CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Yi-Hao Tong,Yu-Zhe Wu,Zhen-Liang Xu,Li-Han Luo,Sun-Jie Xu
This work was expected to develop a new loose NF membrane with facile materials to conduct dye/salt separation and endow it with versatile capacities to offer an applicable solution to treat textile wastewater. Ethylene vinyl alcohol (EVAL) was first chosen to fabricate loose nanofiltration (NF) membrane through non-solvent induced phase separation (NIPS) method. Besides, MIL-101(Fe) showed outstanding photocatalytic capacity in degrading organic molecules while a low-cost bio-inspired coating, catechol, was utilized to modify MIL-101(Fe). A combination of modified MIL-101(Fe) and EVAL could have a high water permeability (43.2 L·m −2 ·h −1 ·bar −1 ) with superior rejection to small molecule negative charged dyes (Chlorazol black T: 99.8%, Congo Red: 99.7%, Eriochrome black T: 98.4%) and low rejection to various salts (Na 2 SO 4 : 4.8 %, NaCl: 2.1 %, MgCl 2 : 2.9%, MgSO 4 : 4.9% and CaCl 2 : 3.3%). Meanwhile, the EVAL loose NF membrane with the best performance had excellent antifouling capacity and long-term stability in EBT/Na 2 SO 4 separation. Moreover, the membrane could degrade dyes to self-clean the membrane surface through photocatalytic process, which originated from the Fe-O clusters in MIL-101(Fe).
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Inorganics
·
2022
·Vol. 10
·期 5
·59
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IF 3.149
Sander Dekyvere,Mohamed Elhousseini Hilal,Somboon Chaemchuen,Serge Zhuiykov,Francis Verpoort
MOF-derived carbon-based materials have attracted widespread attention due to their relatively large surface area, morphology, and their stability in water. Considering these advantages, these materials present themselves as excellent adsorbents. In this work, a novel method was designed for the fabrication of a nano zero-valent-iron (nZVI) carbon composite. The utilization of zinc oxide nanorods (ZnONRs) in the role of sacrificial consumable nuclei for the synthesis of MIL-53 sacrificial zinc oxide nanorods (MIL-53-SNR) and the subsequent pyrolysis at 700 °C in the inert atmosphere led to a graphitic-supported nZVI material (Fe-C-SNR). Fe-C-SNR was compared with a commercial zinc oxide bulk (MIL-53-SB) and with a pristine MIL-53. By virtue of the ZnONRs, Fe-C-SNR exhibited a greatly improved mesoporous structure. Consequently, the pyrolyzed materials were applied as adsorbents for methylene blue. Fe-C-SNR’s performance increased to more than double of the pyrolyzed MIL-53 (Fe-C), with a remarkably fast adsorption time (10 min) for a concentration of 10 mg L−1with only 200 mg L−1adsorbent required. This functional composite also displayed exceptional recyclability; after ten complete cycles, Fe-C-SNR was still capable of completely adsorbing the methylene blue. The utilization of ZnONRs proves itself advantageous and could further be extended to other MOFs for a wide range of applications.Keywords:mesoporous material;zero-valent-iron nanoparticles;methylene blue adsorption;metal–organic framework
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Journal of Water Process Engineering
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2022
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IF 7.34
JongNam Choe,JongMin Ji,MyongBok Kim,JuHyon Yu,JongYol Ri,KyongSu Ri,HyonIl Kim
In this paper, a novel hydrophilic composite polyethersulfone (PES) ultrafiltration membrane was prepared by blending sunlight response photocatalyst NH 2 -MIL-125 via the phase inversion method. The physical-chemistry performance of membrane was carried out by XRD, FTIR, UV-VIS/DRS, contact angle, and cross-section SEM images. The separation ability, anti-fouling ability, and self-cleaning efficiency of ultrafiltration membrane were analyzed by ultrafiltration experiment using the congo red solution. The results indicate that fouling resistance and the flux recovery ratio of ultrafiltration membrane is significantly improved, and it has higher solar response energy. There was no significant change in the rejection ratio of pollutants before and after illumination. For the pristine PES membrane and the 0.5% NH 2 -MIL-125/PES nanocomposite membrane, the water flux recovery ratio (FRR) could increase from 37.84% to 77.09%, and the R r could increase from 22.22% to 44.09%, and the R ir could decrease from 67.11% to 47.09%. In a conclusion, the addition of NH 2 -MIL-125 at a low concentration could result in membranes with more pure water flux, better rejection, and good fouling resistance compared to the unfilled PES membrane.