JOURNAL OF APPLIED POLYMER SCIENCE
·
2023
·Vol. 140
·期 25
·e53978
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IF 3
Xiaocan Zhang,Huixiao Ma,Tong Pei,Ruochen Zhang,Yiran Liu
Incorporating phosphotungstic acid (HPW) in proton exchange membranes (PEMs) is an effective way to improve proton conductivity, but its leakage remains a problem. It can be solved by immobilizing acid in membranes to enhance the stability of PEMs. Herein, we proposed a novel sulfonated poly(ether ether ketone) (SPEEK) composite membrane (SPEEK/HPW@MIL) that was prepared by blending amino-modified MIL-101(Cr) to anchor HPW. In this work, HPW was anchored through hydrogen bond to minimize its leakage and enhance the overall compatibility. The incorporation of MIL-101(Cr)-NH 2 also helped lower the swelling ratio and improve the dimensional stability. Compared with pristine SPEEK and SPEEK/MIL membrane, the proton conductivity of the SPEEK/HPW@MIL composite membrane increased by 26% and 14%, respectively. The superior performance recommended a promising conception for anchoring HPW in PEMs.
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Arabian Journal of Chemistry
·
2023
·
IF 6
Qingrong Han,Fei Liu,Chengjiu Wang,Zhentao Tang,Cheng Peng,Yuzhu Tan
In recent years, the quality and safety issues of Chinese medicinal herbs have received great attention worldwide. Thereinto, heavy metal contamination has been one of the most serious concerns. Compared to the wide research in the analysis of heavy metals in medicinal herbs, the studies on the removal of heavy metals are relatively limited. In this study, polyethylene glycol functionalized Fe 3 O 4 @MIL-101(Cr) (Fe 3 O 4 @MIL-101(Cr)@PEG) was designed and synthesized to remove heavy metals from the decoction of Ligusticum chuanxiong Hort. The in-house fabricated Fe 3 O 4 @MIL-101(Cr)@PEG was characterized by a porous structure and a large specific surface area. Then, the efficiency of the material for the removal of five heavy metals was tested under optimal adsorption conditions. Meanwhile, the content of Senkyunolide A, Senkyunolide I, and Ferulic acid, the solid content, and the HPLC fingerprints similarity were used as the quality monitoring indicators of Ligusticum chuanxiong Hort decoction before and after the heavy metal removal. Results showed that the magnetic nanomaterial had excellent removal efficiency for As 5+ (81.4 %), Cd 2+ (88.19 %), and Pb 2+ (83.79 %) and certain removal efficiency for Ni 2+ (51.59 %) and Zn 2+ (55.4 %) under the spiked concentration of 50 μg/mL. The content of Senkyunolide A, Senkyunolide I, and Ferulic acid were decreased by less than 8.00 % after the removal of heavy metals. Besides, the loss rate of solid content was only 0.18 %, and the fingerprints similarity was over 99.9 %. The results indicated that Fe 3 O 4 @MIL-101(Cr)@PEG could efficiently and selectively remove heavy metals from Ligusticum chuanxiong Hort without affecting its effective components. Due to the advantages of low-cost, simple manipulation, and good efficiency, the material can be recommended for heavy metals removal from the aqueous solutions of medicinal herbs, providing a new and promising application for the removal of exogenous contaminants in medicinal herbs.
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BIOMASS & BIOENERGY
·
2022
·
IF 5.774
Jiawen Hao,Wei Mao,Guirong Ye,Yi Xia,Cui Wei,Ling Zeng,Jinghong Zhou
5-hydroxymethylfurfural (HMF) is considered a promising platform chemical, from which numerous chemicals can be produced. Hence, developing an efficient catalytic system to convert glucose into HMF has drawn considerable attention. In this study, a series of Lewis acidic Sn–Cr bimetallic metal–organic frameworks, MIL-101(Cr, Sn), with different Sn ion loading were synthesized hydrothermally using acetic acid as the mineralizer and water as the solvent. The resulting MIL-101(Cr, Sn) was systematically analyzed as a catalyst for the conversion of sugar to HMF. Moreover, the effects exerted by various reaction parameters on HMF yield and selectivity were investigated. With glucose as the substrate and 0.5-wt% H 2 SO 4 as a catalyst, an 85.75% glucose conversion with 22.64% HMF yield and 26.41% selectivity was achieved. Meanwhile, these parameters were improved via addition of MIL-101(Cr, Sn)-0.1. That is, glucose conversion, HMF yield, and selectivity were increased to 86.36%, 60.75%, and 70.35%, respectively, when using MIL-101(Cr, Sn)-0.1 and H 2 SO 4 as the catalyst under the same reaction conditions. The MIL-101(Cr, Sn) structure enabled high stability of the catalyst in aqueous solutions with different pH values, while improving its thermal stability. Moreover, the catalyst could be reused several times despite a slight reduction in its catalytic activity . The current results illustrate that MIL-101(Cr, Sn) is an excellent acid and sustainable catalyst for the production of HMF from fructose, glucose, and starch .
