JOURNAL OF APPLIED POLYMER SCIENCE
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2025
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IF 2.8
Ke Liu,Qisong Liu,Rui Fan,Hongfa Huang,Hua Yi,Chao Hu
Mixed matrix membranes (MMMs) incorporating metal–organic frameworks (MOFs) as fillers show attractive selectivity and permeability for gas separation. However, the performance improvement is restricted by undesirable interfacial interaction and inhomogeneous dispersion of MOFs in the membrane matrix. In this paper, amino-functionalized UIO-66 (U6N) with high porosity was employed as a filler and further regulated by a controlled plant polyphenol-induced surface modification strategy. The process involved the formation of tannic acid-iron(III) complex (TA-Fe(III)) on the U6N surface, which improved interfacial compatibility with the polyimide matrix while introducing abundant hydroxyl groups to enhance gas transport properties. Accordingly, the modified MMMs containing 30 wt.% U6N@TA-Fe(III) achieved optimized gas separation performance. Specifically, the CO 2 permeability increased to about 2495.9 Barrer with a CO 2 /CH 4 selectivity of 19.32, which exceeded the 2008 Robeson upper limit and showed an increase of 22.1% and 25.6%, respectively, compared to the MMMs embedded with unmodified U6N. Moreover, the improved dispersion of the U6N@TA-Fe(III) within the membrane structure is conducive to improving separation performance for CO 2 /N 2 and O 2 /N 2 . Therefore, this work provides a novel insight into the rational design of the MMMs via a facile modification strategy, which can further improve the gas separation performance of the MMMs.
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ACS Applied Polymer Materials
·
2024
·
IF 4.4
Zhaojie Wang,Qinglong Liu,Xinle Sun,Caifeng Xia,Qikang Yin,Maohuai Wang,Xiaodong Chen,Huili Zhang,Shuxian Wei,Xiaoqing Lu,Siyuan Liu
MOFs-filled mixed matrix membranes (MMMs) have great potential to break the trade-off effects of traditional gas separation membranes. However, achieving good interfacial compatibility and adequate dispersion of the MOF is not straightforward. In this study, a continuous postmodification was developed for advanced CO2/N2 MMMs. UiO-66-NH2 was easily modified with trimesoyl chloride (UiO-66-TMC) and polyethylene glycol (UiO-66-PEG) sequentially, which was utilized as fillers to construct polyimide (PI) mixed matrix membranes (MMMs). Rich interactions between modified UiO-66-NH2 and the PI polymer contribute to efficient CO2 and N2 separation. At 25 °C and 0.1 MPa, UiO-66-TMC/PI MMMs showed a CO2/N2 selectivity of 55.3, and a CO2 permeability of 616.17 Barrer, and those are 56.7 and 686 Barrer for UiO-66-PEG200/PI MMMs. Both of their CO2/N2 separation performances exceed the 2008 Robeson upper bound. The ether bonds in PEG exhibit strong interactions with the CO2 molecules and improve the CO2 dissolution selectivity. Meanwhile, the introduction of organic ingredients realized good dispersion and interfacial compatibility within the PI matrix. This work lays the groundwork for the further fabrication of highly selective CO2 separation materials with specific microscopic interface structures and properties.
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高影响因子
Journal of Water Process Engineering
·
2024
·
IF 6.3
Nan Zhao,Kangjie Zhang,Yuexiang Lu,Shuang Liu,Zhe Wang,Xiangke Wang
The photocatalytic method has been proven as one of the effective methods for uranium removal from radioactive wastewater. Herein, a photocatalyst UiO-66-NH 2 -Pt was prepared using the adsorption-photoinduction method. Pt was first adsorbed on the substrate and then photo-reduced under light irradiation to be doped into the structure of UiO-66-NH 2 . The characterization results implied the formation and atomic dispersion of Pt with a loading content of 1.90 wt%. The loading of Pt has promoted the effective separation and transfer of photogenerated electron-hole pairs, broadened the visible light adsorption range and narrowed down the bandgap, thus to enhance the photocatalytic activity. Then they were applied for the photo-removal of uranium under air atmosphere. The reaction rate of UiO-66-NH 2 -Pt was about 7 times that of pure UiO-66, confirming the higher photocatalytic activity after the loading of Pt. It showed good reusability and was also universal for different water matrix. The detection of hydroxyl radicals with EPR method indicated the formation of H 2 O 2 , which could react with uranyl ions to form metastudtite under air. This work further verified the feasibility of photoinduced synthesis of Pt single atom and provided a novel material for photocatalytic removal of uranyl ion under air.
