Materials
·
2021
·Vol. 14
·期 9
·2419
·
IF 3.623
Mingfei Chen,Yingxue Tu,Songhai Wu
There is an urgent need to develop catalytic degradation technologies for chemical warfare agents (CWAs) that are environmentally friendly and do not require secondary treatment. UiO-66-NH2and other metal–organic frameworks (MOFs) based on zirconium have been shown to promote the catalytic degradation of CWAs. At the same time, MOFs have been studied, and they have shown interesting properties in CWA removal because of their ultrahigh surface area, tunable structures, and periodically distributed abundant catalytic sites. However, MOFs synthesized by conventional methods are mostly powdery crystals that are difficult to process and have poor mechanical stability, which largely limit the development of MOFs in practical applications. An emerging trend in MOF research is hybridization with flexible materials. Polymers possess a variety of unique attributes, such as flexibility, thermal and chemical stability, and process ability, and these properties can be combined with MOFs to make a low-cost and versatile material that also provides convenience for the subsequent integration of such MOFs into independent substrates or textiles. In this article, we used a green and simple method to coat the surface of UiO-66-NH2with polydopamine (PDA), PDA can promote the catalytic hydrolysis of UiO-66-NH2to DMNP (a simulant of chemical warfare agents). Additionally, it can adsorb the toxic hydrolysis product p-nitrophenol, avoiding the trouble of secondary treatment. The half-life of UiO-66-NH2coated with polydopamine (UiO-66-NH2@PDA) for catalytic hydrolysis is 8.9 min, and that of pure UiO-66-NH2is 20 min. We speculate that the surface coated with PDA can improve the diffusion of DMNP to the active sites of UiO-66-NH2.
研究领域:
材料科学
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环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
RARE METALS
·
2024
·
IF 9.6
Liu Cheng,Shi Ying-Zhang,Chen Qi,Ye Bing-Hua,Bi Jin-Hong,Yu Jimmy C.,Wu Ling
Defect engineering in metal organic frameworks (MOFs) has captured significant attention in the field of photocatalysis. A series of UiO-66(Ce) (UiO = University of Oslo) MOFs with different contents of missing-linker defects have been developed for the photocatalytic selective oxidation of benzylamine (BA) and thioanisole (TA) under visible light. The introduction of missing-linker defects promotes the formation of unsaturated Ce sites with a high Ce 3+ content. It also generates a high concentration of oxygen vacancies. In situ Fourier transform infrared spectroscopy (FTIR) results revealed that BA and TA molecules were activated on coordinatively unsaturated Ce sites via the H–N···Ce and the C–S···Ce interactions, respectively. Simulated in situ electron paramagnetic resonance (EPR) data indicate that O 2 activation and reduction occur at coordinatively unsaturated Ce 3+ sites to form ·O 2 – . This is accelerated by the Ce 3+ /Ce 4+ redox cycle associated with the photogenerated electrons. The corresponding photogenerated holes are involved in the deprotonation of the activated BA and TA. The most active sample exhibits 98.4% and 95.5% conversion rates for BA and TA oxidation. Mechanisms for the molecular activation are proposed at the molecular level. Graphical abstract
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Yuchen Cui,Xiaolei Cui,Lubomira Tosheva,Chunzheng Wang,Yongming Chai,Zixi Kang,Qiang Gao,Kun Wang,Zhihan Zhang,Hailing Guo,Daohong Xia,Daofeng Sun
