JOURNAL OF MOLECULAR STRUCTURE
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2023
·
IF 3.8
Xiyue Wang,Shang Gao,Junfu Wang,Xinying Fan,Chi Song,Chuanwei Zhou,Shuyun Shi,Dandan Wang,Hongji Li
In this work, a novel sensor for selective detection of 2,6-dichlorophenol (2,6-DCP) is developed by combining the selectivity of molecular imprinting technology (MIPs) with the sensitivity of SERS technology. In order to enhance SERS activity of the substrate, Ag nanoparticles are loaded on Ta 2 O 5 particles by means of photodeposition. The synthesized Ta 2 O 5 @Ag is combined with MIL-101 (Fe) to enrich more target molecules and reduce the limit of detection. Finally, Ta 2 O 5 /Ag/MIL-101(Fe)@MIPs (TAM@MIPs) is synthesized by precipitation polymerization for selective detection of 2,6-DCP. When the concentration of 2,6-DCP changes between the range of 10 −2 ∼ 10 −9 M, the Raman intensity and concentration present a good linear relationship. The correlation coefficient (R 2 ) is 0.9969 and the limit of detection (LOD) of 2,6-DCP is 10 −9 M. Furthermore, Under UV-irradiation, the TAM@MIPs also presents photocatalytic performance, which can effectively degrade the organic interfering molecule adsorbed on its surface and present high-efficiency reproducibility. This method broadens the application field of SERS detection and provides a new procedure for the phenolic pollutant detection.
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CHEMICAL ENGINEERING JOURNAL
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2022
·
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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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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MICROCHIMICA ACTA
·
2021
·Vol. 188
·期 10
·1-11
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IF 5.833
Qin
Peige,Han Lizhen,Zhang Xiaowan,Li Mengyuan,Li Dan,Lu Minghua,Cai Zongwei
Abstract Using MIL-101(Fe) as the source of carbon and Fe, a magnetic porous carbon (MPC) material with Fe 3 C nanoparticles encapsulated in porous carbon was prepared through one-pot pyrolysis under N 2 atmosphere. With MPC as adsorption material, a stir bar sorptive-dispersive microextraction (SBSDME) method was proposed to extract and preconcentrate sulfonamides (SAs) prior to HPLC-DAD determination. To investigate their extraction ability, different MPC materials were prepared under different carbonization temperatures (600, 700, 800, 900, and 1000 °C). The material prepared under 900 °C (MPC-900) exhibited the highest extraction ability for SAs. The as-prepared MPC materials were also characterized by Raman spectroscopy, scanning electron microscopy, X-ray photoelectron spectroscopy, zeta potential, and other techniques. The main parameters that affect extraction were systematically studied. Under optimal conditions, favorable linearity ( R 2 ≥ 0.9938) and detection limits (0.02–0.04 ng mL −1 ) of sulfonamides were obtained. The average recoveries for spiked milk and lake water samples ranged from 76.9 to 109% and from 75.4 to 118% with RSDs of 3.10–9.63% and 1.71–11.3%, respectively. Sulfameter and sulfisoxazole were detected in milk sample. Sulfisoxazole was detected in the lake water sample. The MPC-900 material demonstrated excellent reusability. It can be reused 24 times with peak areas having no obvious decline. The method can be applied to extract ultra-trace compounds in complex sample matrices. Graphical abstract
Schematic presentation of a stir bar sorptive-dispersive microextraction (SBSDME) by using magnetic porous carbon (MPC) composites as sorbent combined with high-performance liquid chromatography for sensitive analysis of sulfonamides in milk and lake water samples.
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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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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2022
·
IF 4.326
Jiakang Wan,Ling Wang,Wentao Xu,Zehai Xu,Junsheng Yuan,Guoliang Zhang
Design and synthesis of high-efficiency and stable heterogeneous catalysts for the electro-Fenton process remain challenging. In this study, a co-doped Ce and N metal–organic framework MIL-101(Fe) heterogeneous catalyst (Ce/N-MIL-101(Fe) was synthesized by a facile one-step solvothermal method. Polyvinyl pyrrolidone played dual roles during the fabrication process, which not only acted as a nitrogen source for doping but also prevented MIL-101(Fe) molecules from aggregating and reinforcing the formation crystal with a complete polyhedral crystal shape. The introduction of Ce significantly enhanced the density of active sites and promoted the Fe3+/Fe2+ cycle of the reaction system. Owing to the specific structure and properties, the rate of electron transfer in the catalytic process was significantly promoted. The synthesized Ce/N-MIL-101(Fe) catalyst exhibited a high degradation rate for dyes (>98%) with competitive stability and reusability. Moreover, compared with common electro-Fenton catalysts usually operated in a limited pH range of 3.0–6.0, the working pH range of Ce/N-MIL-101(Fe) was widened up to 10.0. The design concept for producing abundant active sites with co-doping into frameworks can be extended to more heterogeneous electro-Fenton catalysts constituted by other porous materials.
