点击蓝字，关注我们
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”！
1
题目：Ligand engineering enhances (photo) electrocatalytic activity and stability of zeolitic imidazolate frameworks via in-situ surface reconstruction
作者：Zheao Huang, Zhouzhou Wang, Hannah Rabl, Shaghayegh Naghdi, Qiancheng Zhou, Sabine Schwarz, Dogukan Hazar Apaydin, Ying Yu *& Dominik Eder*
摘要：The current limitations in utilizing metal-organic frameworks for (photo)electrochemical applications stem from their diminished electrochemical stability. In our study, we illustrate a method to bolster the activity and stability of (photo)electrocatalytically active metal-organic frameworks through ligand engineering. We synthesize four distinct mixed-ligand versions of zeolitic imidazolate framework-67, and conduct a comprehensive investigation into the structural evolution and self-reconstruction during electrocatalytic oxygen evolution reactions. In contrast to the conventional single-ligand ZIF, where the framework undergoes a complete transformation into CoOOH via a stepwise oxidation, the ligand-engineered zeolitic imidazolate frameworks manage to preserve the fundamental framework structure by in-situ forming a protective cobalt (oxy)hydroxide layer on the surface. This surface reconstruction facilitates both conductivity and catalytic activity by one order of magnitude and considerably enhances the (photo)electrochemical stability. This work highlights the vital role of ligand engineering for designing advanced and stable metal-organic frameworks for photo- and electrocatalysis.
期刊信息：Nat. Commun.
DOI：10.1038/s41467-024-53385-0
论文链接：
2
题目：Enhanced peroxymonosulfate activation for antibiotic and heavy metal removal using ZIF-67-derived magnetic Ni/Co-LDH@NC: Bimetallic electronic synergy and oxygen vacancy effects
作者：Mengqing Hu,Di Zhao,Xinlong Yan*,Yun Wang,Jin Zhang,Xiaoyan Hu,Ming Zhou*,Porun Liu
摘要：Designing advanced bimetallic catalysts is essential to improving peroxymonosulfate (PMS) activation.Herein,a novel magnetic nickel/cobalt-layered double hydroxide decorated nitrogen-doped carbon(Ni/Co LDH@NC)catalyst we synthesized using carbonized ZIF-67 as a template for simultaneous removal of sulfamethoxazole(SMX)and Pb(Ⅱ)by PMS activation.The synthesized Ni/Co LDH@NC achieved complete degradation of SMX within 20 min and adsorbed Pb(Ⅱ) at 90.3 mg g−1in 2 h.Notably,in simulated mixed wastewater,Ni/Co LDH@NC removed 100 % of SMX and simultaneously absorbed 84 % of Pb(Ⅱ) within 60 min.Density functional theory (DFT) studies revealed that synergistic Ni-Co sites and “bridging oxygen” vacancies enhanced electron transfer to PMS,facilitating O-O bond cleavage.The catalyst maintained high performance after four cycles,with over 85 % SMX degradation and 80 % Pb(Ⅱ) removal.This study highlights the potential of MOF-derived catalysts for efficient,simultaneous remediation of antibiotic and heavy metal pollutants,contributing to advanced wastewater treatment.