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Jiaxing Wang,Yaseen Muhammad,Zhu Gao,Syed Jalil Shah,Shuangxi Nie,Lihan Kuang,Zhongxing Zhao,Zhiwei Qiao,Zhenxia Zhao
Adsorption of volatile organic compounds (VOCs) under high humidity is crucial for metal–organic frameworks (MOFs) in practical applications. To enhance competitive adsorption of VOCs under humidity, polyethylene glycol (PEG) with hydrophobic short-chains was implanted as hydrophobic barrier into MIL-101(Cr). Characterization and simulation results showed that the terminal –OH groups of PEG chains were coordinated with the Cr sites in MIL-101(Cr) and formed a hydrophobic pore (11.2 Å) of “cage-in-cage” geometry. PEG chains significantly hindered the diffusion of water into the MOFs while allowed toluene molecules. The new hydrophobic pores of PEG 5 @MIL-101 enhanced adsorption capacity and diffusivity for toluene by 30.8% (4.68 mmol/g at 1 mbar) and 31.5% (1.88 × 10 −2 ), while decreased adsorption capacity and diffusivity for water by 53.7% and 26.8% compared to primary MOF. Breakthrough curve showed 3.3 times of toluene working capacity on PEG 5 @MIL-101 at 80% RH compared to pristine MIL-101(Cr).
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Catalysts
·
2020
·Vol. 10
·期 4
·453
·
IF 3.52
Emmanuelia Akimana,Jichao Wang,Natalya V. Likhanova,Somboon Chaemchuen,Francis Verpoort
Mild reaction conditions (nearly room temperature and atmospheric CO2pressure) for the cycloaddition of CO2with epoxides to produce cyclic carbonates were investigated applying MIL-101(Cr) as a catalyst. The MIL-101 catalyst contains strong acid sites, which promote the ring-opening of the epoxide substrate. Moreover, the high surface area, enabling the adsorption of more CO2(substrate), combined with a large pore size of the catalyst is essential for the catalytic performance. Additionally, epoxide substrates bearing electron-withdrawing substituents or having a low boiling point demonstrated an excellent conversion towards the cyclic carbonates. MIL-101(Cr) for the cycloaddition of carbon dioxide with epoxides is demonstrated to be a robust and stable catalyst able to be re-used at least five times without loss in activity.Keywords:MIL-101;heterogeneous catalyst;CO2cycloaddition;carbonate;ambient conditions
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DALTON TRANSACTIONS
·
2019
·Vol. 48
·期 16
·5384-5396
·
IF 4.052
Xueping Quan,Zhongqiao Sun,Hao Meng,Yide Han,Junbiao Wu,Junli Xu,Yan Xu,Xia Zhang
Developing novel solid adsorbents with high efficiency and excellent selectivity is always an important target in the removal of toxic metal ions from waste water. In this study, a composite nano-adsorbent NH2-mSiO2@MIL-101(Cr) has been fabricated and applied in the efficient removal of Pb(II) and Cr(VI) for the first time. The nanocomposites were characterized by using field emission scanning electron microscopy (FESEM), X-ray diffraction (XRD), fourier-transform infrared (FT-IR) spectroscopy and thermal gravimetry analysis (TG). The results indicate that a typical core@shell structure has been fabricated by fully coating a mesoporous SiO2 shell over the micro/mesoporous MIL-101(Cr). As a result, the surface charge and the zeta potentials change significantly. Two toxic metal ions, namely, Pb(II) and Cr(VI) were chosen as the main adsorption targets to evaluate the surface adsorption activities. The adsorption conditions were optimized, the influences of other coexisting ions were explored, and the adsorption selectivity was investigated. Interestingly, the NH2-mSiO2@MIL-101(Cr) nanocomposites display a prominent adsorption activity compared with the original MIL-101(Cr) and non-aminated mSiO2@MIL-101(Cr) and excellent selectivity toward Pb(II) in the presence of other divalent metal ions. The adsorption kinetics and adsorption thermodynamics were simulated accordingly, and the enhanced adsorption mechanism was also suggested. The good reusability and adsorption selectivity of the NH2-mSiO2@MIL-101(Cr) suggest their potential applications in the selective removal of special metal ions such as Pb(II) from the waste water.