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Surfaces and Interfaces
·
2024
·
IF 5.7
Qian Cheng,Xiaohan Liu,Chuhan Huang,Hongman Sun,Fazle Subhan,Xinyi Zhou,Yuankai Liu,JiaHui Yang,Qi Li,Youhe Wang,Zifeng Yan
Recently, there has been a growing interest in the fundamental understanding of the mechanism of how MIL-101(Fe)/g-C 3 N 4 heterojunctions facilitate the occurrence of photocatalytic nitrogen fixation reactions, especially the electron transfer mechanism has attained increasing attention in photocatalysis. Herein, we implemented a "triple win scenario" strategy to fabricate the S-scheme MIL-101(Fe)/g-C 3 N 4 heterojunction through a straightforward solvothermal process. The MC-6 heterojunction minimizes the recombination of photogenerated carriers, enhances light utilization efficiency, and activates the N≡N bond, thus boosting photocatalytic nitrogen fixation efficiency. The transition metal iron activates the N≡N bond, while S-scheme heterojunctions reduce the photogenerated carrier recombination. In addition, the decrease in band gap (E g ) leads to an increase in visible light utilization efficiency. ISIXPS proved the mechanism of interelectron transfer of MIL-101(Fe)/g-C 3 N 4 heterojunction under illumination. Upon the creation of the heterojunction, electrons migrate from g-C 3 N 4 to MIL-101(Fe), establishing an inherent electric field due to the disparate Fermi levels between the two materials. The electrons (e - ) on the g-C 3 N 4 CB with a more negative reduction potential and the holes ( h + ) on the MIL-101(Fe) VB are retained, which increased the redox capacity to a great extent required for the reduction of N 2 to NH 3 . The ammonia production efficiency of MC-6 photocatalyst was 160 µmol g cat -1 h -1 , representing an 8-fold and 2.8-fold improvement over pristine g-C 3 N 4 (20 µmol g cat -1 h -1 ) and MIL-101(Fe) (57 µmol g cat -1 h -1 ), respectively.
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CARBOHYDRATE POLYMERS
·
2025
·
IF 12.5
Sa Liu,Yapeng Chen,XinKuan Li,Yijia Yao,Huashan Wang,Meiyi Wang
Food packaging films containing antimicrobial reagents play a crucial role in preventing bacterial-induced fruit decay. This study proposes a bilayer film consisting of an internal amino-modified starch hydrophilic layer and an external amino-modified polyvinyl alcohol/polylactic acid hydrophobic layer, embedding alliin@MIL-101(Fe) as an antibacterial agent, utilizing the pH reduction of fruit decay sites to achieve pH-responsive release, enhancing antibacterial performance. Fourier transform infrared (FTIR) and scanning electron microscopy (SEM) analyses confirm successful crosslinking between amino and aldehyde groups, resulting in the formation of imine bonds and a mesh-like structure conducive to adsorption. Under acidic conditions, the cumulative release rate of alliin reached 74 % within 36 h. Compared to a simple mixture, the tensile strength of the alliin@MIL/NST-NPVA/PLA film reached 34.771 MPa, and transmittance in the wavelength range of 200–370 nm decreased to 0. The scavenging rate of DPPH free radicals in the film can reach 83 %. In addition, the water vapor permeability and oxygen permeability of the film are approximately 7.62 × 10 −16 [g/ (m 2 ‧24 h‧0.1 mm)] and 6.83 (m 2 ‧24 h‧0.1 MPa), respectively; moisture content and water solubility decreased to 10.99 % and 20.77 %. This composite film extended the shelf life of strawberries from 2 to 7 days, significantly enhancing freshness.
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
·
2024
·Vol. 25
·期 18
·9855
·
IF 4.9
Yiting Luo,Rongkui Su
Tetracycline’s accumulation in the environment poses threats to human health and the ecological balance, necessitating efficient and rapid removal methods. Novel porous metal–organic framework (MOF) materials have garnered significant attention in academia due to their distinctive characteristics. This paper focuses on studying the adsorption and removal performance of amino-modified MIL-101(Fe) materials towards tetracycline, along with their adsorption mechanisms. The main research objectives and conclusions are as follows: (1) NH2-MIL-101(Fe) MOF materials were successfully synthesized via the solvothermal method, confirmed through various characterization techniques including XRD, FT-IR, SEM, EDS, XPS, BET, and TGA. (2) NH2-MIL-101(Fe) exhibited a 40% enhancement in tetracycline adsorption performance compared to MIL-101(Fe), primarily through chemical adsorption following pseudo-second-order kinetics. The adsorption process conformed well to Freundlich isotherm models, indicating multilayer and heterogeneous adsorption characteristics. Thermodynamic analysis revealed the adsorption process as a spontaneous endothermic reaction. (3) An increased adsorbent dosage and temperature correspondingly improved NH2-MIL-101(Fe)’s adsorption efficiency, with optimal performance observed under neutral pH conditions. These findings provide new strategies for the effective removal of tetracycline from the environment, thus holding significant implications for environmental protection.
