CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Jin Liu,Zhirui Fan,Wenzhe Zhao,Peipei Song
Recently, escalating antibiotics contamination in aquatic environments has become a critical global threat to public health. In this study, a novel cathode catalyst (NH 2 -MIL-101(Fe)@Mel-MoPc/BC) was fabricated via hydrothermal method for efficient degradation of ofloxacin (OFX) through an electro-activated peroxymonosulfate (PMS) system. The incorporation of Mo-C and Fe/Mo-N substantially enhanced the electrocatalytic performance. The influence of various parameters, including the internal mass ratio of the catalyst, current, PMS concentration, OFX concentration, pH, as well as electrolyte concentration and type on OFX degradation were systematically evaluated. Under optimal conditions, OFX degradation reached 92.6 %, with 84.2 % total organic carbon removal, outperforming previous studies. The free radical quenching experiment and electron paramagnetic resonance analysis identified singlet oxygen ( 1 O 2 ) as the dominant active species. In situ Raman spectroscopy, high performance liquid chromatography-mass spectrometry and density functional theory calculation elucidated the degradation mechanism and pathways of OFX, including demethylation, decarboxylation, hydroxylation, and dehydrogenation, ultimately forming water, carbon dioxide, and inorganic ions. Furthermore, computational toxicology and seed germination tests confirmed significantly reduced wastewater toxicity after treatment by electro-activated PMS system based on NH 2 -MIL-101(Fe)@Mel-MoPc/BC cathode. Additionally, it also exhibited superior cyclic stability and excellent performance in various real water matrices and for other organic pollutants such as Rhodamine B, phenol, tetracycline, and dimethyl phthalate, demonstrating great application potential. This work provides valuable insights into cathode catalyst design and establishes a sustainable technology for antibiotic wastewater treatment.
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APPLIED SURFACE SCIENCE
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2022
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IF 7.392
Qinchao Shao,Xiubin Zhang,Pei Liang,Qiang Chen,Xiaohua Qi,Mingqiang Zou
Fabrication of a magnetic substrate based on metal–organic frameworks (MOFs) with high sensitivity and stability for surface-enhanced Raman scattering (SERS) analysis were reported in this paper. MIL-101(Cr) nanoparticle prepared via a traditional hydrothermal reaction, which was combined with Fe 3 O 4 to synthesize the Fe 3 O 4 /MIL-101(Cr) composites. Then, the concentration of chloroauric acid and the time of reduction reaction were adjusted to acquire the optimal Au/Fe 3 O 4 /MIL-101(Cr) (AF-MIL) SERS substrate. The detection ability of the substrate can down to 10 -8 mol/L for Rhodamine 6G (R6G) as probe molecule, and the relative standard deviation (RSD) is only about 4.48 %, which indicates that it possesses wonderful SERS performance and uniformity. Finally, the as-synthesized substrate has been adopted to test the trace level sulfapyridine, with its desirable detection ability can down to 10 -6 mol/L. Such desirable SERS substrate with facile and effective operation holds great promise in the fast sensitive detection of the antibiotic residue and some other pollutants in environment.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Yanqing Cong,Yanan Li,Xiaoran Wang,Xing Wei,Lin Che,Shi-Wen Lv
In this study, a double p-n heterojunction based on g-C 3 N 4 @NiO/Ni@MIL-101 ternary composite was successfully prepared by a feasible method. Results suggested that the rational growth of NiO and MIL-101 on the surface of g-C 3 N 4 can improve the absorption capacity for visible light. Importantly, the formation of double p-n heterojunction can effectively inhibit the recombination of photogenerated electrons and holes. Due to the significant Fermi level differences among NiO, MIL-101 and g-C 3 N 4 , the internal electric fields were established on the interface after constructing the composite, consequently reducing the electrical resistance and accelerating the transfer of photoinduced charge carriers. As expected, the g-C 3 N 4 @NiO/Ni@MIL-101 ternary composite with good stability had excellent photocatalytic performance in the degradation of emerging pollutants, and the removal efficiency of ibuprofen was as high as 95.6%. The •O 2 − , •OH and 1 O 2 were the major active species in the reaction system. Furthermore, developed photocatalytic oxidation system can also achieve the rapid inactivation of bacteria. Based on the synergistic effects of energy band position and double internal electric fields, the separation and transfer of photogenerated charge carriers followed a traditional type-II route. In short, current work not only constructed a promising photocatalyst, but also shared an effective strategy for boosting the photocatalytic activity.
