JOURNAL OF MEMBRANE SCIENCE
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2021
·
IF 8.742
Chi Wang,Xiaoxuan Zhao,Jinghui Wu,Xia Yang,Xiaochun Cui,Wenzhe Geng,Zhi Geng,Xianze Wang
Efficient utilization of renewable solar energy is attractive in the membrane separation process of water treatment. In this study, a series of tight reactive hybrid ultrafiltration membranes were fabricated by covalently grafting Ag@NH 2 -MIL-125 nanoclusters on the side chains of a poly(aryl ether sulfone) matrix containing trifluoromethyl and carboxyl groups. Due to the homogeneous introduction of functional nanoreactors with high-efficiency solar photocatalytic degradation ability, the prepared tight hybrid membranes could approach good self-cleaning anti-fouling properties under sunlight irradiation. And the optimal sample exhibited an excellent water flux recovery ratio of 99.1% after irradiated by 10 min simulated sunlight. Additionally, the tight reactive hybrid membranes displayed excellent anti-aging robustness via the use of a fluorine-containing poly matrix, maintaining the stable high pollutant retention rate during the long-term ultrafiltration separation process. This work provided a new strategy to fabricate high-performance solar-driven reactive hybrid membranes for ultrafiltration separation processes.
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Catalysts
·
2019
·Vol. 9
·期 11
·906
·
IF 3.444
Jieyang Yang,Zequan Zeng,Zhanggen Huang,Yan Cui
In this work, the activation effect of vacuum thermal treatment on MIL-101(Fe) (MIL: Materials of Institute Lavoisier) was investigated for the first time. It demonstrated that vacuum thermal activation could accelerate the activation of persulfate (PS) by MIL-101(Fe), and the enhancement of the catalytic capacity of MIL-101(Fe) was mainly attributed to the change in the FeII/FeIII mixed-valence center. The results of the SEM and XRD showed that vacuum thermal activation had a negligible effect on the crystal structure and particle morphology of MIL-101(Fe). Meanwhile, the higher temperature of vacuum thermal activation caused a higher relative content ratio of FeII/FeIII. A widely used azo dye, X-3B, was chosen as the probe molecule to investigate the catalytic performance of all samples. The results showed that the activated samples could remove X-3B more effectively, and the sample activated at 150 °C without regeneration could effectively activate PS to remove X-3B for at least 5 runs and approximately 900 min. This work highlights the often-overlooked activation effect of vacuum thermal treatment and provides a simple way to improve the catalytic capacity and reusability of MIL-101(Fe) which is beneficial for the application of MIL-101(Fe)/PS systems in azo dye wastewater treatment.Keywords:vacuum thermal activation;MIL-101(Fe);persulfate;azo dye
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Journal of Materials Chemistry B
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2019
·Vol. 7
·期 44
·7006-7013
·
IF 5.047
Li Zhang,Xiaoni Ma,Hongbo Liang,Huihui Lin,Guangyu Zhao
Non-enzymatic glucose sensors are attracting significant attention owing to their low cost, storage convenience and reusability; however, their poor anti-interference caused by their weak selectivity towards glucose limits their practicability. In the present study, a MIL-53(NiFe) metal–organic framework (MOF) was prepared on Ni foam to serve as a self-supported electrode for non-enzymatic glucose detection. Due to the abundant active sites in the MIL-53(NiFe) MOF and its good stability in an alkaline solution, the sensors exhibited a high sensitivity (41.95 mA mM−1 cm−2) and a low detection limit (0.67 μM). Moreover, the molecular sieve effect of the MIL-53(NiFe) MOF led to a remarkable anti-interference ability, even at the interference concentrations of up to 20% glucose, a higher value than that in human serum. In addition, a heat treatment was carried out to remove the residual terephthalic acid in the MOF tunnels, and this promoted the detection linear range to 2–1600 μM. The reusability, reproducibility and long-term stability of the sensors were also studied, and the results implied good practicability of the MIL-53(NiFe) MOF-based sensors. Furthermore, the good practicability of the sensors was verified by testing human serum samples. The results showed the relative standard deviation of 2.73% from the hospital results, and the standard recovery was nearly 100%.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2019
·
IF 4.978
Zhenjiang He,Yuxi Yang,Peng Bai,Xianghai Guo
Selective adsorption and separation of three xylene isomers of seven stable metal-organic frameworks (MOFs) were investigated, where MIL-53(Cr) manifested the highest adsorption capacity and apparent preference for o -xylene. Further detailed studies with MIL-53(Cr) showed that pseudo-second-order model fit best with adsorption kinetics of xylene isomers, and the isotherms were perfectly fitted by Langmuir isotherm model. The adsorption was proved to be a quick process, and both the changes of entropy and enthalpy contributed to the o -xylene selectivity, but which mainly resulted from the entropy effect. The adsorption capacity of preferable isomer o -xylene, on account of better packing efficiency, was record-breaking 8.19 mmol/g, and selectivity of OX/PX, OX/MX and MX/PX were 13.75, 8.01 and 1.72, respectively. Both the adsorption capacity and OX selectivity on MIL-53(Cr) in liquid phase adsorption and breakthrough experiments were super high, which discriminated it from zeolites and other materials reported so far. Combined with extremely short equilibrium time and high stability, MIL-53(Cr) can be a promising adsorbent for separation of xylenes in industrial process.
