Journal of Inorganic and Organometallic Polymers and Materials
·
2021
·Vol. 31
·期 11
·4195-4208
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IF 3.543
Wang Lulu,Zeng Xiangrui,Wang Haiyan,Wang Yujia
Abstract A series of porous confined ionic liquid phosphotungstate were synthesized by encapsulated of N-(3-sulfopropyl)morpholinium phosphotungstate ([C 3 SO 3 Hnhm] 3 -PW 12 O 40 ) into MIL-101. Then the aforementioned porous confined ionic liquid phosphotungstate as heterogeneous catalyst will be used together with H 2 O 2 for the catalytic synthesis of adipic acid from cyclohexene. During the experiment, the effect of weight content of [C 3 SO 3 Hnhm] 3 PW 12 O 40 on the catalytic performance was investigated in detail. And the chemical structure of the catalyst was also characterized by XRD, FT-IR, 1 H-NMR, SEM–EDX and N 2 adsorption–desorption isotherms. Experimental results revealed that the desired products has been successfully prepared, and the best catalytic performance (81.2% yield of the adipic acid) was obtained under the dose of [C 3 SO 3 Hnhm] 3 PW 12 O 40 was 31wt%, which was almost close to the catalytic activity of original [C 3 SO 3 Hnhm] 3 PW 12 O 40 (85.3% yield of the adipic acid), which was also proved the strategy of packaging ionic liquid phosphotungstate with MIL-101 in this research is feasible. Furthermore, recycled catalytic performance of the catalyst under repeat 6 times was evaluated and the result revealed that the yield in adipic acid was still higher than 80.0%, which also proved that the catalytic active component was stable in the catalyst. Graphic Abstract
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Hui He,Yuexin Wang,Juan Li,Shanliang Jiang,Subhan Sidra,Wenxue Gong,Ying Tang,Yang Hu,Rule Wei,Dongxiao Yang,Xuesheng Li,Zhongxing Zhao
High light adsorption and fast charge separation are crucial for photo-Fenton catalytic activity of MOFs. Herein, bottom-up design was proposed to fabricate polypyrrole (PPy C ) nanowires in MIL-88B(Fe) cages as photo-Fenton catalyst for Sulfamethoxazole (SMX) efficient degradation. Pyrrole was prior anchored into MIL-88B(Fe) cluster via Fe-N coordination, and then the additional monomer pyrrole was further triggered bottom-up polymerization in confined cages of MIL-88B(Fe) and formed PPy C @Py-MIL(Fe) composite. These PPy C nanowires were dispersed in Py-MIL(Fe) cages and tightly connected with MOFs clusters via Fe-N bonding. Characterization proved that: (1) Interfacial Fe-N can significantly promote the efficient electron transport from PPy C nanowires to Py-MIL(Fe), enhance optical absorption property, and construct strong Lewis acidic sites and ligand vacancies in PPy C @Py-MIL(Fe). (2) The confined PPy C nanowire via Fe-N connection remarkably promote photo-generated electron-hole separation, Fe 2+ |Fe 3+ redox ability of MOF, and improved photo-electric corrosion ability. As a result, it significantly enhanced the photo-Fenton catalytic performance for SMX degradation. Catalytic oxidation was attributed to the generation of ‧OH species that oxidized 93% SMX in 60 min, showing ultra-rapid degradation and TOC removal rates of 33.7 min −1 ·mg·g −1 and 8.68 min −1 ·mg·g −1 respectively, which was about 4–220 times higher than those reported state-of-the-art catalysts. Additionally, the PPy C @Py-MIL(Fe) catalyst showed minimal loss in catalytic activity even after recycling for 10 times, exhibiting good recycling stability compared to many MOFs. Systematic analysis shown that in-situ anchored growth of polypyrrole in confined porous cages of MOF can effectively enhance the catalytic activity and stability of MIL-88B(Fe), and has great development potential applications for photo-Fenton catalytic degradation of organic pollutants.
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CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Wen Cao,Yuhang Yuan,Cao Yang,Shichuan Wu,Jianhua Cheng
For the first time, visible-light-driven g-C 3 N 4 /MIL-68(In)-NH 2 heterojunction composites with high photocatalytic activity were prepared for the degradation of ibuprofen (IBP) using an in-situ solvothermal synthesis method assisted with ultrasonication. The composites achieved intensive visible-light absorption, enhanced separation efficiency of photogenerated carriers, and high adsorption capacity, thus achieving excellent photocatalytic degradation for IBP. Among all the composites, 10 wt% g-C 3 N 4 /MIL-68(In)-NH 2 exhibited the maximum photocatalytic rate (0.01739 min −1 ), 19.28 and 2.00 times higher than those of g-C 3 N 4 and MIL-68(In)-NH 2 , respectively. Moreover, the pH, ibuprofen concentration, and catalyst dosages played important roles both in photodegradation and adsorption. In addition, the photocatalytic mechanism was also elucidated, demonstrating that h + was the main reactive species, followed by OH and O 2 − radicals, responsible for the degradation of IBP. Finally, seven aromatic intermediates of IBP were identified, and five possible degradation pathways were proposed, mainly involving hydroxylation, aldehyde oxidation, decarboxylation, and dehydrogenization reactions.