期刊信息：Appl. Catal., B
DOI:10.1016/j.apcatb.2024.124753
论文链接：
3
题目：Hourglass-shaped europium cluster-based secondary building unit in metal–organic framework for photocatalytic wastewater purification and sterilization via enhanced reactive oxygen species production
作者：Guan-Huang Zhang, Hai-Ling Wang, Lei Cheng*, Yun-Lan Li, Zhong-Hong Zhu*, Hua-Hong Zou*
摘要：A large number of diseases caused by water pollution have become a global public health issue, and the development and construction of innovative and efficient photocatalytic systems for water remediation is vital to improve water quality and prevent bacteria-induced diseases. Herein, a europium-based metal–organic framework (Eu-MOF) was self-assembled with complex hourglass-shaped Eu9 clusters as secondary building units (SBUs), achieving excellent photoinduced reactive oxygen species (ROS) generation ability. Moreover, Eu-MOF can quickly and efficiently degrade organic dyes and kill a variety of bacteria under low-power light irradiation conditions. Time-dependent scanning electron microscopy (SEM) and infrared absorption spectroscopy (IR) were used for the first time to track the formation process of complex clusters into cluster-based MOFs, and the gradual transformation of amorphous intermediates into crystalline Eu-MOF was clearly tracked. Electrochemical impedance spectroscopy (EIS) results showed that Eu-MOF has a smaller semicircle than the organic ligands, demonstrating its excellent charge separation ability. The excellent ROS generation capacity of Eu-MOF was jointly demonstrated by electron paramagnetic resonance (EPR) spectroscopy and the results obtained using the 2’,7’-dichlorodihydrofluorescein (DCFH) indicator. More importantly, using low-power (60 mW/cm2) Xe lamp irradiation, Eu-MOF can almost completely degrade 10 mg/L aqueous solutions of rhodamine B (RhB), methylene blue (MB), and crystal violet (CV) within 30, 90, and 120 min, respectively. In addition, the excellent light-induced ROS production ability of Eu-MOF contributes to its significant cell killing and antibacterial effects. Under light irradiation conditions, Eu-MOF can effectively kill Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus), with average inhibition zone sizes of 2.54 ± 0.17 and 2.56 ± 0.08 cm, respectively. This work opens up new horizons for the build of efficient photocatalytic systems based on lanthanide porous materials and promotes the progress of lanthanide MOFs (Ln-MOFs) crystal engineering.
期刊信息：J. Colloid. Interf. SCI
DOI：10.1016/j.jcis.2024.10.133
论文链接：
4
题目：Dual signal amplification strategy-based electrochemical aptasensor utilizing redox molecule/MOF composites for multi-pesticide detection MOF composites for multi-pesticide detection
作者：Fen Wu,Haiqian Guo,Beibei Wang,Kai Kang,Lanyue Wang,Yuping Wang,Xueping Ji*
摘要：Electrochemical aptasensor is a great tool for simultaneously assessing harmful pesticide residues in agricultural products and foods. This study ingeniously designed an electrochemical aptasensor based on dual signal amplification strategies for concurrent detection of various pesticide residues. Firstly, poly(diallyldimethylammonium chloride)-functionalized reduced graphene oxide (PR) and Au-Pt-Pd trimetallic nanoflowers supported on HP-UiO66-NH2 were creatively employed together as substrates to load more aptamers, ascribed to the improved conductivity, abundant sites and a large electrochemical effective surface area. Secondly, ferrocene-cysteine gold nanoparticles supported on CeMOF(Ⅲ, Ⅳ) and methylene blue-loaded MOF235 were innovatively engineered to build two distinctive signal labels, which displayed comparable large and stable signal currents among other redox molecule/MOF composites. Additionally, PR contributed further signal amplification. Consequently, the constructed aptasensor showed superior performance for simultaneous detection of acetamiprid (AD) and malathion (ML), with linear ranges from 10 pM to 0.1 μM and detection limits of 4.8 pM for AD and 0.51 pM for ML. Moreover, the aptasensor performed well in the assay of AD and ML in Chinese cabbage samples with high accuracy compared with a high-performance liquid chromatography-tandem mass spectrometry method. Overall, the strategies proposed herein provided a useful and potential route for general development of electrochemical aptasensors to simultaneously detect multiple pesticide residues.
期刊信息：Sens. Actuators, B
DOI：10.1016/j.snb.2024.136757
论文链接：
5
题目：Sm-MOF decorated cotton for efficient on-demand oil-water separation and organic pollutants removal
作者：Jiefeng Meng , Jun Teng , Feng Li*, Taohai Li , Rossella Greco , Wei Cao
摘要：Complex wastewater containing oil–water and contaminant mixtures is a constant threat to ecosystems and public health. However, efficient water–oil separation and water treatment are required, with a preference for simple but universal matrices for possible large-scale applications. Herein, effective oil–water separation and organic pollutant removal are simultaneously realized on cotton balls decorated with polydimethylsiloxane combined with a samarium metal–organic framework. Cotton balls containing polydimethylsiloxane (10 %) and Sm-MOF (Synthesis temperature was 110℃, 15 mg/L) were successfully prepared by a simple precipitation method, with a high water contact angle of 150.75 ± 1.1°. After pre-wetting with a low surface energy solution, the modified cotton was endowed with repeatable super-wetting transitions between superhydrophobic/superoleophilic and superhydrophilic/underwater superoleophobic properties. In addition to on-demand separations of immiscible oil–water mixtures at a rate of 95 %, water-in-oil emulsions could be separated by the addition of different surfactants. The mechanism of demulsification of the treated cotton ball was studied based on the type of emulsifier and the results of emulsified oil separation. Cotton balls modified with 10 % PDMS and Sm-MOF (Synthesis temperature was 140 °C; 15 mg/L) showed higher adsorption capacity compared to pure cotton balls, adsorbing about 98.7 % of Eriochrome Black T within 2 h. Cotton balls modified by PDMS and Sm-MOF are an effective, safe and green material with promising applications in the simultaneous separation of oil–water mixtures and removal of organic pollutants from water systems.