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Journal of Materials Chemistry B
·
2019
·Vol. 7
·期 31
·4794-4800
·
IF 5.047
Kun Ye,Linjie Wang,Hongwei Song,Xin Li,Xiangheng Niu
Alkaline phosphatase (ALP) is extensively used as a clinical biomarker because of its close relevance with a variety of diseases. Thus, exploring reliable and practical methods for ALP analysis is of great significance. In the present work, we explored MIL-53(Fe) as a bifunctional platform with pyrophosphate (PPi)-mediated peroxidase-like activity and oxidation-stimulated fluorescence switching for ALP sensing. The proposed MIL-53(Fe) could exhibit favorable peroxidase-mimicking activity to catalytically decompose H2O2 to hydroxyl radicals, which had strong oxidizing ability to oxidize the terephthalic acid bridging ligand, resulting in the oxidation-stimulated turn-on fluorescence of MIL-53(Fe) itself. Due to the strong coordination interaction between PPi and Fe3+, the former with a relatively large molecular structure was able to inhibit the catalytic activity of MIL-53(Fe) via capping active Fe3+ sites, leading to the suppression of its self-fluorescence response. When ALP was present, it could hydrolyze the PPi inhibitor and restore the dual functions of MIL-53(Fe) to provide fluorescence again. With the above principle, highly sensitive and selective determination of ALP with a linear scope of 2–80 U L−1 and a detection limit down to 0.7 U L−1 was achieved. The MIL-53(Fe) was also demonstrated to be very reliable in measuring the target in human serum, indicating its great promise as an integrated tool for ALP detection in clinical practice.
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APPLIED CATALYSIS A-GENERAL
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2018
·
IF 4.521
Zhenzhen Lin,Mengting Luo,Yindi Zhang,Xiaoxue Wu,Yanghe Fu,Fumin Zhang,Weidong Zhu
Heterogeneous catalytic conversion of biomass-derived methyl levulinate (ML) to γ-valerolactone (GVL) is highly attractive as a sustainable route to mitigating the dependence on nonrenewable fossil resources. However, this route is limited by its low selectivity toward GVL and severe reaction conditions. Here, we present a synergistic catalytic process that offers exclusive GVL selectivity with complete ML conversion under mild conditions (80 °C, 0.5 MPa of H 2 pressure). This is achieved over a dual-functionalized catalyst of Ru nanoparticles (Ru-NPs) and Brønsted acid SO 3 H groups in a Cr-based metal-organic framework (MIL-101). The Ru-NPs served as metal sites for the hydrogenation of ML to methyl-3-hydroxyvalerate (MHV) and the acidic SO 3 H moieties promoted the cyclization of MHV to generate GVL via lactonization. In contrast, GVL production was significantly suppressed over the physically mixed congener (2.0 wt% Ru/MIL-101 + MIL-101-SO 3 H). This result demonstrates an unrivalled advantage of the dual integration of metal/acid sites in a single MOF crystal, and the relative amount of sulfonic acid groups in the catalyst can exert significant influence on the overall catalytic performances. The activation energies for the hydrogenation and lactonization steps with the developed catalyst were 29.5 and 42.1 kJ/mol, respectively, which are much lower than those observed with the traditional 5.0 wt% Ru/AC catalyst.
