INTERNATIONAL JOURNAL OF ENERGY RESEARCH
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2020
·Vol. 44
·期 6
·4426-4437
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IF 3.741
Fangyan Cui,Wenyi Wang,Caini Liu,Xingyu Chen,Ning Li
Summary One-dimensional (1D) sodium ligninsulfonate functionalized carbon nanotubes (SCNT), two-dimensional (2D) graphene oxide (GO), and three-dimensional (3D) zirconium-based metal-organic frameworks (UiO-66) are self-assembled as filler materials for proton-exchange membranes (PEMs) because of their potential for extending proton transport pathways. Herein, UiO-66-SCNT and UiO-66-SCNT@GO were prepared by a facile solvothermal synthesis and then the nanohybrid chitosan (CS) PEMs were fabricated via solution casting. The hybrid PEMs with higher ion exchange capacity than the pure CS membrane displayed higher proton conductivity and selectivity. The proton conductivity of nanohybrid membrane doped with 7 wt% UiO-66-SCNT@GO (CS/U-S@GO-7) was enhanced to 64 mS cm −1 at 70°C. Simultaneously, the selectivity was reached 19.4 × 10 4 S s cm −3 and was much higher than the pristine CS membrane (0.13 × 10 3 S s cm −3 ). Moreover, the mechanical properties of all composite membranes were significantly enhanced compared with that of the pure CS membrane. The results showed that our research provided a valuable strategy for designing high-performance CS-based PEMs in direct methanol fuel cell (DMFC). Highlights A simple and facile solvothermal synthesis was used to prepare UiO-66-SCNT@GO. UiO-66-SCNT@GO was introduced into chitosan (CS) matrix to optimize proton transport channels. CS-based hybrid membranes exhibit high proton conductivity and selectivity. CS-based hybrid membranes show low methanol permeability.
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Journal of the Taiwan Institute of Chemical Engineers
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2021
·
IF 5.876
Liu Yang,Yu-Long Liu,Xian-Xian Ji,Cheng-Guo Liu,Ying Fu,Fei Ye
Background A novel luminescent sensor with dual-emitting platforms, Tb@UiO-66 , was used for highly detecting Sm 3+ and teflubenzuron. Methods Tb@UiO-66 was synthesized on basis of the exchange of guest molecules, where Tb 3+ ions were encapsulated into the cages of UiO-66 . Significant finds The results of multiband fluorescence originated from the linker-to-cluster charge transfer and the characteristic emission of Tb III . Tb@UiO-66 displayed luminescence enhancements or quenches according to small molecules. Especially for Sm 3+ and teflubenzuron, the characteristic peaks of Tb@UiO-66 at 490, 545, 585, and 621 nm increased with the increasing of the concentration of the analytes, where Tb@UiO-66 exhibited the effect of luminescence enhancement. The detection limits for detecting Sm 3+ and teflubenzuron were 0.09 μM and 0.21 μM, and the changes of luminescence intensities could be observed by naked eyes under the UV light at 365 nm. Tb@UiO-66 could also be used to detect teflubenzuron in real water samples. Tb@UiO-66 could be reused for at least 5 cycles for the detection of Sm 3+ and teflubenzuron with the framework of Tb@UiO-66 uncollapsed. These results implied that the integration of Ln III luminescent materials and Zr-MOFs by doping method provided a new strategy for fabricating novel luminescent sensors for detecting polluting small molecules.
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ACS Omega
·
2019
·
IF 2.584
Junjie Zhu,Linbo Wu,Zhiyang Bu,Suyun Jie,Bo-Geng Li
UiO-66-NH2, a zirconium-based functional metal–organic framework (MOF), was postsynthetically modified via Schiff base reaction between aldehyde groups in glutaraldehyde and amino groups in UiO-66-NH2 and CO2-preabsorbed polyethyleneimine (PEI). The resulting PEI-modified MOFs, abbreviated as PEIC@UiO, were characterized with 1H NMR, Fourier transform infrared, powder X-ray diffraction, Brunauer–Emmett–Teller, scanning electron microscopy, and thermogravimetric analysis and evaluated as CO2 adsorbents. In comparison with pristine UiO-66-NH2, the PEIC@UiO adsorbents have reduced specific surface area (7–150 m2/g) but maintained the same crystal structure. Particularly, the PEIC96@UiO adsorbent exhibited significantly improved CO2/N2 adsorption selectivity (48 vs 25) and higher CO2 adsorption capacity (3.2 vs 2.7 mmol/g). The adsorbent also displayed moderate desorption energy (68 kJ/mol CO2), superior moisture endurance, and recyclability, which are very desirable for practical applications.