期刊信息：Sep. Purif. Technol
DOI：10.1016/j.seppur.2024.130248
论文链接：
6
题目：Fast removal of sulfamethoxazole by MIL-101(Fe)–NH2/perylene diimide activated persulfate under visible light
作者：Yanyan Jia , Liang Duan*, Haisheng Li*, Chang Zhang , Qiusheng Gao , Hengliang Zhang , Shilong Li , Mingyue Li
摘要：Photocatalytically induced persulfate (PS) activation is considered a viable approach to counter the threat of resistance genes caused by the continuous accumulation of sulfamethoxazole (SMX) in the aqueous environment. In this study, the electrostatic interaction between MIL-101(Fe)–NH2 and perylene diimide (PDI) was exploited to fabricate composite catalysts (MNPx) with Z-scheme heterojunctions, which were applied to active peroxydisulfate (PDS) for SMX degradation under visible light. The most efficient MNPx/PDS/vis system recorded a 99.2 % reduction in SMX concentration, with an associated reaction rate of 0.8873 min−1. This performance was superior to the PDI/PDS/vis and MIL-101(Fe)–NH2/PDS/vis systems, being 106.9-fold and 15.2-fold more effective, respectively. The Z-scheme heterojunction of the photocatalyst accelerated electron transport, inhibited electron-hole recombination, and improved the efficiency of PDS activation; meanwhile, the substantial surface area of the MIL-101(Fe)–NH2 provided additional reaction sites, these features synergize to enable the rapid removal of SMX. The MNPx/PDS/vis system degraded SMX at a higher rate under acidic and neutral conditions. Besides, degradation pathways for SMX have been proposed, and the biotoxicity of SMX as well as the by-products gradually decreased as the degree of degradation deepens. This study presented a simple strategy for the Z-scheme heterojunction photocatalyst preparation and a reference for the disposal of sulfamethoxazole-containing wastewater.
期刊信息：Sep. Purif. Technol
DOI：10.1016/j.seppur.2024.130292
论文链接：
7
题目：Rationally tailored configuration of multifunctional scavengers by encapsulating nanoscale Fe0 and FeS into zeolite imidazole framework–8 with reinforced perrhenate/pertechnetate confinement
作者：Zheyu Fan , Kedan Ding , Hongtao Zhu , Guodong Sheng*, Hongliang Dong
摘要：In order to probe into the potential application prospects of multifunctional scavengers in remediating nuclear wastewater, we combined versatile functionality of nanoscale Fe0 and FeS with tailorable porosity of zeolitic imidazole frameworks–8 (ZIF–8) to manufacture two multifunctional scavengers for ReO4– confinement i.e., NZVI@ZIF–8 by reduction approach and FeS@ZIF–8 by coprecipitation approach. Batch approaches unveiled that as–manufactured scavengers illustrated an reinforced performance towards ReO4– confinement. The pseudo-second-order model was well simulated with the kinetic of ReO4– confinement. Thermodynamic analysis unraveled that ReO4– confinement was endothermic and spontaneous. The mechanism was explored via characterization alters of structure and composition of NZVI@ZIF–8 and FeS@ZIF–8 before and after ReO4– confinement. Specifically, fourier transform infrared spectrometer (FTIR) and X-ray diffraction (XRD) indicated that NZVI and FeS were successfully encapsulated into ZIF–8, and NZVI@ZIF–8 and FeS@ZIF–8 remained stable after ReO4– confinement. X–ray absorption fine structure (XAFS) unveiled that various Fe mineral phases were formed on the scavenger surfaces under various reaction conditions. X-ray photoelectron spectroscopy (XPS) unraveled existence of Re(VI)/Re(IV) on scavengers surfaces, unveiling ReO4– was initially enriched NZVI@ZIF–8 and FeS@ZIF–8 surfaces with subsequent reduction into Re(VI)/Re(IV). This work proposed an innovative perspective to tailored multifunctional scavengers in nuclear waste management.