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JOURNAL OF MOLECULAR STRUCTURE
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2022
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IF 3.841
Lulu Wang,Jing Lu,Yujia Wang,Haiyan Wang,Jilin Wang,Tieqiang Ren
In this study, a series of MIL-101-X catalysts were prepared by confining acidic ionic liquid phosphotungstate in MIL-101 nanocages using the organic electron-rich N-heterocyclic compound as a chemical bridge and the aforementioned catalysts were used for the oxidation of cyclohexene to adipic acid. During the aforementioned process of post-synthetic modification, a Bronsted acidic ionic liquid phosphotungstate ([C 3 SO 3 Hnhm] 3 PW 12 O 40 ) was synthesized in the nanocage of MIL-101. The research results reveal that the yield of adipic acid for the cyclohexene oxidation catalyzed by the constructed MIL-101-X catalyst was up to 78.16% in solvent-free condition. And its catalytic activity is not significantly reduced after six cycles. The novel catalyst synthesized in this paper combines the common advantages of ionic liquid phosphotungstate and MIL-101 nanocage microenvironment to facilitate the diffusion of reactants and their interaction with the catalytic activity center. This research will provide a new idea to solve the problem in terms of the shortage of efficient catalysts in the field of catalytic oxidation of cyclohexene to adipic acid.
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MICROCHIMICA ACTA
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2020
·Vol. 187
·期 6
·1-9
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IF 6.232
Qin Peige,Zhu Wenli,Han Lizhen,Zhang Xiaowan,Zhao Bing,Zhang Xuebin,Lu Minghua
The monodispersed mesoporous SiO 2 @metal-organic framework (MSN@MIL-101(Fe)) composites were prepared by grafting MSN-NH 2 onto MIL-101(Fe) particles with a solvothermal method. The adsorption ability of the composites was greatly improved compared to that of pristine MSNs or MIL-101(Fe) for phytohormones (Phys). The MSN@MIL-101(Fe) composites were characterized by scanning electron microscopy, transmission electron microscopy, Fourier transform infrared spectroscopy, X-ray diffraction, energy dispersive spectrometer, and mapping analysis. Using MSN@MIL-101(Fe) composites as sorbent, a dispersive solid-phase extraction procedure (dSPE) was developed to extract three endogenous Phys (abscisic acid (ABA), indole-3-aceticacid (IAA), and indole-3-butyric acid (IBA)) and two exogenous Phys (1-naphthylacetic acid (1-NAA) and 2-naphthylacetic acid (2-NAA)) prior to HPLC-DAD analysis. The experimental parameters including sample volume, sorbent amount, adsorption time, adsorption pH, desorption time, and desorption solvent on extraction efficiency were optimized and evaluated. Under optimized conditions, the working range of 0.08 to 0.45 ng mL −1 with enrichment factors from 144 to 207 were achieved. The linear range is 0.75–200 ng mL −1 for IAA, 0.20–200 ng mL −1 for ABA, and 1.0–200 ng mL −1 for IBA, 1-NAA, and 2-NAA. With MSN@MIL-101(Fe) as sorbent for extraction of Phys and determination by HPLC-DAD, two endogenous Phys (IAA and ABA) were detected from mung bean sprouts which were made in a laboratory, and the results were further confirmed by high-resolution mass spectrometry. The composites can be applied to extract other small molecules, which have similar chemical structures with Phys in biological, environmental, and food samples.
Schematic presentation of a dispersive solid-phase extraction using monodispersed mesoporous SiO 2 @metal-organic framework composites (MSNs@MIL-101(Fe)) as the sorbent for extraction, clean-up, and preconcentration of phytohormones in mung bean sprouts prior to HPLC-DAD analysis.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
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IF 8.6
Basem E. Keshta,Haojie Yu,Li Wang,Ali H. Gemeay
MIL-101(Cr) MOF (MIL-Materials of Institute Lavoisier; Metal-organic framework) as an adsorbent has great application in water treatment because of its high stability against air, temperature, and chemicals. Herein, we develop a novel value-added, sustainable, and eco-friendly green method to prepare MIL-101(Cr) hydrothermally based on organic and inorganic waste recycling (G-MIL-101(Cr)@R) without hydrofluoric acid (HF) addition. Several characterization techniques suggest that G-MIL-101(Cr)@R was successfully synthesized. Then, it was used as an adsorbent for acid blue 92 dye (AB-92) as a model of anionic dyes. The adsorption parameters were studied, such as adsorbent dose, contact time, pH, dye concentration, temperature, salinity, and dye selectivity. The results showed that the adsorption of AB-92 is a monolayer according to the Langmuir isotherm with a q max of 2176 mg/g. Adsorption kinetics follow the pseudo second-order model (R 2 = 0.99), occurring in three steps according to the intra-particle diffusion kinetic model. The adsorption of AB-92 over G-MIL-101(Cr)@R is spontaneous and exothermic. The adsorption mechanism is mainly defined by electrostatic interactions. G-MIL-101(Cr)@R can adsorb the anionic dyes more efficiently than cationic dyes. It could also be reused for up to five cycles with an uptake efficiency of not less than 80 % without any change in its structure. Finally, G-MIL-101(Cr)@R is considered a superior adsorbent for anionic dyes. So, it will pave the way for developing MIL-101(Cr), based on organic and inorganic waste recycling, as an efficient adsorbent for removing organic dyes from wastewater.