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Catalysis Science & Technology
·
2018
·Vol. 8
·期 7
·1936-1944
·
IF 5.365
Zhongmin Liu,Yongchuan Wu,Jitao Chen,Yaru Li,Jingyu Zhao,Kaihua Gao,Ping Na
A bifunctional cake-like TiO2 was successfully synthesized via calcination of MIL-125(Ti) at a suitable temperature by a one-step method and was applied for As(III) removal by simultaneous photocatalytic oxidation and adsorption. The as-synthesized samples were characterized by XRD, TGA/DSC, SEM, TEM, N2 adsorption–desorption isotherms, PL spectra, photocurrent, FTIR and XPS. The effects of calcination temperature on the specific surface areas of the samples, transformation of the TiO2 crystal phase and properties of As(III) removal were investigated. The results showed that higher calcination temperature resulting in a lower specific surface area and more transformations of the TiO2 crystal phase from anatase to rutile. The TiO2 calcined at 380 °C (MIL-125(Ti)-380 °C) exhibited excellent properties for As(III) removal, including photocatalytic oxidation of As(III) and simultaneous adsorption of the generated As(V). In addition, MIL-125(Ti)-380 °C could be reused at least four times without significant reduction in the photocatalytic oxidation and adsorption performances. The excellent photocatalytic oxidation and adsorption abilities of MIL-125(Ti)-380 °C can be attributed to the synergistic effects of strong photogenerated electron–hole separation and high specific surface area. The bifunctional cake-like TiO2 provides a wonderful strategy to remove As(III) completely from contaminated water using a single step.
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DALTON TRANSACTIONS
·
2015
·Vol. 44
·期 13
·6212-6218
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IF 4.197
Lan Wen,Xiaoqiong Du,Jun Su,Wei Luo,Ping Cai,Gongzhen Cheng
Well-dispersed bimetallic Ni–Pt nanoparticles (NPs) with different compositions have been successfully grown on the MIL-96 by a simple liquid impregnation method using NaBH4 as the reducing agent. Powder X-ray diffraction, transmission electron microscopy, energy-dispersive X-ray spectroscopy, N2 adsorption–desorption, and inductively coupled plasma-atomic emission spectroscopy measurements were employed to characterize the NiPt/MIL-96. Catalytic activity of NiPt/MIL-96 catalysts was tested in the hydrogen generation from the aqueous alkaline solution of hydrazine at room temperature. These catalysts are composition dependent on their catalytic activity, while Ni64Pt36/MIL-96 exhibits the highest catalytic activity among all the catalysts tested, with a turnover frequency value of 114.3 h−1 and 100% hydrogen selectivity. This excellent catalytic performance might be due to the synergistic effect of the MIL-96 support and NiPt NPs, while NiPt NPs supported on other conventional supports, such as SiO2, carbon black, γ-Al2O3, poly(N-vinyl-2-pyrrolidone) (PVP), and the physical mixture of NiPt and MIL-96, all of them exhibit inferior catalytic activity compared to that of NiPt/MIL-96.
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JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL
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2015
·
IF 3.615
Huiyan Pan,Xiaohong Li,Yin Yu,Junrui Li,Jun Hu,Yejun Guan,Peng Wu
Metal organic-framework MIL-101 and inorganic mesoporous composites Al 2 O 3 @SBA-15 supported Pt catalysts, Pt/MIL-101 and Pt/Al 2 O 3 @SBA-15 catalysts, were prepared and characterized by means of X-ray diffraction (XRD), N 2 adsorption–desorption, scanning electron microscopy (SEM), transmission electron microscopy (TEM), CO chemisorption and thermo-gravimetric (TG) analysis. Pt nanoparticles were highly dispersed on both supports. In liquid-phase hydrogenation of nitrobenzene, benzaldehyde and their derivatives, the Pt/MIL-101 catalyst was superior to the Pt/Al 2 O 3 @SBA-15 catalyst in water. For liquid-phase hydrogenation of nitrobenzene with the Pt/MIL-101 catalyst, owing to high solubility of nitrobenzene in ethanol, the reaction in ethanol went much faster than that in water, furnishing a turnover frequency (TOF) in ethanol up to 18,053 h −1 , almost triple of that obtained in water under similar conditions. The highest TOF of 25,438 h −1 was obtained in ethanol for hydrogenation of 3-chloro-nitrobenzene with the Pt/MIL-101 catalyst. As for hydrogenation of benzaldehyde series, 2-fluoro-benzaldehyde and 3-fluoro-benzaldehyde gave the highest TOFs of 5146 h −1 and 3165 h −1 in water with the Pt/MIL-101 and Pt/Al 2 O 3 @SBA-15 catalysts, respectively. We deduce that surface property of MIL-101 with high hydrophobicity is helpful to enrich reactants around the Pt/MIL-101 catalyst in water, where nitrobenzene or benzaldehyde and its derivatives have a limited solubility, so that high catalytic performance was achieved with the Pt/MIL-101 catalyst in water. Of particular note is that the Pt/MIL-101 catalyst can be reused at least four times without loss in activity or selectivity.