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Yucheng Li,Xiangyu Wang,Zhengyin Duan,Dehai Yu,Qiang Wang,Dandan Ji,Wenxia Liu
Treating dye-contaminated wastewater using the visible light–driven photo-Fenton reaction is beneficial to environmental remediation. This paper reports the synthesis of a novel, highly effective photo-Fenton catalyst, the Zn/Co-ZIFs@MIL-101(Fe) composite, by a facile internal-growth method. The composite, which had an MOF-in-MOF structure, activated H 2 O 2 to decompose RhB, a polluting-dye model, under visible-light illumination. The transfer of the electron–hole pair was synergistically accelerated by the reaction centers of the composite (the MIL-101(Fe) shell and Zn/Co-ZIFs core), which enhanced H 2 O 2 activation. The generated OH, O 2 − , and 1 O 2 effectively decomposed RhB. The composite’s catalytic performance was significantly enhanced by the electronic hybridization of its Fe 3+ , Co 2+ , and Zn 2+ metal centers. Thus, the composite demonstrated a remarkable capability to remove RhB. The composite polymetallic MOFs loaded with 3% Zn/Co-ZIFs prepared by us showed good reusability and water stability, and their morphology and structure did not change significantly after four runs, depending on the iron, cobalt, and zinc metal leaching concentrations 0.134 mg/L, 0.06 mg/L and 0.054 mg/L respectively. This study provides a novel method to construct an Zn/Co-ZIFs@MIL-101(Fe) catalyst with dual reaction centers that enhance the transfer of electron–hole pairs. Our findings inspire the application of MOF-based photo-Fenton catalysts to wastewater treatment and environmental remediation.
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CHINESE JOURNAL OF ANALYTICAL CHEMISTRY
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2022
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IF 1.193
Yan-Yan XING,Mei-Ling CHEN,Xin-Ai SHEN,Ning LIANG,Xiao-Hong HOU
In consideration of the promising application of peroxidase (POD)-like nanozymes in biomedical analysis, the development of POD mimics with good catalytic performance under neutral conditions remains significant. As a new catalyst, metal-organic frameworks have been explored as candidate nanozymes owing to their high catalytic activity, good stability, flexible and simple synthesis methods, diverse types, and properties. Herein, rod-like Fe-MIL-88A was successfully synthesized via a simple hydrothermal method. Fe-MIL-88A exhibited POD-like properties under neutral conditions and a stronger affinity for substrate 3,3 ' ,5,5 ' -tetramethylbenzidine and H 2 O 2 than natural horseradish POD. This result was primarily due to the additional exposed (100) facets of rod-like Fe-MIL-88A, which can catalyze the decomposition of H 2 O 2 to •OH more easily. Based on the POD-like properties of Fe-MIL-88A under neutral conditions, combined with glucose oxidase, a one-pot colorimetric analysis method for glucose detection was established. The proposed measurement had a linear range of 1–100 µM and a limit of detection of 0.45 µM. The colorimetric method was accurate, reliable, highly selective, convenient, and time-saving. Furthermore, the one-pot method was successfully applied to detect the concentration of glucose in human blood samples, and the measured results were consistent with those of commercial glucose meters, indicating that the proposed method can be a potential candidate for glucose detection.
