RSC Advances
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2019
·Vol. 9
·期 57
·33238-33245
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IF 3.049
Zhi Li,Guangbo Che,Wei Jiang,Lihui Liu,Hairui Wang
In the present study, a novel photocatalyst, CQDs@MIL-125(Ti) (CQDs = carbon quantum dots), was prepared via a solvothermal procedure. The photocatalytic properties were tested by the degradation of tetracycline (TC) with a 250 W Xe lamp (λ > 420 nm). Compared with pure MIL-125(Ti), the 10 wt% CQDs@MIL-125(Ti) photocatalyst can significantly improve the degradation process of TC, and the degradation efficiency can reach 90% within 4 h. The enhancement in the photocatalytic performance is due to the CQDs, which can promote the absorption of visible light and also efficiently accelerate the separation of photogenerated electron–hole pairs. We have also demonstrated that superoxide radicals (·O2−) and holes (h+) play crucial roles in the photocatalytic degradation of TC through capture experiments. The current work provides a new idea for constructing high-efficiency photocatalysts based on MIL-125(Ti).
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MOLECULES
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2018
·Vol. 23
·期 7
·1524
·
IF 3.098
Xue-Xue Liang,Nan Wang,You-Le Qu,Li-Ye Yang,Yang-Guang Wang,Xiao-Kun Ouyang
In this study, novel composite titanium-based metal-organic framework (MOF) beads were synthesized from titanium based metal organic framework MIL-125 and chitosan (CS) and used to remove Pb(II) from wastewater. The MIL-125-CS beads were prepared by combining the titanium-based MIL-125 MOF and chitosan using a template-free solvothermal approach under ambient conditions. The surface and elemental properties of these beads were analyzed using scanning electron microscopy, Fourier transform infrared and X-ray photoelectron spectroscopies, as well as thermal gravimetric analysis. Moreover, a series of experiments designed to determine the influences of factors such as initial Pb(II) concentration, pH, reaction time and adsorption temperature was conducted. Notably, it was found that the adsorption of Pb(II) onto the MIL-125-CS beads reached equilibrium in 180 min to a level of 407.50 mg/g at ambient temperature. In addition, kinetic and equilibrium experiments provided data that were fit to the Langmuir isotherm model and pseudo-second-order kinetics. Furthermore, reusability tests showed that MIL-125-CS retained 85% of its Pb(II)-removal capacity after five reuse cycles. All in all, we believe that the developed MIL-125-CS beads are a promising adsorbent material for the remediation of environmental water polluted by heavy metal ions.Keywords:metal-organic framework;chitosan beads;adsorption;Pb(II)
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2019
·
IF 6.361
Haibo Zhang,Jia Wen,Ying Fang,Siyu Zhang,Guangming Zeng
Hypothesis Modification of MIL-100(Fe) with ethanediamine (ED) is expected to improve the removal percentage of Pb(II) ions from aqueous solution. Nevertheless, the adsorption performance of ED-MIL-100(Fe) in natural waters will be affected by natural organic matter such as fulvic acids (FA). Hence, it is necessary to study the influence of FA on the physicochemical property, adsorption behavior and mechanisms of ED-MIL-100(Fe) towards the removal of Pb(II) from water. Experiments Batch adsorption experiments were conducted to compare adsorption capacity of MIL-100(Fe) and ED-MIL-100(Fe) for Pb(II). In addition, XRD , FTIR, SEM and XPS techniques were applied to investigate the characteristics, adsorption isotherms , and kinetics in the presence and absence of FA. Findings ED-MIL-100(Fe) enabled 99% removal of Pb(II) from water at or below 60 mg L −1 , whereas the MIL-100(Fe) hardly adsorbed any Pb(II). Additionally, the adsorption percentage of the Pb(II) ions (76%) outcompeted that of other metal ions (i.e. Co, Cu, Ni, Zn, and Cd) (each ≤ 25%) in the mixed solution. The negative surface charge of ED-MIL-100(Fe) was not affected by FA. Increasing FA concentration steadily increased the functional groups surrounding the ED-MIL-100(Fe) via electrical interaction, thus facilitating the Pb(II) ions adsorption.
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Journal of the Taiwan Institute of Chemical Engineers
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2015
·
IF 3
Zhongwei
Jiang,Yuanfang Li
Integration of other functional materials onto the surface or into the matrixes of metal-organic frameworks (MOFs) is an attractive and effective approach to fabricate multifunctional MOFs. Herein, we report a facile and novel strategy for in situ synthesis of magnetic hybrid Fe 3 O 4 /MIL-101 via heterogeneous coprecipitation assembly. Characterizations showed that the Fe 3 O 4 nanoparticles were uniformly coated on the outer-surface of MIL-101. The as-synthesized Fe 3 O 4 /MIL-101 composite holds larger BET surfaces area, pore volume and higher positive charge than MIL-101. These preferable properties make it to be an excellent candidate for adsorption and removal of anionic dye from aqueous solution. The present work provides a new insight for in situ synthesis of Fe 3 O 4 -functionalized MOFs, offering an alternative way to prepare magnetic hybrid materials for a wide range of applications.