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ACS Applied Materials & Interfaces
·
2018
·
IF 8.097
Yanan Wei,Bingfeng Wang,Xinfang Cui,Yaseen Muhammad,Yanjuan Zhang,Zuqiang Huang,Xuesheng Li,Zhenxia Zhao,Zhongxing Zhao
MIL(Fe)/Fe-doped nanospongy porous biocarbon (Fe-SPC) composite was fabricated from MIL-100(Fe) via in situ growth on a unique Fe-doped nanospongy porous biocarbon (Fe-SPC) and was used as Fenton-like catalyst for advanced degradation of thiamethoxam (THIA). Fe was loaded on silkworm excrement and calcined to Fe-SPC with nanospongy and high sp2 C structure. The in situ growth strategy embedded the Fe-SPC into MIL-100(Fe) crystals and formed conductive heterojunctions with an intensified interface by Fe-bridging effect, which was confirmed by negative shift of Fe3+ binding energy in X-ray photoelectron spectroscopy. MIL(Fe)/Fe-SPC composites exhibited high degree of crystallinity and surface area (Brunauer–Emmett–Teller: 1730 m2/g). Liquid chromatography–mass spectrometry and density functional theory simulations demonstrated that THIA was converted to a relatively stable compound (C4H5N2SCl), which could be captured by MIL-100(Fe) with strong chemical bonding energy (Fe–N, −587 kJ/mol), followed by a significant geometric distortion, resulting in a thorough degradation. Efficient charge separation and synergistic chemisorption-catalysis strategy resulted in the high catalytic activity of MIL(Fe)/Fe-SPC. The composite catalyst concurrently exhibited high mineralization ratio with 95.4% total organic carbon removal (at 25 °C and 180 min) and good recycling ability under wider neutral/alkaline conditions. Endorsing to these intriguing properties, MIL(Fe)/Fe-SPC can be deemed an efficient contender for removal of hard-degradable pesticides and other environmental pollutants in practical applications.
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CATALYSIS COMMUNICATIONS
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2015
·
IF 3.699
Yong Liu,Shao-Yi Jia,Song-Hai Wu,Ping-Li Li,Chun-Jiang Liu,Yi-Ming Xu,Feng-Xiang Qin
Highly dispersed metallic nanoparticles immobilizing inside the pores of MIL-101(Cr) were prepared using double solvent method (DSM). The particle size of Au, Ag, Pd, and AuPd NPs were 2.9 ± 0.7 nm, 1.9 ± 0.6 nm, 2.1 ± 0.6 nm and 2.8 ± 0.7 nm, respectively. The catalytic activity determined by the reduction of p-nitrophenol by NaBH 4 to p-aminophenol of Pd and AuPd prepared by DSM is 9.6 and 8.3 times higher than that of Pd and AuPd prepared by conventional impregnation method. The structure and activity of the catalysts prepared by DSM have no significant changes after three cycles.
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RSC Advances
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2016
·Vol. 6
·期 43
·37110-37117
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IF 3.289
Mingjuan Han,Zheng Gu,Chong Chen,Zuowang Wu,Yigen Que,Qiang Wang,Hui Wan,Guofeng Guan
A new, simple and effective strategy to confine dicationic acid ionic liquids (DAILs, 1,4-bis[3-(propyl-3-sulfonate) imidazolium] butane hydrogen sulfate) in the cages of MIL-100(Fe) frameworks was constructed. The target catalyst, defined as MIL-100(Fe)@DAILs, was characterized by XRD, FTIR, SEM, TEM, EA, TGA and N2 adsorption–desorption. Meanwhile, the catalytic activity of the MIL-100(Fe)@DAILs catalyst was evaluated by the esterification reaction with oleic acid and methanol. The results indicated that the DAILs had been effectively encapsulated within the cages of the MIL-100(Fe) frameworks. Moreover, the influence of reaction time, reaction temperature, molar ratio of methanol to oleic acid and catalyst dosage on the conversion of oleic acid was studied by univariate analysis. The conversion of oleic acid decreased from 93.5% to 86.0% when the catalyst was reused five times, which indicated that the target catalyst possessed higher catalytic activity and superior catalytic activity. Finally, an esterification mechanism catalyzed by this novel catalyst was illustrated.