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JOURNAL OF MOLECULAR STRUCTURE
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2022
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IF 3.841
Wei Zhang,Yong-Zhuan Zhang,Ji-Min Yang
The separation of synthetic dyes from industrial wastewaters is an important objective in addressing water pollution. The removal of pollutant dyes from industrial wastewater prior to its release into the environment is an essential task; thus, synthesizing new adsorbent materials with superior adsorption efficiency is an important undertaking. Herein, we report the synthesis of MIL-100(Fe)@GO (graphene oxide) composites exhibiting superior adsorption performance toward methyl orange (MO), Congo red (CR), methylene blue (MB), and acid chrome blue K (AC). The room-temperature adsorption capacities of MIL-100(Fe)@GO-1 for these dyes were 533.7 (MB), 760.1 (MO), 1386.3 (AC), and 1786.6 (CR) mg g –1 , exceeding those values previously reported for pristine MIL-100(Fe) by 31.1%, 17.8%, 54.8%, and 8.9%, respectively. The adsorption behavior of the composites can be described on the basis of the structural and morphological characteristics and zeta potential of MIL-100(Fe)@GO and the adsorption capacity and structural characteristics of the dyes. The adsorption uptakes of MIL-100(Fe)@GO toward the pollutant dyes was controlled by the synergistic effects of the hydrogen-bonding, hydrophobic interactions, and π–π interactions and agglomeration pores of MIL-100(Fe)@GO. The obtained results revealed that the synergetic interplay of electrostatic, hydrogen-bonding, π–π, and hydrophobic interactions and adsorption space led to two distinct adsorption regimes for MO and AC depending on the adsorbate concentration.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Xuedong Du,Wenyang Fu,Pei Su,Qizhan Zhang,Minghua Zhou
The reduced S-modified MIL-53(Fe) was prepared by sulfurizing MIL-53(Fe) at low temperature, which was an efficient electro-Fenton catalyst at wide pH range (3–9) for sulfamethazine (SMT) degradation. The best temperature and MIL-53(Fe)/S ratio were 350 °C and 1:2, at which the BET surface area was much enlarged. The MIL-53(Fe) surface was etched by S to many 2D nanosheets with the thickness of ~50 nm, while S 2–2 replaced OH - to coordinate with Fe 2+ and increased the Fe 2+ content, which improved the catalytic performance. Even at initial pH of 7.0, the SMT removal was 95.8%, and the rate constant ( k ) in the Hetero-EF process was 16-folds of that in the Homo-EF process. The turnover frequency (TOF d ) value of MIL-53(Fe)/S(1:2)−350 was 0.48 L g −1 min −1 , which was 6.8 times that of commercial FeS 2 . The S 2–2 in catalyst adjusted the pH superfast, and promoted the generation of Fe 2+ and thus efficiently activating H 2 O 2 to form surface · OH, which was verified to be the main radical by EPR and radical scavenger experiments. This catalyst showed promising prospect for environmental application and could be regenerated by sulfidation method. S-doped MIL-53(Fe) was an excellent pH regulator, thus promoting promising application in Hetero-EF processes.