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SENSORS AND ACTUATORS B-CHEMICAL
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2023
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IF 8.4
Wenyuan Li,Xiaoting Yu,Ying Tang,Zian Li,Syed Jalil Shah,Yuying Liu,Hanqing Zhao,Mingxin Song,Junjie Li,Guanchen Wang,Liqin Zhou,Zhongxing Zhao,Suya Liu,Zhenxia Zhao
Fabrication a reusable and highly sensitive fluorescence sensor in a controllable manner for water detection in solvents and humidity remains a top priority target yet a challenging task. In this work, carbon dots (CDs) are successfully implanted into confined metal–organic framework MIL-101(Cr) cages via “ship in the bottle” strategy and the confined CDs are firstly observed in MIL-101(Cr) cage showing high dispersion and high N content by advanced iDPC STEM technique. The highly selective water capture and sensitive changes of the fluorescence property with solution polarity and hydrogen-bonding donor acidity efficiently enhance the detection sensitivity and realize reusable turn-on detection based on the adsorption-solvent synergistic mechanism. Consequently, CDs@MIL-101 exhibits high sensitivity (detection limit: 0.036% and 0.028% v/v), wide response range (0.04–100% and 0.03–45%) and reusable stability for liquid water detection in acetone and tetrahydrofuran , respectively. Meanwhile, it can also detect gaseous water and the detection range is 23% to 85%. The analysis of real samples confirms the proposed method. Such construction strategy and detection mechanism will offer guidance for optimizing and expanding the detection performance of CDs, which is of great significance in the design and construction of novel multiphase sensors.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Shuang Liu,Mengjie Sheng,Bingqing Quan,Yabi Yang,Qinghong Ji,Xinpeng Hu,Xiang Lu,Jinping Qu
It is certainly one of the most feasible ways to extract fresh water from seawater in the face of the current depletion of fresh water resources. Although solar energy as a heat source for desalination is the cleanest and most abundant way, its intermittent and seasonal also poses an obstacle to its practical application. In order to solve the above-mentioned issues, we prepared a series of phase change composites (PCCs) with excellent light-absorbing and magnetic properties by growing MIL-101(Fe) in situ on cotton fabric. All-day desalination through the synergistic action of phase change material (PCM) and magnetic particles. The evaporation rate of PCC can reach 2.76 kg m −2 h −1 with an evaporation efficiency of 90.19 % under one sunlight condition. The evaporation rate of sea water under the synergistic effect of magnetic particles and PCM reached 4.53 kg m −2 h −1 in the absence of sunlight. This paper provides a new approach to all-day desalination without contact heating.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Basem E. Keshta,Haojie Yu,Li Wang,Md Alim Uddin,Heba G. El-Attar,Amr E. Keshta,Ali H. Gemeay,Fathy Hassan,Sherif M. Eid
Fabricating an ion-to-electron transducer (IET) from waste in the solid contact screen-printed ion-selective electrodes (SC-SP-ISEs) technique is challenging because its properties determine the potential stability and reproducibility of the designed sensors. Herein, we fabricated an IET substrate from recyclable wastes, and we applied it as an IET layer in an ISE-based sensor for fast and on-site detection of lead ions (Pb 2+ ) in an environmental sample. First, MIL-101(Cr) was prepared based on a combination of PET and Cr +6 waste recycling (R-MIL-101(Cr)). Polyaniline (PANI) was polymerized over R-MIL-101(Cr) to prepare a conductive PANI@R-MIL-101(Cr) composite. Then, it was applied as an IET substrate in the construction of pb 2+ -ISE for the detection of Pb 2+ ions in sediment samples collected from Lake Idku, Egypt. Three Pb 2+ sensors were fabricated and abbreviated as sensors I, II, and III corresponded to PANI, R-MIL-101(Cr), and PANI@R-MIL-101(Cr) as IET substrates, respectively. The performance of the sensors was studied to be applied for fast and selective detection of Pb 2+ at low concentration levels. Among the fabricated sensors, PANI@R-MIL-101(Cr) shows fast response (5 sec), low detection limit (1 × 10 −7 mol/L), and long lifetime reaches 70 days with a potential drift of 0.9 mV h −1 . The electrochemical characteristics prove the fast ion-to-electron transportation in the case of PANI@R-MIL-101(Cr) owing to its lower impedance and high capacitance. In-situ polymerization of PANI significantly enhanced the conductivity of the PANI@R-MIL-101(Cr) composite. The hydrophobic nature of PANI@R-MIL-101(Cr) ensures high stability by preventing the formation of water layers at the electrode/membrane interface. These results show the great potential of the IET-based PANI@R-MIL-101(Cr) layer for Pb2 + sensing in environmental samples with low detection limits and high stability for the future development of SC-ISEs.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2024