Effective separation of CO 2 from CH 4 is crucial for the purification of natural gas, which requires membrane materials with high permeability, selectivity, and stability of under high pressures. In this work, a high CO 2 -affinity MOF-based nanofiller (P in @NH 2 -UiO-66) was prepared and integrated in polyetherimide (PEI) to prepare mixed matrix membranes (MMMs) for enhanced CO 2 /CH 4 separation capabilities. The P in @NH 2 -UiO-66 nanofiller comprised an in situ-formed polyethyleneimine-NH 2 -UiO-66 composite prepared via a one-pot synthesis. The polyethyleneimine was covalently attached to the H 2 BDC-NH 2 ligand allowing for a stronger integration within the PEI matrix. The polyethyleneimine affects the nucleation of MOF, leading to miniaturization of the MOF particles. The smaller-sized filler is beneficial for improved interaction at the filler-matrix interface. The numerous amino functionalities grafted onto the NH 2 -UiO-66 increased the CO 2 adsorption sites, thereby enhancing the affinity for CO 2 . Owing to the improved interaction, the elevated CO 2 attraction, and the inherent properties of the porous NH 2 -UiO-66, the fabricated MMMs preformed superior in separating CO 2 /CH 4 . The 30-P in @NH 2 -UiO-66-PEI membrane (containing 30 wt% nanofiller) exhibited a CO 2 /CH 4 selectivity of 27.7 and a CO 2 permeability of 2498.9 Barrer. The CO 2 permeability was 21 times greater than that of the pristine PEI membrane, and 4 times higher compared to P@NH 2 -UiO-66 MMM with polyethyleneimine modified MOF filler prepared by a traditional wet impregnation method. Additionally, the novel MMM demonstrates excellent separation stability under conditions that mimic industrial settings, demonstrating its potential application for natural gas purification.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2017
·
IF 4.601
Xiaotian Zhang,Pengcheng Huang,Aili Liu,Mingyuan Zhu
Owing to the high prices and other shortcomings associated with the existing methods of complex catalyst preparation, we used the UIO-66(Zr) metal–organic frameworks to directly catalyze the oxidative desulfurization (ODS) reaction. The synthesized UIO-66(Zr) was characterized using nitrogen adsorption–desorption isotherm analysis, X-ray diffraction, Fourier transform infrared spectroscopy, transmission electron microscopy, and X-ray photoelectron spectroscopy. Under optimal reaction conditions, the ODS conversion of dibenzothiophene (DBT) reached 100%. This excellent catalytic activity was attributed to the unsaturated coordination of Zr, which may produce beneficial Lewis acid sites.
研究领域:
化学工程
·
催化材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
·
2024
·
IF 8.1
Xiaochang Lin,Bo Sun,Pengsen Wang,Min Zhao,Dejia Liu,Qiyu Zhang,Baile Wu,Dezhao Liu
A magnetic Fe n UiO-66 adsorbent was created to achieve high phosphate adsorption capacity. The incorporation of Fe 3 O 4 facilitated the precipitation and growth of UiO-66 during crystallization, resulting in a shift towards a multilayer heterogeneous distribution of adsorption sites. The increased Fe 3 O 4 content notably enhanced the magnetic properties of Fe n UiO-66, while negligibly affecting its adsorption performance. The Fe 1.5 UiO-66 demonstrated exceptional phosphate adsorption capacity (136.54 mg/g), outstanding selectivity, and sustained reusability, with an 80% removal efficiency after nine cycles of treating actual water. The mechanism of phosphate adsorption by Fe n UiO-66 involved electrostatic attraction, ligand exchange, and linker exchange. Notably, while linker exchange significantly contributed to high adsorption capacity, it resulted in irreversible damage to the Fe n UiO-66 crystal. These unequivocal findings will serve as a solid foundation for further research and underline the critical role of linkers in the process of phosphate adsorption.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Desalination and Water Treatment
·
2024
·
IF 1
Honghuan Yin,Huaiwen Wang,Dongai Wang,Miaomiao Shi,Xi Xu,Jiaqi Yang