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PubMed
高影响因子
FOOD CHEMISTRY
·
2023
·
IF 8.8
Yu-Han Sun,Liu Yang,Xian-Xian Ji,Yuan-Zhen Wang,Yu-Long Liu,Ying Fu,Fei Ye
Flusilazole is a triazole fungicide with residues that are potentially toxic to humans. It enters the human body mainly through food, although its bactericidal activity is substantial. In this study, an electrochemical sensor Fe/Fe 2 O 3 @C with a core–shell structure was constructed to efficiently detect flusilazole by annealing MIL-53(Fe) which was prepared by a simple solvothermal method. Transmission electron microscopy and scanning electron microscopy were used to characterize the apparent morphology of MIL-53(Fe) and Fe/Fe 2 O 3 @C , and their structures were further characterized by X-ray photoelectron spectroscopy, Raman spectroscopy, powder X-ray diffraction, and the mapping of elements by energy dispersive spectroscopy. The electrochemical behavior of Fe/Fe 2 O 3 @C in the detection of flusilazole was evaluated by differential pulse voltammetry under optimal conditions. The results of the study indicate that the Fe/Fe 2 O 3 @C electrochemical sensor displayed excellent detection capabilities for flusilazole, where the sensor exhibited a wide detection range from 1.00 × 10 −4 to 1.00 × 10 −12 mol/L with an incredibly low LOD of 593 fM, making it highly sensitive to trace amounts of flusilazole. Moreover, Fe/Fe 2 O 3 @C demonstrated superior reproducibility, stability, and resistance to interference, highlighting its reliability in practical applications. The sensor was also successfully utilized to quantitatively detect flusilazole in various real samples, which suggests that Fe/Fe 2 O 3 @C has broad-spectrum environmental resistance and can effectively and rapidly detect flusilazole residues in different types of food items and environmental matrices. The study also delved into the mechanism of Fe/Fe 2 O 3 @C for the detection of flusilazole, providing a deeper understanding of the functionality of this sensor. Overall, these findings emphasize the practical significance of Fe/Fe 2 O 3 @C as an electrochemical sensor, showcasing its potential for real-world applications in food safety and environmental monitoring.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Xiaohan Guo,Yanfang Liu,Hongxiang Zhu,Xiaohui Yu,Feng Shi,Qinqin Liu,Qiang Liu,Ying Xu
Asp donates electrons to reprogram Fe O clusters of MIL-53(Fe). • This electronic switch redirects dominant ROS from •OH to •O 2 − . • The mechanism enables neutral-pH POD-like activity of MIL-53(Fe)@Asp. • The Asp-modified nanozyme integrates with GOX for cascade glucose sensing. MIL-53(Fe) exhibits peroxidase-like activity only under acidic conditions, limiting its biosensing applications. We overcome this by using aspartic acid (Asp) as a structure-directing agent to modify MIL-53(Fe) (MIL-53(Fe)@Asp) via hydrothermal synthesis followed by Asp coordination. Unlike conventional pH-reduction strategies, Asp modification does not alter bulk pH but induces intrinsic electronic restructuring of Fe O clusters, as confirmed by increased Fe 3+ /Fe 2+ ratio and introduction of N → Fe coordination (XPS). At pH 6.9, the TMB-based activity of MIL-53(Fe)@Asp is 27-fold higher than that of pristine MIL-53(Fe). Steady-state kinetics show favorable Km values (TMB 0.27 mM, H 2 O 2 1.38 mM) at neutral pH. Mechanistic studies (ROS identification, EPR, band structure, DFT) reveal that Asp exerts an electron-donating effect that reprograms the electron distribution of Fe O clusters, activating the otherwise inactive MIL-53(Fe) framework at neutral pH and diversifying the catalytic pathways to include a less pH-dependent •O 2 − route alongside the partially maintained •OH pathway. This pathway diversification enables efficient neutral-pH peroxidase-like catalysis, with •O 2 − as the dominant pathway. Leveraging this, we construct a cascade nanoplatform (MIL-53(Fe)@Asp@GOX) integrating glucose oxidase, which exhibits excellent cascade activity at neutral pH. The method is applied to glucose detection in blood and saliva, demonstrating good linearity, precision, selectivity, and recovery. The glucose concentrations determined by our sensor correlated well with those obtained using a commercial assay kit. Notably, the limit of detection for glucose in saliva reaches 2.08 μM, offering a promising route toward non-invasive glucose sensing. This work establishes a design principle for creating pH-adaptive catalytic microenvironments in Fe-MOFs through electronic restructuring and pathway diversification, overcoming a long-standing limitation of MIL-53(Fe) for biomedical applications. Download: Download high-res image (111KB) Download: Download full-size image