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PubMed
高影响因子
JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2019
·
IF 2.298
Xiuna Jia,Sijia Li,Yudan Wang,Ting Wang,Xiaohong Hou
The occurrence of numerous antibiotics, such as sulfonamides (SAs), in environmental water has recently heightened concerns in consideration of their potential threat to human health and aquatic ecosystems. The removal of pharmaceuticals by adsorption comprises some of the most promising techniques because of their easy regeneration, low cost, and high efficiency. In this work, MIL-101(Cr)@GO, with a high surface area, was synthesized. Its adsorption properties toward three SAs were examined in batch adsorption experiments to probe the underlying factors of adsorption behavior and the mechanism for the first time. The pronounced factors that influenced the adsorption and removal process were investigated. The adsorption kinetics and isotherms were studied in order to characterize the operation. The adsorption kinetics demonstrated that the adsorption process would match the pseudo-second-order kinetic model. Furthermore, the adsorption was spontaneous, entropy was decreased, and the process was exothermic, and the equilibrium data was more appropriate described by the Freundlich isotherm model. Moreover, the adsorption–desorption of MIL-101(Cr)@GO could be consecutively cycled at least five times. MIL-101(Cr)@GO exhibited remarkable removal efficiency compared to MIL-100(Fe), MIL-101(Cr), and other adsorbents. These results demonstrated that MIL-101(Cr)@GO would be a promising adsorbent for the removal of sulfonamides from water samples and even for environmental protection.
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DALTON TRANSACTIONS
·
2018
·Vol. 48
·期 3
·989-996
·
IF 4.099
Ling Yang,Tian Zhao,Ishtvan Boldog,Christoph Janiak,Xiao-Yu Yang,Qiang Li,Yan-Jia Zhou,Yong Xia,Deng-Wang Lai,Yue-Jun Liu
The concentration of benzoic acid was found to exercise efficient control over the formation of either MIL-101(Cr) or MIL-88B(Cr) under otherwise similar hydrothermal synthetic conditions. Nanocrystals of MIL-101(Cr) with ∼100 nm average size and excellent SBET = 3467 m2 g−1 are obtained at lower concentrations of benzoic acid, while at higher concentrations the microparticulated MIL-88B(Cr) product is formed. Hereby a new efficient synthetic method towards the elusive MIL-88B(Cr), yet reported only once without synthetic details, is proposed. The obtained MIL-88B(Cr) has an interesting and potentially valuable property of retaining its high-volume form (Vcell ∼ 2000 Å3) after thermal activation. The degassing of MIL-88B(Cr) in a vacuum at 250 °C yields a porous material with a SBET area of 1136 m2 g−1, which is around the theoretical maximum. The transition to the denser ‘closed’ form (Vcell ∼ 1500 Å3) occurs only at 350 °C, when all of the benzoate/benzoic acid, hindering the process, is removed.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2016
·
IF 3.299
Ning Zhuo,Yaqian Lan,Weiben Yang,Zhen Yang,Xiaomin Li,Xia Zhou,Yang Liu,Jiachun Shen,Xuntong Zhang
Porous metal-organic frameworks (MOFs) have great potential as high-effective adsorbents for water treatment. However, poor separability restricts their practical application. To overcome the drawback, both MIL-101(Cr)/sodium alginate (MIL-101(Cr)/SA) and MIL-101(Cr)/chitosan (MIL-101(Cr)/CS) composite beads were prepared and characterized. Adsorption of three selected pharmaceuticals and personal care products (PPCPs) (benzoic acid (BEN), ibuprofen (IBU) and ketoprofen (KET)) onto the two composite beads was investigated and compared with pristine SA and CS beads. Kinetic plots, pH dependence, isotherm data, and influences of ionic strength were reported. The MIL-101(Cr)/CS beads exhibit much higher adsorption capacity than SA, CS and MIL-101(Cr)/SA, and the adsorption amounts of three PPCPs onto MIL-101(Cr)/CS follow the order of KET > IBU > BEN. The adsorption amounts of the three PPCPs on the MIL-101(Cr)/CS increased quickly during the first 60 min of contact time and then achieved the adsorption equilibrium after ∼180 min. Not only the protonated amine groups but also the Cr center of the adsorbents exerted electrostatic attraction with the deprotonated carboxyl groups of contaminants, as elucidated by X-ray photoelectron spectroscopy (XPS). Based on the adsorption isotherms and π-energy analysis of three PPCPs, π-π interaction of aromatic groups between adsorbents and contaminants also contributed to the adsorption. The MIL-101(Cr)/CS beads exhibited good regenerability over several repeated adsorption/desorption cycles. Overall, this study is believed to enlarge the application of MOFs on the removal of emerging contaminants from waters.
