, Yun Chen, Jianhong Zhao, Yumin Zhang, Tianwei He, Bin Xiao, Jin Zhang, Feng Liu, Hao Cui, Qingju Liu*
摘要：Metal-organic frameworks (MOFs) have gained tremendous notice for the application in alkaline water/seawater oxidation due to their tunable structures and abundant accessible metal sites. However, exploring cost-effective oxygen evolution reaction (OER) electrocatalysts with high catalytic activity and excellent stability remains a great challenge. In this work, a promising strategy is proposed to regulate the crystalline structures and electronic properties of NiFe-metal-organic frameworks (NiFe-MOFs) by altering the organic ligands. As a representative sample, NiFe-BDC (BDC: C8H6O4) synthesized on nickel foam (NF) shows extraordinary OER activity in alkaline condition, delivering ultralow overpotentials of 204, 234 and 273 mV at 10, 100, and 300 mA cm−2, respectively, with a small Tafel slope of 21.6 mV dec−1. Only a slight decrease is observed when operating in alkaline seawater. The potential attenuation is barely identified at 200 mA cm−2 over 200 h continuous test, indicating the remarkable stability and corrosion resistance. In-situ measurements indicate that initial Ni2+/Fe2+ goes through oxidation process into Ni3+/Fe3+ during OER, and eventually presents in the form of NiFeOOH/NiFe-BDC heterojunction. The unique self-reconstructed surface is responsible for the low reaction barrier and fast reaction kinetics. This work provides an effective strategy to develop efficient MOF-based electrocatalysts and an insightful view on the dynamic structural evolution during OER.
期刊信息：J. Colloid Interface Sci.
DOI：10.1016/j.jcis.2024.08.206
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题目：Boosted photo-Fenton-like process for selective degradation of emerging contaminants by dehydrated Fe-based metal–organic framework with thermodynamically-favorable center metal electron density and confinement effect
作者：Wei Guo, Xiaoyan Zhang, Ke Wang, Xueyi Zou, Guoshen Zeng, Jiapeng Zhong, FengHui Tian, Chuanhao Li*
摘要：The Heterogeneous Fenton reaction has long stood out as a highly effective technology for water purification. However, it is nowadays facing challenges such as low selectivity, sluggish Fe(III) reduction, and limited H2O2 conversion efficiency. Herein, dehydrated MIL-100(Fe)-250 was synthesized through thermal treatment, demonstrating superior efficiency in removing emerging contaminants, with a three-fold efficiency higher than undehydrated sample. The dehydrated MIL-100(Fe)-250 exhibited selective acceleration in the removal of quinolones and phenolic organics, rendering the system resistant to interference from coexisting matter. Through in-situ diffuse reflectance infrared Fourier-transform spectroscopy and density functional theory calculation, it was manifested that dehydration process regulates the steric hindrance and local electron density of Fe ions. This adjustment enhances charge transfer, thereby facilitating Fe(III) reduction and promoting the H2O2 activation and conversion efficiency. Moreover, the quasi-steady-state concentrations of hydroxyl radical in MIL-100(Fe)-250 were found to be 2.2 times higher than that those in undehydrated sample. Impressively, the dehydrated MIL-100(Fe)-250 displayed adaptability across a broad pH range of 5.0–9.0. The present study underscores the significant potential of porous MIL-100(Fe)-250 with spatial confinement, which imparts a clear size exclusion effect. As a result, this catalyst emerges as a promising candidate for eliminating contaminants in real water matrices, offering a viable strategy for water pollution control.
期刊信息：Sep. Purif. Technol
DOI：10.1016/j.seppur.2024.129198
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题目：Efficient synthesis of MOF-808 nanoparticles for rapid hydrolysis of V-series nerve agent simulant
作者：Yan-Ling Guo, Sai-Nan Guo, Ke-Qing Liu, Yan Wei, He Zheng*, Jie-Xin Wang*
摘要：The degradation of nerve agents is essential due to their high toxicity and lethality. The Zr-based metal–organic framework MOF-808 has emerged as a promising catalyst for the destruction of nerve agents and their simulants. However, its efficient synthesis is still a great challenge. In this study, we reported a convenient method for rapidly preparing MOF-808 nanoparticles in a rotating packed bed (RPB) reactor using high-gravity technology. Compared to a conventional stirred tank reactor, the preparation time of MOF-808 in the RPB was greatly shortened from 12 h to 30 min, while the mean particle size was obviously decreased by about 74 %. The obtained MOF-808 nanoparticles exhibited excellent catalytic performance for the hydrolysis of the nerve agent simulant O, O-diethyl S-phenyl phosphorothioate (DEPPT). Particularly, the 339 nm MOF-808 can rapidly degrade DEPPT with a half-life (t1/2) of 4.36 min and an equilibrium degradation rate of 92.6 % at a dosage of 2.5 mg, respectively 1.5 and 1.25 times higher than those of 1.3 µm MOF-808 (t1/2 = 6.36 min, 74.3 %). Furthermore, the DEPPT degradation mechanism was elucidated through a combination of experimental studies and density functional theory calculations. This work provides valuable insights into the efficient synthesis of nano-MOFs with enhanced catalytic activity for the hydrolysis of nerve agents.