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APPLIED CATALYSIS A-GENERAL
·
2013
·
IF 3.41
Zhiguo Sun,Gang Li,Hai-ou Liu,Liping Liu
A series of MOF-based catalysts, metal-salen complexes incorporated into amino-functionalized MIL-101 matrices by salicylaldehyde condensing to amino group and coordinating metal ion through one pot method, have been prepared and characterized. The successful preparation of catalysts demonstrates that postsynthetic modification (PSM) is a practical and powerful route to generate MOF-based catalyst with multiple active sites. The catalytic performances of prepared catalysts were investigated via selective oxidation of cyclohexane to cyclohexanone and cyclohexanol (KA-oil) by molecular oxygen in the absence of solvent. It was found that NH 2 -MIL-101(Cr)-Sal-Co, as a typical case, behaves as cooperative catalyst for cyclohexane selective oxidation. That is, salen-Co(II) attached to framework of MOF is able to assist in the generation of new radicals from peroxides via a Haber–Weiss catalytic cycle to promote conversion of cyclohexane while framework Cr ion is able to catalyze the dehydration of intermediate product cyclohexyl hydroperoxide (CHHP) to improve KA-oil selectivity. Furthermore, this catalyst exhibits good recyclability and behaves as truely heterogeneous catalyst.
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JOURNAL OF SEPARATION SCIENCE
·
2016
·Vol. 39
·期 12
·2356-2364
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IF 2.741
Fuyou Du,Qun Qin,Jianchao Deng,Guihua Ruan,Xianqing Yang,Laihao Li,Jianping Li
In this work, a magnetic metal–organic framework designated as MIL-100(Fe) was prepared and applied as a magnetic solid-phase extraction sorbent for the determination of trace polycyclic aromatic hydrocarbons in environmental water samples by coupling with high-performance liquid chromatography and fluorescence detection. The magnetic microspheres exhibited large surface areas and high extraction ability, making them excellent candidates as sorbents for enrichment of trace polycyclic aromatic hydrocarbons. Under the optimized experimental conditions, good sensitivity levels were achieved with low detection limits ranging from 32 to 2110 pg/mL and good linearities with correlation coefficients higher than 0.9990 for the investigated 13 polycyclic aromatic hydrocarbons. The proposed method has been validated in the analysis of real water samples with mean recoveries in the range of 81.4–126.9% at four spiked levels and the relative standard deviations in the range of 1.3–17.0%. The magnetic MIL-100(Fe) microspheres were stable enough for 150 extractions without a significant loss of extraction performance.
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MICROCHIMICA ACTA
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2016
·Vol. 183
·期 8
·2467-2472
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IF 4.831
Yang Yang,Ma Xiaowei,Feng Fan,Dang Xueping,Huang Jianlin,Chen Huaixia
The article describes the synthesis of core-shell magnetic nanoparticles (MNPs) of the type Fe 3 O 4 @MIL-100 (MIL standing for Material Institut Lavoisier), and their application as sorbent for magnetic solid-phase extraction (MSPE) of triclosan. The MNPs were prepared via circular self-assembly of ferric chloride and benzenetricarboxylic acid. The functionalized MNPs were characterized by transmission electron microscopy, FTIR and thermogravimetry. Following extraction, triclosan was eluted with ammoniacal methanol and then submitted to HPLC with UV detection. The amount of magnetic microspheres, sample pH and ionic strength, adsorption time, desorption time, desorption solvent and the volume of the eluent were optimized. Under optimum conditions, the method showed good linearity in the 0.1 to 50 mg·kg −1 triclosan concentration range in toothpaste samples. Other features include (a) intra-day and inter-day relative standard deviations (RSD, for n = 4) of <5.5 %, (b) a 30 μg·kg −1 limit of detection, and (c) extraction recoveries between 90.86 % and 101.1 %. The method was successfully applied to the determination of triclosan in children’s toothpaste.
The article describes the synthesis of core-shell magnetic nanoparticles (MNPs) of the type Fe 3 O 4 @MIL-100, and their application as sorbent for magnetic solid-phase extraction (MSPE) of triclosan.