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Analytical Methods
·
2016
·Vol. 8
·期 15
·3263-3269
·
IF 1.915
Yangjuan Wang,Kejing Du,Yifu Chen,Yijun Li,Xiwen He
Green octahedral crystals of MIL-101(Cr) were synthesized and used for the determination of Pb2+ at the trace level by differential pulse anodic stripping voltammetry (DPASV) because of their good adsorption capability for Pb2+. The synthesized MIL-101(Cr) was characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), thermogravimetric analysis (TGA) and X-ray photoelectron spectroscopy (XPS). Parameters affecting the electrochemical process, such as the pH of the electrolyte solution, the volume of the MIL-101(Cr) suspension, the potential and the time for accumulation, were investigated in detail. Under optimal conditions, the electrochemical sensor had a linear response over the concentration range of 1.0 × 10−9 to 1.0 × 10−6 mol L−1 (R2 = 0.999) with a detection limit of 5.0 × 10−10 mol L−1 (S/N = 3). The method was successfully applied to the determination in real samples and good recoveries are obtained from different spiked samples.
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MICROCHIMICA ACTA
·
2016
·Vol. 183
·期 12
·3151-3157
·
IF 4.831
Yu Haili,Long Dengying
The authors describe a highly chemiluminescent metal-organic framework (MOF) that was obtained by loading the pores of MIL-101(Cr) with luminol. Immobilization is based on Lewis acid-base interactions between the coordinatively unsaturated metal sites of MIL-101(Cr) and the amino groups of luminol. The luminol-loaded MOF displays strong chemiluminescence (CL) in the presence of hydrogen peroxide (H 2 O 2 ) in alkaline solution. Pyrophosphate (PPi), in turn, acts as a quencher of this CL. These findings have been exploited in the design of a CL based method for the determination of either H 2 O 2 or PPi. The assays for H 2 O 2 works in the 3 to 100 μM concentration range and has a detection limit of 0.5 μM. The quenchometric assay for PPi works in the 5 to 70 μM concentration range and has a 1.2 μM detection limit.
Luminol-embedded metal-organic frameworks (MOFs) with high chemiluminescent activity were prepared and used for the sensitive determination of either H 2 O 2 or pyrophosphate ions.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Yanyan Xing,Mengke Tian,Ruoman Ji,Ting Wang,Xiaohong Hou
The immobilization of bovine serum albumin (BSA) with high efficiency, good reproducibility and stability for chiral separation has attracted much attention in the medicinal field. BSA was immobilized into MIL-101(Cr) by three ways for efficient chiral separation in this research. MIL-101(Cr)@BSA was firstly prepared by adsorption, NH 2 -MIL-101(Cr) ⊂ BSA by direct bonding, and NH 2 -MIL-101(Cr) ⊂ Glu ⊂ BSA by glutaraldehyde crosslinking bonding. Compared to the other two materials, NH 2 -MIL-101(Cr) ⊂ BSA as a new enantioselective separator, with the most BSA loading rate of 437.6 mg g −1 exhibited excellent chiral separation performances and succeeded in realizing a complete chiral separation of racemic 1–phenylethanol within 14 s. It was found that the NH 2 -MIL-101(Cr) ⊂ BSA was more strongly bound to R -1-phenylethanol and the ee value could reach 100 % when the material was added in three batches. The different interactions between BSA and racemates mainly including hydrogen bonding, hydrophobic interaction and π-π interaction were revealed by the molecular docking studies, especially hydrogen bonding, accounting for the observed selective chiral recognition capacity of racemic 1–phenylethanol of NH 2 -MIL-101(Cr) ⊂ BSA. Moreover, both of NH 2 -MIL-101(Cr) ⊂ BSA and NH 2 -MIL-101(Cr) ⊂ Glu ⊂ BSA showed excellent stability and reusability. This combination of theory and experiment provided a clearer basis for other researchers to have different requirements for protein immobilization, and provided new ideas and methods for the development of chiral selectors.
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