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CHEMICAL PHYSICS LETTERS
·
2025
·
IF 3.1
Kangyue Qiao,Songyao Du,Yue Wang,Tongxin Xiao,Guodong Hao,Chao Sui,Yihan Yan
To address the severe Cr(VI) contamination in industrial wastewater, an NH 2 -MIL-101(Fe)/g-C 3 N 4 type-II heterojunction photocatalyst was synthesized via a solvothermal one-pot method. Structural characterization using XRD, SEM, XPS, and BET confirmed successful composite formation with high specific surface area and favorable interfacial contact. Photocatalytic experiments revealed that under conditions of pH = 2, a catalyst dosage of 20 mg, and an initial concentration of 10 mg/L, NM-101(Fe)/0.2CN achieved a 99.5 % reduction efficiency within 80 min. Its reaction rate constant was 3.6 times higher than that of NM-101(Fe) used alone. This study provides new insights for developing highly efficient MOF/polymer composite photocatalysts.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2024
·Vol. 31
·期 16
·23924-23941
·
IF 0
Li Kaiqian,Zhang Xupeng,Huang Xueqin,Li Xianghong,Chang Qiaowen,Wang Jing,Deng Shuduan,Zhu Gang
In response to the escalating concerns over antibiotics in aquatic environments, the photo-Fenton reaction has been spotlighted as a promising approach to address this issue. Herein, a novel heterogeneous photo-Fenton catalyst (Fe 3 O 4 /WPC) with magnetic recyclability was synthesized through a facile two-step process that included in situ growth and subsequent carbonization treatment. This catalyst was utilized to expedite the photocatalytic decomposition of ciprofloxacin (CIP) assisted by H 2 O 2 . Characterization results indicated the successful anchoring of MIL-101(Fe)-derived spindle-like Fe 3 O 4 particles in the multi-channeled wood-converted porous carbon (WPC) scaffold. The as-synthesized hybrid photocatalysts, boasting a substantial specific surface area of 414.90 m 2 ·g −1 and an excellent photocurrent density of 0.79 μA·cm −2 , demonstrated superior photo-Fenton activity, accomplishing approximately 100% degradation of CIP within 120 min of ultraviolet-light exposure. This can be attributed to the existence of a heterojunction between Fe 3 O 4 and WPC substrate that promotes the migration and enhances the efficient separation of photogenerated electron–hole pairs. Meanwhile, the Fe(III)/Fe(II) redox circulation and mesoporous wood carbon in the catalyst synergistically enhance the utilization of H 2 O and accelerate the formation of •OH radicals, leading to heightened degradation efficiency of CIP. Experiments utilizing chemical trapping techniques have demonstrated that •OH radicals are instrumental in the CIP degradation process. Furthermore, the study on reusability indicated that the efficiency in removing CIP remained at 89.5% even through five successive cycles, indicating the structural stability and excellent recyclability of Fe 3 O 4 /WPC. This research presented a novel pathway for designing magnetically reusable MOFs/wood-derived composites as photo-Fenton catalysts for actual wastewater treatment.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Quan Huo,Gongquan Liu,Haihui Sun,Yanfei Fu,Yao Ning,Boyu Zhang,Xubiao Zhang,Jing Gao,Jiarun Miao,Xiaolin Zhang,Suyan Liu
CeO 2 /MIL-101(Fe) catalysts for a photocatalysis-extraction oxidation desulfurization (PEODS) system were designed by introducing different amounts of CeO 2 into MIL-101(Fe). And, the materials were further analyzed via some characterization technologies. Moreover, an optimization system, composed of CeO 2 /MIL-101(Fe), extractant acetonitrile and oxidant H 2 O 2 , was selected to remove dibenzothiophene (DBT) from model oil under visible-light irradiation. Evaluation results illustrated that 90% of DBT in oil phase was able to be transformed within 2 h as the adding amount of CeO 2 , the volume ratio of model oil to acetonitrile and the molar ratio of H 2 O 2 to DBT was 60 mg, 2:1 and 3:1, respectively. Radical scavenger experiments verified that · OH and · O 2 – were main reactive species in the process. The high photocatalytic activity was originated from a synergic effect produced between active sites of CeO 2 and active surface of MIL-101(Fe) and formed heterostructure in the catalyst, which broadened optical response ranges and facilitated photoinduced charge separations and transfers. Additionally, a convinced PEODS mechanism was proposed and rationalized.
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