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RSC Advances
·
2016
·Vol. 6
·期 113
·112502-112511
·
IF 3.289
Jiumei Wang,Jinquan Wan,Yongwen Ma,Yan Wang,Mengjie Pu,Zeyu Guan
MIL-88A was synthesized in diverse preparation conditions and characterized by various techniques. The catalytic performance of MIL-88A series for degrading Orange gelb (OG) through persulfate activation were also tested at temperature of 25 °C and the results were shown in the following sequence: 85 °C/2 h > 65 °C/2 h > 105 °C/2 h > 65 °C/6 h > 65 °C/12 h. MIL-88A produced at the synthesis temperature of 85 °C and in the crystallization time of 2 h (85 °C/2 h) was the best one with a removal rate of 96.4% mainly due to high SBET and much greater leach-out of Fe. An optimal dosage (0.3 g L−1) for MIL-88A in the MIL-88A/PS/OG system exists because of inhibition and promotion by fumaric acid. The filtrate experiment indicated that the catalytic activation involved heterogeneous reactions on the surface of the catalyst and homogeneous reactions in solutions. But the heterogeneous reaction occupied the principal position and the probable mechanism was obtained. Moreover, only solution pH < 4 could show a high degradation effect without the help of temperature. Comparing two different methods in the recycling experiment, the removal rate of OG decreased after the fourth run in both. Loss of active catalytic sites for Fe(III) in MIL-88A in the process of separating and sampling was responsible for activity decay.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Syed Jalil Shah,Xinqi Luan,Xin Yu,Weige Su,Yucheng Wang,Zhongxing Zhao,Zhenxia Zhao
The development of metal organic framework (MOF)-based π-π conjugated structures capable of effectively transforming H 2 O from humid air to • OH radicals for VOCs photodegradation is a significant but difficult task. Herein, an amino-ionic liquid (NH 2 -IL) based dual-mode bridging strategy was proposed to connect 3D-graphene with NH 2 -MIL-125 forming IL-3DGr/NM(Ti) nanohybrids for advanced acetaldehyde photodegradation. The rational integration of these components was responsible for: (1) maintaining π-π conjugated electron transport system; (2) generating abundant coordinatively unsaturated sites and oxygen vacancies; (3) increasing surface area of the nanohybrids. With these attributes, IL-3DGr/NM(Ti) demonstrated enhanced charge separation and transportation electrochemical impedance spectroscopy (EIS): 7-times), acetaldehyde adsorption (22 %), light absorption (bandgap: 1.51 eV). The rapid H 2 O adsorption and photoconversion to • OH radicals by IL-3DGr/NM(Ti) enabled it to demonstrate superior CH 3 CHO photodegradation rate under high humidity, surpassing many state-of-the-art photocatalysts by 9 to 187 times under static air conditions and with nearly similar catalyst dosages* (photocatalyst weight and initial acetaldehyde concentration (mg ppm −1 ) ratio). Interestingly, the IL-3DGr/NM(Ti) photocatalytic activity was enhanced by increasing RH% up-to 80 %. Besides, the nanohybrids demonstrated tremendous stability, with only a 3.9 % decline observed after 5 consecutive-cycles. This strategy provides new prospects to improve the compatibility of graphene/MOF materials for futuristic photoelectrical applications under high humidity.
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Materials Science and Engineering B-Advanced Functional Solid-State Materials
·
2024
·
IF 3.9
Kashif Nawaz Khattak,Maosen Zhang,Caixia Deng,Shuang Li,Ling Jiang,Pran Gopal Karmaker,Xiupei Yang
In this work, the hybrid material NH 2 -MIL-125(Ti)@TpPa-NO 2 was synthesized by grafting an amino-functionalized titanium-based metal–organic framework (NH 2 -MIL-125(Ti)) with 2,4,6-tri(4-pyridyl)-1,3,5-triazine-nitro (TpPa-NO 2 ) moieties. The resulting composite material exhibited remarkable removal efficiency owing to the synergistic effects derived from the combination of the NH 2 -MIL-125(Ti) and TpPa-NO 2 components. The material demonstrated excellent stability and recyclability, making it a promising candidate for the treatment of wastewater containing rhodamine-B (Rhd-B). Some characterization techniques were employed to elucidate the structural features and surface morphology of the hybrid material. The adsorption capacity of NH 2 -MIL-125(Ti)@TpPa-NO 2 for Rhd-B dye was evaluated, and the results revealed an exceptional removal efficiency of 99.96 % and a high adsorption capacity of 25.54 mg/g, highlighting the superior adsorption performance of the material. The adsorption process was found to follow Langmuir isotherm and pseudo-second-order kinetics, indicating that chemisorption is the predominant mechanism governing the uptake of Rhd-B dye onto NH 2 -MIL-125(Ti)@TpPa-NO 2 .
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