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MOLECULES
·
2017
·Vol. 22
·期 6
·920
·
IF 2.861
Youxun Liu,Yuanyuan Geng,Mingyang Yan,Juan Huang
The successful encapsulation of 2,2′-azino-bis(3-ethylbenzthiazoline-6-sulfonic acid) (ABTS), a well-known laccase mediator, within a mesoporous metal-organic framework sample (i.e., MIL-100(Fe)) was achieved using a one-pot hydrothermal synthetic method. The as-prepared ABTS@MIL-100(Fe) was characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), Fourier transform infrared (FT-IR) spectroscopy, nitrogen sorption, and cyclic voltammetry (CV). Our ABTS@MIL-100(Fe)-based electrode exhibited an excellent electrochemical response, indicating that MIL-100(Fe) provides an appropriate microenvironment for the immobilization and electroactivity of ABTS molecules. ABTS@MIL-100(Fe) was then evaluated as an immobilized laccase mediator for dye removal using indigo carmine (IC) as a model dye. Through the application of laccase in combination with a free (ABTS) or immobilized (ABTS@MIL-100(Fe)) mediator, decolorization yields of 95% and 94%, respectively, were obtained for IC after 50 min. In addition, following seven reuse cycles of ABTS@MIL-100(Fe) for dye treatment, a decolorization yield of 74% was obtained. Dye decolorization occurred through the breakdown of the chromophoric group by the Laccase/ABTS@MIL-100(Fe) system, and a catalytic mechanism was proposed. We therefore expect that the stability, reusability, and validity of ABTS@MIL-100(Fe) as a laccase mediator potentially render it a promising tool for dye removal, in addition to reducing the high running costs and potential toxicity associated with synthetic mediators.Keywords:laccase;ABTS;metal-organic framework;mediator;decolorization
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CARBOHYDRATE POLYMERS
·
2025
·
IF 12.5
Xin Wang,Pan Jiang,Xinjian Dai,Hao Guan,Xiaoqing Wang
Developing high-performance metal-organic framework (MOF)-based composites with high loading and uniform distribution of MOF nanoparticles is crucial for their adsorption-associated applications but remains challenging due to the lack of ideal carriers. Herein, a novel MOF-based composite was developed by in situ growth of MIL-53(Al) crystals within the carboxylated wood sponge (CWS) derived from natural balsa wood. The conversion of the cellular structure of natural wood into a lamellar structure greatly enhances the accessibility of the wood scaffold, while the introduction of carboxyl groups onto the cellulose skeleton of the wood sponge encourages the selective growth of MIL-53(Al) crystals on the lamellae of CWS. The structural features of the obtained MIL-53(Al)@CWS were investigated with FT-IR, XRD, SEM, and N 2 adsorption/desorption isotherms. The MIL-53(Al) loading can be finely tuned by adjusting the concentration of the MOF precursor solutions, and an appropriate MIL-53(Al) loading of 23 wt% results in the uniform dispersion of MIL-53(Al) crystals within the wood sponge without agglomeration. Benefiting from the high loading of MIL-53(Al) and the unique lamellar channels of CWS, the developed MIL-53(Al)@CWS can effectively adsorb various organic dyes such as rhodamine B (RhB), methylene blue, Congo red, and methyl orange in water, with a high adsorption capacity of 135.82 mg g −1 for RhB. Density functional theory (DFT) calculations reveal the detailed dynamic diffusion pathways and the molecular interactions between RhB and MIL-53(Al). This work demonstrates the advantages and potentials of lamellar wood sponges as a promising host matrix in supporting MOF powders for adsorption-associated applications.
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TALANTA
·
2017
·
IF 4.162
Li Liang,Xinghua Wang,Ying Sun,Pinyi Ma,Xinpei Li,Huilan Piao,Yanxiao Jiang,Daqian Song
The metal-organic framework (MOF) functionalized magnetic graphene oxide/mesoporous silica composites (Fe 3 O 4 @SiO 2 -GO/MIL-101(Cr)) were synthesized and utilized as magnetic solid-phase extraction (MSPE) adsorbent for the extraction of seven triazine herbicides (terbuthylazine, secbumeton , terbumeton , atraton , atrazine , prometon and trietazine) in rice samples. Several experimental parameters, including type and volume of extraction solvent, amount of MIL-101(Cr), extraction time, volume of desorption solvent and desorption time were investigated and optimized. The limits of detection (LODs) of seven triazine herbicides obtained by using the proposed MSPE method combined with high performance liquid chromatography (HPLC) were in the range of 0.010–0.080 µg kg −1 . The recoveries of the triazine herbicides in spiked rice samples ranged from of 83.9–103.5% with the relative standard deviations lower than 8.7%. The intra and inter-day (n = 6) precisions for all triazine herbicides at the spiked level of 100.0 µg kg −1 were 1.4–5.9% and 2.6–7.8%, respectively.
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