Developing low-cost and stable adsorbent is urgent and attractive to remove hazardous dye from water. In this study, zirconium based metal-organic framework (NH 2 -UiO-66) was grown on waste wool fibers and the fabricated composite adsorbent (NH 2 -UiO-66/wool) was used to remove anionic dye methyl orange (MO). After characterizing the adsorbents, we determined the effect of pH and initial concentration of MO on adsorption performance. Moreover, adsorption kinetics and isotherms were conducted to reveal the adsorption mechanism. The results showed that NH 2 -UiO-66/wool achieved the highest adsorption capacity at natural pH with the maximum adsorption of 61.0 mg/g adsorbent, which is higher than most biomass based adsorbents. Moreover, NH 2 -UiO-66/wool enabled a broad range of pH (3−11) and initial concentration of MO (10–50 mg/L). Adsorption kinetics and isotherms of NH 2 -UiO-66/wool fitted well with pseudo-second-order model and Langmuir mode, respectively. NH 2 -UiO-66/wool presented 40.3 times higher of kinetics constant than that of original wool in the presence of initial MO concentration of 10 mg/L due to the positive nature of NH 2 -UiO-66. Ultimately, NH 2 -UiO-66/wool presented excellent regeneration ability with 500 mg/L NaCl solution and regeneration efficiency remained 98% after 10 cycles. Overall, this work may provide new insights into the development of MOFs/wool adsorbents for enhanced dye removal.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL RESEARCH
·
2025
·
IF 7.7
Zhilun Liu,Lei Zhao,Xu He,Shuang Lu,Ding Hou,Jun Ma,Xueyan Li,Fuqiang Guo
In this study, acetic acid (HOAc) was applied to induce missing linker defects on UiO-66 via coordination competition strategy and its role on the outstanding adsorption capacity for ketoprofen (KTP) was investigated systematically. This strategy was proved to simultaneously modulate the defect sites and increase the pore size, pore volume, and surface area of the UiO-66. The missing linker defects constructed porous structure, which dramatically enhanced specific adsorption for KTP. Results showed that the surface area of UiO-66 possessed 27 % enhancement as defect sites increased (from 875.38 to 1439.86 m 2 /g) and exhibited good linearity ( R 2 = 0.998) with adsorption capacity (from 645.5 to 1136.4 mg/g). The adsorption performance of UiO-66 on KTP was investigated on both kinetics and isotherms which were fit by the pseudo-second-order kinetic model and Langmuir model, respectively. According to the Arrhenius equation and Van't Hoff equation, the activation energy increased with missing linker defects and the adsorption is a spontaneous, exothermic and randomness–increasing process. Remarkably, the defective UiO-66 maintained high adsorption resilience across a broad pH range and demonstrated superior selectivity for KTP in the presence of competing ions and humic acid (HA). The results of characterization (FTIR, XPS) and DFT calculations indicated that the adsorption of KTP was primarily driven by chemisorption at the Lewis acid metal centers of UiO-66, accompanied by secondary interactions such as van der Waals forces and hydrogen bonding.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2018
·
IF 3.141
Yan Li,Jiangtao Liu,Kehu Zhang,Lei Lei,Zhongli Lei
A hybrid polymer–MOFs architecture UiO-66-NH2@PMAA was synthesized by tethering polymethacrylic acid (PMAA) onto the surface of the metal–organic frameworks UiO-66-NH2, and it was further employed for pectinase immobilization by electrostatic interactions. The hybrid architecture was prepared through a combination of atom transfer radical polymerization (ATRP), click chemistry and postsynthetic modification (PSM). The optimal immobilization parameters were at 25 °C and pH 4.0 with 10 U/mL of pectinase for 2 h, under which pectinase showed the highest enzymatic activity (1.215 U/mg) and protein loading (448.5 mg/g), respectively. Compared with free pectinase, the immobilized was found to exhibit higher pH, thermo, and storage stability. Additionally, the immobilized pectinase had remarkable reusability, the residual activity reached as high as 81% after 8 cycles continuously. Meanwhile, the desorption of immobilized pectinase can be achieved by changing pH values of the medium. Obviously, the UiO-66-NH2@PMAA with attractive properties is highly promising for enzyme immobilization.