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ANALYTICAL CHEMISTRY
·
2022
·
IF 8.008
Jiali Liu,Xianbiao Wang,Yangyang Zhao,Yongfei Xu,Yang Pan,Shaojie Feng,Jin Liu,Xianhuai Huang,Huanting Wang
Radioactive U(VI) in nuclear wastewater is a global environmental pollutant that poses a great threat to human health. Therefore, it is of great significance to develop a U(VI) sensor with desirable sensitivity and selectivity. Inspired by electron-donating group modification for enhancement of binding affinity toward U(VI), we report an amine group functionalization of UiO-66-NH2, using a low-cost, environmentally friendly, and low-temperature NH3 plasma technique as a fluorescence switching nanoprobe for highly sensitive and selective detection of U(VI). The resulting amine-functionalized UiO-66-NH2 (LTP@UiO-66-NH2) shows dramatically enhanced fluorescence emission and selective sensitivity for U(VI) on the basis of the quenching effect. The quenching efficiency increases from 58 to 80% with the same U(VI) concentration (17.63 μM) after NH3 plasma functionalization. As a result, the LTP@UiO-66-NH2 has the best Ksv (1.81 × 105 M–1, 298 K) and among the lowest LODs (0.08 μM, 19.04 ppb) compared with those reported in the literature. Intraday and interday precision and application in real environment experiments indicate stable and accurate U(VI) detection performance. Fluorescence lifetime and temperature-dependent detection experiments reveal that the quenching mechanism belongs to the static quenching interaction. The highly selective fluorescence detection is attributed to the selective binding of U(VI) by the rich functionalized amine groups of LTP@UiO-66-NH2. This work provides an efficient fluorescence probe for highly sensitive U(VI) detection in water, and a new strategy of tailored plasma functionalization for developing a practical MOF sensor platform for enhanced fluorescence emission, sensitivity, and selectivity for detecting trace amounts of radioactive species in the environment.
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Environmental Science-Nano
·
2018
·Vol. 5
·期 6
·1441-1453
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IF 6.087
Jingmiao Wei,Wei Zhang,Weiyi Pan,Chaoran Li,Weiling Sun
Adsorption behaviors and mechanisms of selenite [Se(IV)] and selenate [Se(VI)] on two types of zirconium metal–organic frameworks (MOFs, UiO-66 and UiO-66-NH2) were investigated using batch experiments, spectroscopic analyses, and theoretical calculations. Se(IV) adsorption was substantially greater than Se(VI) adsorption. Intriguingly, with increasing solution pH, Se(IV) adsorption increased to a maximum at pH 7, whereas Se(VI) adsorption monotonically decreased. Se(IV) adsorption was not influenced by coexisting ions except for PO43−, whereas Se(VI) adsorption was in general decreased with increasing coexisting ion concentrations. The underlying molecular binding mechanisms were elucidated via zeta potential, XPS, and FTIR analyses as well as density functional theory calculations. Se(IV) formed a strong inner-sphere complex with the MOFs via Lewis acid/base complexation between the Zr coordinatively unsaturated sites and HSeO3− or SeO32− (−59.4 to −142 kJ mol−1) and hydrogen bonding between Zr–O–C and H2SeO3 (−24.4 to −29.8 kJ mol−1). Se(VI) formed outer-sphere complexes with the MOFs through electrostatic interactions (−50.6 to −62.1 kJ mol−1). Thus, the BET surface area was the predominant factor determining the Se(IV) adsorption, whereas both the surface charge and BET surface area controlled the Se(VI) adsorption. This study provided new insights on the molecular interactions between Se(IV) and the MOFs, and revealed the distinct differences between the Se(IV) and Se(VI) adsorptions.
