Molecular Catalysis
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2024
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IF 3.9
Pushuang Xing,Cong Li,Yixin Chen,Rong-Lan Zhang
PMoV 2 was encapsulated in four MOFs (MIL-101, HKUST-1, UiO-67, ZIF-8) with different cavity sizes and window sizes using a hydrothermal synthesis method. Then, a layer of mesoporous silica was coated on the surface of the MOFs to obtain four designed three-layer encapsulated catalysts 30%PMoV 2 @MOF@mSiO 2 . The physicochemical properties of the catalysts were characterized through various characterization methods, and the influence of different MOF window sizes of the four catalysts on the removal rate of four thiophene sulfides was investigated. The optimal reaction conditions were also explored for the optimal catalyst. The results indicate that under simulated fuel of 2400 ppm, 30%PMoV 2 @UiO-67@mSiO 2 owns the highest catalytic activity. Under optimal conditions, the total removal rate of four thiophene compounds was 91.52 %, and after ten cycles, the efficiency could still reach 86.24 %. This is attributed to the sufficient cavity size of UiO-67, which provides assurance for the loading of PMoV 2 and the large window size, making it possible for the smooth reaction between sulfides and PMoV 2 .
研究领域:
材料科学
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催化化学
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环境科学
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产品关联
DOI
高影响因子
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
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化学工程
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DOI
高影响因子
MOLECULES
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2024
·Vol. 29
·期 17
·4195
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IF 4.2
Yu Wang,Zhimin Yang,Xichang Wu,Wenxuan Quan,Qi Chen,Anping Wang
In the present study, an acid catalyst (UiO-66-SO3H) with Brønsted and Lewis acid sites was synthesised for the preparation of highly efficient biodiesel from oleic acid and methanol using chlorosulphonic acid sulfonated metal–organic frameworks (UiO-66) prepared with acetic acid as a moderator. The prepared catalysts were characterised using XRD, SEM, FT-IR and BET. The catalytic efficiency of the sulfonated catalysts was significantly improved and successful sulfonation was demonstrated by characterisation techniques. Biodiesel was synthesised by the one-pot method and an 85.0% biodiesel yield was achieved under optimum conditions of the reaction. The esterification reaction was determined to be consistent with a proposed primary reaction and the kinetics of the reaction was investigated. A reusability study of the catalyst (UiO-66-SO3H) was also carried out with good reproducibility. In conclusion, the present study provides some ideas for the synthesis of catalysts with high catalytic activity for the application in the catalytic preparation of biodiesel.
研究领域:
化学工程
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催化科学
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DOI
PubMed
高影响因子
Polymers
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2024
·Vol. 16
·期 2
·275
·
IF 4.7
Shaojun Chen,Youhan Zeng,Weifeng Bi,Haitao Zhuo,Haiqiang Zhong
The flame-retardancy of polymeric materials has garnered great interest. Most of the flame retardants used in copolymers are functionalized additives, which can deteriorate the intrinsic properties of these materials. As a new type of flame retardant, functionalized metal–organic frameworks (MOFs) can be used in surface coatings of polymers. To reduce the flammability, a mixture of phytic acid, multi-wall carbon nanotubes, zirconium-based MOFs, and UiO-66 was coated on a PC/ABS substrate. The structure of the UiO-66-based flame retardant was established by FT-IR, XRD, XPS, and SEM. The flammable properties of coated PC/ABS materials were assessed by LOI, a vertical combustion test, TGA, CCT, and Raman spectroscopy. The presence of a UiO-66-based coating on the PC/ABS surface resulted in a good flame-retardant performance. Heat release and smoke generation were significantly reduced. Importantly, the structure and mechanical properties of PC/ABS were less impacted by the presence of the flame-retardant coating. Hence, this work presents a new strategy for the development of high-performance PC/ABC materials with both excellent flame-retardancy and good mechanical properties.
研究领域:
材料科学
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化学工程
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF CATALYSIS
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2024
·
IF 6.5
Cheng Liu,Huiling Chen,Qi Chen,Jinhong Bi,Jimmy C. Yu,Ling Wu
A series of Al 3+ -doped UiO-66(Ce) MOFs (U(Ce x Al 1−x )) was developed to reveal the roles of metal doping on active site formation and substrate activation in photocatalytic selective transformation of amines to imines. Al 3+ doping induced crystal structure distortion to form coordinately unsaturated metal (Al, Ce) sites as Lewis acid sites to chemisorb and activate benzylamine (BA). In situ FTIR revealed that the Al site with stronger acid strength facilitated BA activation. The activation degree of N–H bonds in BA was evaluated by changes of calculated force constant. The intermediate products were confirmed through time-dependent in situ FTIR. The Al 3+ -doped sample U(Ce 0.90 Al 0.10 ), the optimal catalyst, showed a significantly increased BA conversion (97.6 %) than that (47.5 %) of undoped sample, which was attributed to enough active sites and the optimal charge mobility. Finally, the present study proposes a synergistic photocatalytic mechanism associated with molecular activation to demonstrate selective oxidation pathways at the molecular level.
研究领域:
材料科学
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化学工程
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催化化学
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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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
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化学工程
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产品关联
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
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催化化学
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产品关联
DOI
高影响因子
CHEMOSPHERE
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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
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产品关联
DOI
PubMed
高影响因子
Desalination and Water Treatment
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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
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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.
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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
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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
危险品化学品经营许可证（带存储）