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 46
·21505-21512
·
IF 3.3
Yuhao Lu,Tao Wang,Chengshun Tang,Qijian Niu,Tianyan You
Oxytetracycline (OTC) residues in the environment seriously endanger ecosystems and human health. Hence, it is critical to develop a selective and sensitive sensor for trace OTC detection. In this work, a facile and highly selective colorimetric aptasensor was constructed for OTC detection by the surface electrostatic assembly between aptamers and Fe-MOFs. Due to the steric effects and the decrease in the electron transfer rate, the peroxidase-like activity of NH2-MIL-88B was significantly inhibited after the adsorption of aptamers. Furthermore, the selective binding between aptamers and OTC triggered the release of aptamers from the surface of NH2-MIL-88B, which led to the reactivation of peroxidase-like activity. The colorimetric aptasensor exhibited a satisfactory detection range (1.0 × 10−10 M to 3.0 × 10−7 M) and the limit of detection (LOD) was as low as 1.9 × 10−11 M. Additionally, the colorimetric aptasensor was successfully used to detect OTC in real samples. The developed colorimetric aptasensor provided an important reference value for the sensitive detection of other antibiotics in the environment.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2023
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IF 5.2
Yan Gao,Shumin Zhao,Miao Yan,Yongxia Li,Jianshe Zhao
In this work, the encapsulating peroxo-polyoxometalate in the mesoporous of metal-organic framework (MIL-101(Fe)) to synthesize composite according to the principle of host-guest matching. The structure of the host-guest composite was analyzed by a variety of methods, and the catalytic activity for desulfurization was investigated under mild conditions. The composites combine the advantages of peroxo-polyoxometalate (high efficiency) and MIL-101(Fe) (good recyclability and high porosity), showing synergistic effect between host and guest. The sulfur-containing organic compounds in simulated liquid fuel can be almost completely removed under the catalysis of PW 4 @MIL-101(Fe). The catalyst PW 4 @MIL-101(Fe) can be reused for 10 times without prominent decrease in desulfurization activity, indicating that it has good reusability due to the confinement effect between the window size of MIL-101(Fe) and molecular size of PW 4 . In addition, several control experiments and electron spin resonance experiment were researched to explore the possible mechanism, and the results show that the active component in the catalyst can promote the decomposition of H 2 O 2 into ·OH and thus accelerate the desulfurization reaction. This work discloses a facile and environmentally friendly method to prepare the "host-guest matching" catalyst with high activity and stable reusability, which provides ways for further developments in heterogeneous catalyst based on POM and MOF.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Chenxi Shi,Kunpeng Wang,Chongchong Chen,Yijun Cao,Guoli Zhou,Jingtao Wang,Cong Li
Gallium, with an average content of about 15 μg g −1 in the Earth's crust, ranks at the forefront of strategic metals. However, the separation of gallium remains challenging due to the similar physical and chemical properties of gallium and other impurity ions. Herein, the tetradentate amidoxime-functionalized MIL-53(Al) nanofiber membranes (PAN/MIL-53-AO) are prepared to separate gallium, aluminum, vanadium ions and so on. The resultant membranes display 231.08 mg g −1 for Ga(Ⅲ) with high selectivity in static and dynamic adsorption. Specially, PAN/MIL-53-AO demonstrates excellent gallium regeneration rate of 84.25% after five cycles. According to DFT calculations, due to the tetradentate structure of MIL-53(Al)-AO, the amidoxime group binds to gallium ion with a lower binding energy (−29.46 eV). In conclusion, the experimental dates and theoretical calculations indicate that the excellent adsorption capacity is derived from the high binding ability of unique rhombic tetragonal coordination structure for gallium ion and the specific MIL-53(Al) cavity size for passage of gallium. Such performances outperform most state-of-the-art adsorption membranes. The special structure of MOF pores provides a novel approach for rapid synthesis of adsorption sites with high selectivity, with potential utilization in the selective adsorption of gallium ions.
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