研究领域:
生物化学
·
材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2014
·
IF 2.063
Yan Cao,Yunxia Zhao,Zijian Lv,Fujiao Song,Qin Zhong
New composites of UiO-66 and graphene oxide (GO) were synthesized and tested as CO 2 adsorbents at room temperature. The materials and the parent composite components were characterized using X-ray diffraction (XRD), thermo-gravimetric analysis (TGA), nitrogen adsorption–desorption isotherm analysis, scanning electron microscopy (SEM), and FT-IR spectroscopy. The CO 2 isotherms on the UiO-66/GO composites and the UiO-66 were measured by a static volumetric method separately. Experiments of multiple adsorption/desorption cycles were conducted to estimate reversibility of CO 2 on the UiO-66/GO. The results showed that the BET surface area of the composites was higher than that of the parent UiO-66, and the adsorption capacities of CO 2 on the composites were greatly higher than that on the UiO-66 sample. The composite UiO-66/GO-5 exhibited the maximum CO 2 uptake of 3.37 mmol/g at 298 K and 1 bar, which increased by 48% in comparison with that of the UiO-66, and was much higher than those of the conventional activated carbons and the zeolites. The CO 2 adsorption capacity was dependent on the BET surface area and the micropore volume of the composites. Finally, the adsorption/desorption cycle experiment revealed that the adsorption performance of UiO-66/GO-5 was fairly stable, without noticeable degradation in the adsorption capacity of CO 2 after 6 cycles. Therefore, this kind of composites has a potential application on CO 2 capture technologies to mitigate global warming.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2015
·Vol. 5
·期 23
·17601-17605
·
IF 3.84
Yueyue Tan,Wei Zhang,Yilong Gao,Jianxiang Wu,Bohejin Tang
Metal organic frameworks (MOFs), a kind of crystalline porous material, have attracted much attention due to their high surface area and controllable porous structure. In this paper, we present a new synthesis of Zr-based MOFs with high electrochemical performance by a facile synthetic method of changing the reaction temperature and stirring condition. By varying the reaction temperature, different particle sizes and degrees of crystallization can be obtained. This paper focuses on the electrochemical properties of Zr-based MOFs as electrode materials in supercapacitors. The maximum specific capacitance of Zr-MOF1 obtained at 50 °C can reach up to 1144 F g−1 at a scan rate of 5 mV s−1, which is far higher than Zr-MOF2 (811 F g−1), Zr-MOF3 (517 F g−1) and Zr-MOF4(207 F g−1). The results of electrochemical measurements show that the Zr-MOF1 we synthesized has excellent capacitance performance and good cycling stability over 2000 cycles, which makes it a promising supercapacitor electrode material.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Journal of CO2 Utilization
·
2024
·
IF 7.2
Heming Deng,Haoshuang Gu
Two-dimensional membranes are considered the next generation separation membrane with great application potential due to their excellent separation performance, good mechanical strength and thermal stability compared with traditional membrane materials. In this work, the flexible NH 2 -UIO-66@MXene membrane was successfully prepared for gas separation by loading NH 2 -UIO-66 particles onto Ti 3 C 2 nanosheets based on an in-situ growth strategy. A LiF-HCl mixed solution was used as the etchant to obtain the Ti 3 C 2 nanosheets. The loading of NH 2 -UIO-66 particles can regulate the interlayer spacing of Ti 3 C 2 nanosheets, improving the specific surface area of Ti 3 C 2 and the adsorption capacity for specific gases. The -NH 2 group in NH 2 -UIO-66 enabled preferential adsorption of CO 2 over H 2 , and the CO 2 molecules adsorbed in the channel can even block the molecules passing through, increasing the resistance of CO 2 diffusion. As a result, the NH 2 -UIO-66@Ti 3 C 2 hybrid membrane realizes the selective separation of H 2 /CO 2 mixed gas, and the separation selectivity is as high as 155. The gas separation selectivity and permeation of the final prepared NH 2 -UIO-66@MXene were enhanced and exceeded the upper limit of Robeson upper bound (2017).
研究领域:
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
INORGANIC CHEMISTRY COMMUNICATIONS
·
2025
·
IF 5.4
Jun Hu,Ye Cao,Lu Cai,Guanzheng Wu,Yuanyu Ge,Ling Lin,Ziyin Li
Metal-organic frameworks (MOFs) based proton conductors, as a promising alternative to proton exchange membranes, are in urgent need of developing effective methods to enhance their proton conductivity. Here, we report the enhanced and ultra-fast proton conduction facilitated by the post-covalent bonding of the flexible zwitterionic arm (sulfobetaine methacrylate: SBMA) with UiO-66. A new zwitterionic MOF based proton conductor (UiO-66-SB) exhibits the higher proton conductivity of 0.1 × 10 −2 S·cm −1 but with the activation energy ( E a ) of only 5.8 kJ/mol at 85 °C and 90 % RH, indicating ultra-fast proton transport. This result was attributed to the continuous and shorter hydrogen bonded network formed by flexible zwitterionic arms, water molecules, and residual –NH 2 . This work also demonstrates that zwitterions are highly advantageous as proton carrier media for the post-modification of MOFs.
研究领域:
材料科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）