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JOURNAL OF MEMBRANE SCIENCE
·
2019
·
IF 7.015
Lifen Liu,Xin Xie,Saren Qi,Ruihan Li,Xiao Zhang,Xiaoxiao Song,Congjie Gao
The removal of boron from seawater remains a challenge and now receives increasing attention worldwide. Boron removal rates offered by conventional reverse osmosis membranes through one-pass desalination processes are not sufficient to achieve WHO standard. In this paper, the UiO-66 nanoparticles , a metal-organic framework (MOF), are proposed to incorporate into the polyamide (PA)-based thin film nanocomposite (TFN) reverse osmosis (RO) membrane for boron removal due to their inherent porous structure, narrow pore size, and strong adsorption to boron. At an optimum blending concentration of 0.05% (w/v), The UiO-66 TFN membrane showed a ∼50% increase in water flux and a marginal increase in rejection compared with the benchmark thin film composite (TFC) membrane in the brackish water desalination test. In a simulated seawater desalination test, the UiO-66 blended TFN membrane promotes the boron rejection by ∼11% compared with the benchmark membrane. The simultaneous increase of water flux and boron rejection at low blending concentrations are likely attributed to the highly porous structure which provides additional pathways for water transport and the strong adsorption to boron which indued a further pore narrowing effect to its intrinsic pore size of ∼6.1 Å. Therefore, this work provides a new and facile approach to enhance the boron removal rate of the polyamide-based RO membrane via the incorporation of UiO-66 nanoparticles.
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RSC Advances
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2019
·Vol. 9
·期 43
·24802-24810
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IF 3.049
Xu Zhang,Yufan Zhang,Tiecheng Wang,Zheng Fan,Guoliang Zhang
A facile controlled interfacial polymerization strategy was proposed for the synthesis of novel thin film nanocomposite (TFN) membranes for enhanced nanofiltration performance. UiO-66 nanoparticles were aminated and pre-immobilized onto a polymer substrate via polydopamine (PDA) coating to achieve a continuous and defect-free polyamide dense layer. The mediation of the PDA coating could not only enhance the structural stability of TFN nanofiltration membranes, but also improve the dispersion and anchorage of UiO-66-NH2, thus closely fixing the position of UiO-66-NH2 nanoparticles on the polymer substrate. Moreover, since the amino group (–NH2) further reacted with PDA via Michael addition or Schiff base reaction, the in situ mutual reaction reduced the nanoparticle losses significantly during the draining off of the monomer solution in the fabrication process, which effectively cut down the actual dosage. The results showed that the PDA interlayer could induce the tight attachment of the PA layer to the support, enhancing the structural stability of TFN membranes. Furthermore, the dosage of UiO-66-NH2 in the as-prepared TFN membranes could also be decreased to as low as 0.01 w/v%, which was nearly a 10–20-fold reduction in the required amount of UiO-66-NH2 for the synthesis. The fabricated TFN/UiO-66-NH2 membranes exhibited very high water permeance and competitive salt rejections in cross-flow nanofiltration, which shows the huge potential for the application of novel TFN membranes with controlled nanoparticle incorporation in industrial separation.