期刊信息：Sep. Purif. Technol
DOI：10.1016/j.seppur.2024.130199
论文链接：
8
题目：Insight into formaldehyde decomposition over MOFs-derived CeO2-MnOx bimetallic oxides
作者：Mingyue Zhu , Wei Liu , Wenjing Li , Peiao Cong , Daowei Gao , Xuchuan Jiang , Riming Hu* , Rongyao Wang* , Guozhu Chen*
摘要：The ubiquitous presence of formaldehyde as a pollutant has aroused significant environmental and health concerns. The design and performance of (OR: transition metal oxide) catalysts in the catalytic oxidation method continue to face a myriad of challenges. Herein, a series of CeO2-x-MnOx catalysts are synthesized using manganous nitrate impregnated Ce-metal–organic-frameworks as the precursor, followed by a traditional calcination step. Interestingly, we found that the gases released during the pyrolysis of metal–organic-frameworks significantly affect the valence states of Ce and Mn, which are key factors responsible for catalytic activity. Characterizations results show that the CeO2-x-MnOx-2.5 sample contains a large amount of Ce3+, a high Mn3+/Mn4+ ratio, and an abundance of reactive oxygen species on its surface. Density functional theory results demonstrate that oxygen vacancies not only effectively suppress charge loss of Mn and Ce atoms but also significantly enhance the adsorption strength of CeO2-x-MnOx-2.5 for both formaldehyde and O2. These structural features jointly influence the adsorption as well as the rapid oxidation of formaldehyde molecules, leading to the excellent catalytic performance towards formaldehyde oxidation. This study provides a promising platform for designing straightforward, cost-effective, and highly efficient bimetallic catalysts suitable for low-temperature formaldehyde oxidation.
期刊信息：Sep. Purif. Technol
DOI：10.1016/j.seppur.2024.130199
论文链接：
9
题目：Polyoxometalate-encapsulated metal–organic frameworks for photocatalytic uranium isolation
作者：Zhimin Dong, Dongling Zeng, Zifan Li, Junjie Chen, Youqun Wang, Xiaohong Cao, Guoping Yang*, Zhibin Zhang*, Yunhai Liua, Feng Yang*
Guan-Huang Zhang, Hai-Ling Wang, Lei Cheng*, Yun-Lan Li, Zhong-Hong Zhu*, Hua-Hong Zou*
摘要：Recycling uranium (U) via adsorption and controlled conversion is crucial for the sustainable development of nuclear energy, in which photocatalytic reduction of U(VI) from aqueous solutions is considered one of the most effective strategies. The primary challenge in the photocatalytic elimination of U(VI) resides in the demand for photocatalysts with exceptional properties for effective U(VI) adsorption and charge separation. Herein, we developed the hybrids of polyoxometalate@Cu-metal–organic frameworks (POM@Cu-MOFs) through a self-assembly strategy and demonstrated the efficient removal of U(VI) via synergistic adsorption and photocatalysis. The abundant oxygen-rich groups in POM served as the adsorption sites, endowing POM@Cu-MOFs with a remarkable removal capacity (1987.4 mg g−1 under light irradiation) to remove 99.4% of UO22+. The attraction of electrons from Cu atoms within Cu-MOFs effectively accelerated the carrier dynamics due to their pronounced electronegativity. A mechanism associated with the synergetic effects of adsorption and photocatalytic reduction of U(VI) was proposed. This work provides a feasible approach for efficiently eliminating U(VI) from aqueous solutions in environmental pollution cleanup using the POM@Cu-MOF photocatalyst.
期刊信息：Chem. Sci.
DOI：10.1039/D4SC05349D
论文链接：
声明：本文仅为了分享与交流学术成果，无任何商业用途。如涉及侵权，请联系我们及时修改或删除。
李书剑，男，北京建筑大学环境工程专业2023级硕士研究生，主要研究方向为金属-有机框架材料及其衍生物的设计、制备及其在水环境修复领域的应用。
扫描下方二维码|关注我们
新型环境修复材料与技术课题组
课题组网站链接：http://nmter.bucea.edu.cn