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IF 4.1
Jingjing Chen,Zhixiang Li,Xiaoqi Li,Yingxiang Du
A fluorescence sensor was developed based on NH 2 -MIL-101(Fe) and silicon-doped carbon quantum dots for the analysis of copper ions. Copper ions enhanced the fluorescence intensity of doped silicon-carbon quantum dots and decreased the intensity of NH 2 -MIL-101(Fe). The addition of copper ions resulted in fluorescence resonance energy transfer, which caused a reverse change in the fluorescence signal. The sensor based on the above mechanism can eliminate false positive interference. The fluorescence sensing system had a remarkable linear range of 0.25–5 µM for copper ions and a detection limit of 11 nM. It was then applied to water samples, resulting in recoveries ranging from 95.43 % to 103.1 %. The successful construction of this optical sensor not only broadened the way to detect copper ions but also provided a new idea for the detection of other targets mediated by copper ions. Finally, an attempt was made to construct a smartphone-assisted colourimetric platforms to detect copper ions in daylight.
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JOURNAL OF CHROMATOGRAPHIC SCIENCE
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2024
·
IF 1.5
Song Lixin,Zhang Jian,Wang Mingyu,Huang Zhipeng,Zhang Yunxia,Zhang Xing,Liang Yutao,He Juan
A novel approach for the simultaneous separation of zearalenone (ZEN) and four types of aflatoxins (AFB1, AFB2, AFG1 and AFG2) from rice samples was presented. This approach utilized modified MIL-101(Cr)-NH2 as core, with molecularly imprinted polymers (MIPs) serving as the shell. The MIL-101(Cr)-NH2 was prepared via ring-opening reaction, while the imprinted polymers were synthesized using warfarin and 4-methylumbelliferyl acetate as co-pseudo template, ethylene glycol dimethacrylate as the cross-linker and azobisisobutyronitrile as initiator. The resulting co-pseudo-template-MIPs (CPT-MIPs) were thoroughly characterized and evaluated. Adsorption studies demonstrate that the adsorption process of CPT-MIPs follows a chemical monolayer adsorption mechanism, with imprinted factors ranging from 1.24 to 1.52 and selective factors ranging from 1.29 to 1.52. Self-made columns were prepared, and the method for separation was developed and validated. The limit of detections ranged from 0.12 to 2.09 μg/kg, and the limit of qualifications ranged from 1.2 to 6.25 μg/kg. To assess the reliability of the method, ZEN and AFs were spiked at three different levels, and the recoveries ranged from 79.53 to 94.58%, with relative standard deviations of 2.90–5.78%.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Huidong Wang,Ziyu Gao,Jianmin Sun
Finding robust combination modes between ionic liquids and MOFs is still a challenge. In this work, using a simple one step-synthesis method, the ionic liquid was grafted onto MOF without any additives, and the binding mode of the two was characterized by means of XPS, FT-IR, TGA, SEM etc. It was found that the carboxyl group in the ionic liquid bonded with the amino group in MOF to form an amide bond. Thus, a novel stable composite material MIL-101-NH 2 -1-carboxypropyl-3-methylimidazolium bromine (1-C-3-M@MIL-101-NH 2 ) was synthesized. This composite employed as a catalyst for CO 2 cycloaddition demonstrated excellent catalytic activity, achieving a target product PC (Propylene carbonate) yield of 91.7 % under the conditions of 80 °C, 1.0 MPa, and a reaction time of 4 h, without the addition of any co-catalysts or solvents. The good catalytic activity was benefit from the synergistic effect of Lewis acidic Cr centers and nucleophilic Br - , as well as the high specific surface area and good CO 2 affinity of 1-C-3-M@MIL-101-NH 2 . In addition, owing to this robust bonding configuration, the catalyst can be recycled up to five times without losing activity. It is a potential catalyst for CO 2 capture and conversion.
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