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JOURNAL OF MEMBRANE SCIENCE
·
2019
·
IF 7.015
Hui Wang,Sihan Tang,Yunxia Ni,Chongrui Zhang,Xiangwei Zhu,Qiang Zhao
Interface compatibility between hydrophilic metal-organic frameworks (MOFs) and hydrophobic polydimethylsiloxane (PDMS) is less effectively reconciled through supramolecular modifications such as surfactant and polymer wrapping. Here we report a covalent cross-linking strategy to strengthen MOFs ~ PDMS interfaces. Zirconium MOFs (UiO-66-NH 2 ) were modified with trimethoxysilan (TMS), which could further react with silanol terminated PDMS to enhance UiO-66 ~ PDMS interface compatibility. High content UiO-66-TMS (up to 50 wt%) were loaded into PDMS while retaining good membrane formation ability, mechanical properties and pervaporation selectivity, in contrast to pristine UiO-66-NH 2 that decreases membrane strength and separation performances even at much lower loading content (10 wt%). Flux of mixed matrix membranes in dehydrating ethanol-water mixtures was highly improved while retaining the selectivity. It allows for the efficient production of concentrated ethanol (equivalent flux: 2234 g/m 2 h; ethanol in permeate: 53 wt%) from dilute feed through two-times consecutive pervaporation at 40 °C. Moreover, the membrane with covalently enhanced interfaces exhibit stable performance during 100 h continuous operation.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2019
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IF 3.375
Tao Bao,Ying Su,Nan Zhang,Yan Gao,Sicen Wang
Immobilization of metal–organic frameworks (MOFs) on multiple substrates is important and challenging in functional materials fields till date. Cotton is a promising carrier material with excellent performance, such as large specific area, mechanical strength and stability, good biocompatibility, and hygroscopicity. In this study, based on the coordination of carboxyl groups and Zr-OH groups, a novel carboxyl cotton chelator-zirconium-based metal–organic framework (CCC@Zr-MOF) was successfully fabricated. The surface of the cotton was first modified by citric acid. Zr-MOF precursor was grown on the carboxyl modified cotton by coordination bond to prepare Zr6O4(OH)4 cluster modified cotton (CCC@Zr6O4(OH)4). Then, Zr-MOF would form and immobilize on CCC@Zr6O4(OH)4 to obtain CCC@Zr-MOF. The CCC@Zr-MOF was characterized by field emission scanning electron microscope equipped with an energy-dispersive X-ray spectrometer, Fourier transform infrared spectroscopy, X-ray diffraction, X-ray photoelectron spectra, and Brunauer–Emmett–Teller. The successful formation of Zr-MOF on the surface of cotton has been demonstrated. CCC@Zr-MOF was packed in the pipette tip for the solid-phase extraction to evaluate its adsorption property for phenolic acid compounds from complex matrix sample. The results showed that CCC@Zr-MOF performed an efficient adsorption and selectivity.
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Journal of CO2 Utilization
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2018
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IF 5.503
Keng Xuan,Yanfeng Pu,Feng Li,Aixue Li,Jing Luo,Lei Li,Feng Wang,Ning Zhao,Fukui Xiao
A series of trifluoroacetic acid (TFA) modulated metal-organic frameworks UiO-66 catalysts were synthesized for the direct synthesis of dimethyl carbonate (DMC) from CO 2 and methanol in this work. Characterization results show that the surface area, pore size, pore volume as well as the amount of missing-linker defects, Lewis acid site, Lewis basic site and hydroxyl of UiO-66-X can be tuned by regulating the amount of TFA modulator. Catalytic activity assessments reveal that TFA modulation enhanced the activity of UiO-66-X. The catalytic activity improvement of the UiO-66-X could be attributed to the increased amount of active sites and the enlargement of porosity originated from TFA modulation. Moreover, a possible reaction mechanism for DMC synthesis from CO 2 and methanol over UiO-66-X was proposed based on the in situ FT-IR results.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2018
·
IF 3.649
Yunzhe Jiang,Chuanyao Liu,Jürgen Caro,Aisheng Huang
A new UiO-66-NH 2 based MOF named UiO-66-NH 2 @ICA has been prepared by grafting imidazole-2-carbaldehyde (ICA) to UiO-66-NH 2 through a post-synthesis reaction via amine condensation. FESEM , XRD , 1 H NMR, FT-IR and N 2 adsorption were used to characterize the morphology and structure of UiO-66-NH 2 @ICA. The grafted ICA mainly reduces the pore volume of UiO-66-NH 2 but increases the number of nitrogen atom as binding site of CO 2 . The UiO-66-NH 2 @ICA showed less BET surface area but a higher CO 2 /CH 4 adsorption selectivity in comparison with UiO-66-NH 2 . UiO-66-NH 2 @ICA and UiO-66-NH 2 crystals were dispersed in Matrimid ® 5218 to form mixed-matrix membranes (MMMs). Single gas permeation and mixed gas separation was carried out to investigate the effects of filler loading and feed gas pressure on the separation performances of the MMMs. The UiO-66-NH 2 @ICA/Matrimid ® MMM with 10 wt % filler showed a high CO 2 /CH 4 selectivity with a separation factor of 64.7, which is an increase by 40% in comparison with UiO-66-NH 2 /Matrimid ® MMM.