期刊信息：Sep. Purif. Technol
DOI：10.1016/j.seppur.2024.129232
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题目：ZnIn2S4/MIL-53-NH2 composite photocatalysts for H2O2 production: Synergistic effect of sulfur vacancy and heterostructure
作者：Yong Tang, Jianhao Qiu*, Dingliang Dai, Guanglu Xia, Biyao Fang, Yixin Li, Jianfeng Yao*
摘要：Defect engineering is used in the development of photocatalysts and has received widespread attention for achieving efficient photocatalysis. Here, ZnIn2S4 with rich sulfur vacancies (VS-ZnIn2S4) was integrated with MIL-53-NH2 for photocatalytic H2O2 production from O2 reduction under visible light. The sulfur vacancy could effectively promote charge separation and O2 capture, and the heterostructure between ZnIn2S4 and MIL-53-NH2 further inhibits charge recombination, which promises highly boosted photocatalytic activities. In ambient air and pure water, VS-ZnIn2S4/MIL-53-NH2 heterostructures exhibit superior photocatalytic H2O2 production performance (705 μmol·L−1) relative to those of monomeric ZnIn2S4 (78 μmol·L−1), VS-ZnIn2S4 (210 μmol·L−1), MIL-53-NH2 (38 μmol·L−1), as well as ZnIn2S4/MIL-53-NH2 (395 μmol·L−1). Mechanistic studies have confirmed that the main pathway for H2O2 formation on VS-ZnIn2S4/MIL-53-NH2 is ⋅O2–-triggered O2 reduction, and sulfur vacancy can adsorb and activate O2 to facilitate the production of ⋅O2–. This study provides new insights into catalyst design and green synthesis of H2O2.
期刊信息：Sep. Purif. Technol
DOI：10.1016/j.seppur.2024.129350
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题目：Multiple strategies enhance visible-light photocatalytic degradation levofloxacin of Fe-doped MOF/AgCl Z-scheme heterojunction composites based on pyrazole carboxylic ligand
作者：Jun Chen, Siyi Zhang, Yifei Xu, Jianning Cai, Yang Yang, Xin Wang, Chaoyue Chen, Jiamin Wei,* Lianshe Fu, Tinghai Yang*
摘要：The construction of visible-light catalysts to degrade water pollutants is significant in environmental governance and solar energy conversion. In this work, a novel Zn-MOF with unsaturated coordination sites was constructed using 1-(Carboxymethyl)-pyrazole-4-carboxylic acid as the organic ligand. Its crystal structure was studied through single crystal X-ray diffraction. To enhance visible light catalytic performance, ZnFe-MOF/AgCl-x Z-scheme heterojunction composites were constructed. The optimized ZnFe-MOF/AgCl-50 material exhibits excellent photocatalytic performance, which can degrade 90.33 % of levofloxacin in 21 min. The results indicate that Fe doping and the construction of the ZnFe-MOF/AgCl-x Z-scheme heterojunction not only broaden the responsive range to visible light, but also effectively promote the internal and interfacial charges transfer efficiency, leading to a superior catalytic performance. In addition, the Ag nanoparticles (NPs) generated during the photocatalytic process can serve as a bridge, achieving rapid charge transfer in Z-scheme heterojunction. This work can offer an innovative perspective for the development of novel and efficient MOF-based Z-scheme heterojunction photocatalysts for wastewater treatment applications.
期刊信息：Appl. Surf. Sci.
DOI：10.1016/j.apsusc.2024.160994
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常淼，女，北京建筑大学环境工程专业2022级硕士研究生，主要从事钢铁废水的资源化利用制备高附加值MOFs的研究，目前以第一作者身份在Progress in Natural Science: Materials International（SCI，IF = 4.3，Q2）发表论文1篇。
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