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ANALYTICAL CHEMISTRY
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2013
·
IF 5.695
Cheng-Xiong Yang,Hu-Bo Ren,Xiu-Ping Yan
Fluorescent metal–organic frameworks (MOFs) have received great attention in sensing application. Here, we report the exploration of fluorescent MIL-53(Al) for highly selective and sensitive detection of Fe3+ in aqueous solution. The cation exchange between Fe3+ and the framework metal ion Al3+ in MIL-53(Al) led to the quenching of the fluorescence of MIL-53(Al) due to the transformation of strong-fluorescent MIL-53(Al) to weak-fluorescent MIL-53(Fe), allowing highly selective and sensitive detection of Fe3+ in aqueous solution with a linear range of 3–200 μM and a detection limit of 0.9 μM. No interferences from 0.8 M Na+; 0.35 M K+; 11 mM Cu2+; 10 mM Ni2+; 6 mM Ca2+, Pb2+, and Al3+; 5.5 mM Mn2+; 5 mM Co2+ and Cr3+; 4 mM Hg2+, Cd2+, Zn2+, and Mg2+; 3 mM Fe2+; 0.8 M Cl–; 60 mM NO2– and NO3–; 10 mM HPO42–, H2PO4–, SO32–, SO42–, and HCOO–; 8 mM CO32–, HCO3–, and C2O42–; and 5 mM CH3COO– were found for the detection of 150 μM Fe3+. The possible mechanism for the quenching effect of Fe3+ on the fluorescence of MIL-53(Al) was elucidated by inductively coupled plasma-mass spectrometry, X-ray diffraction spectrometry, and Fourier transform infrared spectrometry. The specific cation exchange behavior between Fe3+ and the framework Al3+ along with the excellent stability of MIL-53(Al) allows highly selective and sensitive detection of Fe3+ in aqueous solution. The developed method was applied to the determination of Fe3+ in human urine samples with the quantitative spike recoveries from 98.2% to 106.2%.
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SEPARATION AND PURIFICATION TECHNOLOGY
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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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DALTON TRANSACTIONS
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2017
·Vol. 46
·期 44
·15512-15519
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IF 4.029
Lili Yao,Wenxiu Yang,Huiling Liu,Jianbo Jia,Guohua Wu,Dan Liu,Ting Liu,Taixing Tan,Cheng Wang
The design of efficient mixed Mn–Co oxides as oxygen reduction reaction (ORR) electrocatalysts in alkaline media has been boosted nowadays. Recently, multivariant MOFs have been demonstrated as versatile precursors to construct these mixed metal oxides. Herein, we synthesized four mixed Mn–Co oxide samples via simply annealing their MIL-53 precursors with different Co/Mn molar ratios. These four samples were dominated by three kinds of Mn–Co spinel phases. The mixed Mn–Co oxides showed enhanced ORR performances compared with the single metal counterparts in alkaline media. In particular, the sample containing a pure MnCo2O4 phase exhibited the highest activity with a half-wave potential of 0.772 V (vs. RHE), only 40 mV negative compared with that of commercial Pt/C. The H2O2 yield was calculated to be below 12.1%, corresponding to the high diffusion-limited current density along with the high electron transfer number. The surface defects, active Mn4+/Mn3+ and electrochemically active surface area together affected the ORR performances of these mixed Mn–Co oxides. The present work highlights the facile controllability of divalent MIL-53 analogues for highly efficient mixed Mn–Co oxides in ORR electrocatalysis.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2016
·
IF 8.328
Yanghe Fu,Long Sun,Huan Yang,Lai Xu,Fumin Zhang,Weidong Zhu
The Ni-doped NH 2 -MIL-125(Ti) catalyst was developed for the photocatalytic aerobic oxidation of aromatic alcohols upon visible light irradiation. The results show that different aromatic alcohols can be effectively transformed to their corresponding aldehydes with almost absolute selectivity using O 2 as the oxidant over Ni-doped NH 2 -MIL-125(Ti) upon visible light irradiation. Compared with the parent catalyst NH 2 -MIL-125(Ti), Ni-doped NH 2 -MIL-125(Ti) exhibits a significantly enhanced photocatalytic activity for the selective oxidation of aromatic alcohols. Preliminary studies indicate that the doping of Ni nanoparticles into NH 2 -MIL-125(Ti) could improve the visible-light harvesting, charge-separation, and electron-transport of the resultant catalyst, leading to the enhanced photocatalytic activity. The current work provides some guidance in the development of MOF-based photocatalysts for organic syntheses.
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Journal of Materials Chemistry C
·
2017
·Vol. 5
·期 36
·9465-9471
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IF 5.256
Ting Lu,Hongjie Song,Xiaoqun Dong,Jianyu Hu,Yi Lv
NH2-MIL-53(Al) nanorods studded with F− were successfully synthesized via coordination modulation with HF as a modulator. The investigation of the growth mechanism pointed out that F− plays a key role in the formation process. The incorporation of F− into the framework of NH2-MIL-53(Al) not only made the crystal morphology tunable but also magnified the fluorescence enhancement performance of NH2-MIL-53(Al) in water vapor, based on which a highly efficient humidity sensor was fabricated. Among different kinds of humidity sensors, the present sensing system stood out due to its fast response rate, good sensitivity and high selectivity with a low detection limit of 0.6 μg mL−1 (S/N = 3) and a wide detection range from 4 to 40 μg mL−1. On the other hand, a majority of the conventional electronic humidity sensors seriously suffered from temperature dependence, while the present sensing system got over this disadvantage. Therefore, the NH2-MIL-53(Al) nanorod layer-based fluorescence sensing system has the potential for application in the real-time monitoring of humidity under ambient conditions.
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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
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2016
·Vol. 183
·期 12
·3151-3157
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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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