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Nanomaterials
·
2018
·Vol. 8
·期 10
·781
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IF 3.504
Xinli Yang,Nan Wu,Yongxia Miao,Haobo Li
Tungsten oxide (WO3) and boron oxide (B2O3) were irreversibly encapsulated into the nanocages of the Zr-based metal organic framework UiO-66, affording a hybrid material B2O3-WO3/UiO-66 by a simple microwave-assisted deposition method. The novel B2O3-WO3/UiO-66 material was systematically characterized by X-ray diffraction, Fourier transform infrared spectroscopy, N2adsorption, ultraviolet–visible diffuse reflectance spectroscopy, scanning electron microscopy, transmission electron microscopy, X-ray phosphorescence, and Fourier transform infrared (FTIR)-CO adsorption methods. It was found that WO3and B2O3were highly dispersed in the nanocages of UiO-66, and the morphology and crystal structure of UiO-66 were well preserved. The B2O3species are wrapped by WO3species, thus increasing the polymeric degree of the WO3species, which are mainly located in low-condensed oligomeric environments. Moreover, when compared with WO3/UiO-66, the B2O3-WO3/UiO-66 material has a little weaker acidity, which decreased by 10% upon the B2O3introduction. The as-obtained novel material exhibits higher catalytic performance in the cyclopentene selective oxidation to glutaraldehyde than WO3/UiO-66. The high catalytic performance was attributed to a proper amount of B2O3and WO3with an appropriate acidity, their high dispersion, and the synergistic effects between them. In addition, these oxide species hardly leached in the reaction solution, endowing the catalyst with a good stability. The catalyst could be used for six reaction cycles without an obvious loss of catalytic activity.Keywords:UiO-66;WO3;B2O3;metal organic frameworks;cyclopentene;glutaraldehyde
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Inorganic Chemistry Frontiers
·
2019
·Vol. 6
·期 10
·2727-2735
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IF 5.934
Xue Song,Pan Yang,Jingchuan Wang,Xiaochong Zhao,Yuanlin Zhou,Yintao Li,Lijun Yang
The exploration of highly efficient catalysts for the hydrolysis of hydrous hydrazine is of great significance for the achievement of future hydrogen economy. In this regard, herein, a catalyst with NiFePd loaded on the metal–organic framework (MOF) UiO-66 was successfully prepared by a simple and safe chemical impregnation method. Due to its high specific surface area, the as-prepared NiFePd/UiO-66 catalyst exhibited efficient catalytic performance for the generation of hydrogen from hydrous hydrazine in an alkaline solution. The results showed that the Ni0.25Fe0.25Pd0.5/UiO-66 catalyst exhibited optimal properties for the decomposition of hydrous hydrazine in an alkaline aqueous solution with a nearly 100% hydrogen selectivity, good activity, and the high total turnover frequency (TOF) value of up to 662.4 h−1 at 80 °C. Moreover, the Ni0.25Fe0.25Pd0.5/UiO-66 catalyst exhibited good durability, which slightly decreased after five cycles of catalytic reaction at 60 °C.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2017
·Vol. 32
·期 2
·e4049
·
IF 2.319
Xiaowen Tong,Zhiquan Yang,Jinna Feng,Ying Li,Hongguo Zhang
Semiconductor-based photocatalysis is an environmental friendly and cost-effective technique for water treatment. Due to their unique properties, metal–organic frameworks (MOFs) are considered as ideal platform to develop composite photocatalyst. In this study, Bismuth oxychloride (BiOCl) was first attempt to be incorporated with highly stable MOFs, UiO-66(Zr) by hydrothermal reaction. Different characterization methods including X-ray diffraction, Scanning electron microscopy, Fourier transform infrared spectroscope, X-ray photoelectron spectroscopy had been used to prove the successful synthesis of composite photocatalyst. The resultant BiOCl/UiO-66 composite showed higher photodegradation performance of Rhodamine B (RhB) under ultraviolet and visible light irradiation than that of pristine materials and their mechanically mixed sample. In addition, the composite exhibited good structural stability and reusability. The photocatalytic mechanism of RhB degradation over the composite under visible light proceeded via a photosensitization process. A better adsorptivity of RhB and effective electron transfer within the hybrid material might be responsible for the enhanced photocatalytic performance.
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