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CRYSTENGCOMM
·
2021
·Vol. 23
·期 25
·4549-4559
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IF 3.545
Zongjian Liu,Zhicong Sun,Lin Zhang,Lifei Xu,Xinyue Lu,Qun Cui,Haiyan Wang
Hierarchical nanocrystal UiO-66 was synthesized by a template-free double solvent-modulated crystallization method. The influences of the ammonium hydroxide (NH4OH)/Zr and acetic acid (HAC)/Zr ratios and pH of reaction solution on the morphological and the porous properties of UiO-66 were investigated. The results show that the nanoscale grains of UiO-66 with the size of ∼20 nm and interparticle mesopores of ∼30 nm are obtained with the NH4OH/Zr of 0.96–3.84, HAC/Zr of 50 and the pH from 1.68 to 2.70. The introduction of NH4OH is favorable to the formation of Zr4+ oxo/hydroxo clusters and deprotonation of the ligands for accelerating the nucleation and crystallization, while HAC can effectively control the hydrolysis of zirconium chloride to avoid the formation of particles with low crystallinity. The equilibrium adsorption capacities of nHEP and MCH on UiO-66(2.88, 50) are higher than that on UiO-66-AS at 323–373 K, respectively. The effective diffusion coefficients of n-heptane/methyl cyclohexane on the hierarchical UiO-66 nanocrystals are about 5 and 18 times higher than that on microporous UiO-66 at 373 K and 0.05–6 kPa, respectively. The introduction of mesopores increases the adsorption performance of the adsorbent for alkanes and enhances mass transfer.
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JOURNAL OF HAZARDOUS MATERIALS
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2020
·
IF 9.038
Pei Jia,Kairong Yang,Jinjie Hou,Yuanyuan Cao,Xin Wang,Li Wang
The increasing deterioration of ecosystem derived from heavy metals residues brings about the environmental and food contamination , which presses the exploration of facile platform for monitoring heavy metals. Herein, a ratiometric fluorescence sensor was designed for Hg 2+ detection based on the compound of UiO-66-NH 2 and Ru(bpy) 3 2+ (Ru@UiO-66-NH 2 ) which was synthesized by situ encapsulation. The innovative composite displayed two emission peaks at 437 and 604 nm, and the addition of Hg 2+ could only quench the blue fluorescence due to static quenching and photo-induced electron transfer mechanism, providing an internal standard to promote the precision. Under optimal conditions, the ratiometric Ru@UiO-66-NH 2 probe revealed outstanding anti-interference capability and performed with a great limit of detection (LOD) of 0.053 μM for Hg 2+ , which was 2-fold lower than that of single-color UiO-66-NH 2 . By merit of Ru@UiO-66-NH 2 , test hydrogels were fabricated to provide a tactics for visual, rapid and on-site detection of Hg 2+ . Additionally, the dual-emitting sensing platform presented satisfactory recoveries and reliabilities in lake water, tap water , and drink water, demonstrating the application potential of this proposed ratiometric fluorescence sensor for monitoring Hg 2+ .
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CHINESE JOURNAL OF CATALYSIS
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2025
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IF 17.7
Rushuo Li,Tao Ban,Danfeng Zhao,Fajie Hu,Jing Lin,Xiubing Huang,Zhiping Tao,Ge Wang
Defect engineering improves the catalytic performance of metal-organic frameworks (MOFs) loaded metal nanoparticles (MNPs@MOFs), but there is still a challenge in defining the structure-activity relationships. Herein, the content of linker-missing defects in UiO-66(Ce) was systematically regulated via formic acid as the modulators, and defective UiO-66(Ce) loaded Ni nanoparticles (NPs) were constructed for dicyclopentadiene (DCPD) hydrogenation. The fine regulation of defect engineering and reduction conditions affected the structure properties of UiO-66(Ce) and the electronic metal-support interaction between MOFs and Ni NPs, thereby optimizing the microenvironment and electronic state of Ni NPs. The optimized U(Ce)-40eq with suitable defects, small size and structure stability effectively promoted the production of highly dispersed abundant electron-deficient Ni 0 active sites, enhancing the adsorption and activation of H 2 and C=C bonds, especially accelerating the rate-determining step. Therefore, U(Ce)-40eq loaded 5 wt% Ni NPs achieved DCPD saturated hydrogenation to tetrahydrodicyclopentadiene (70 °C, 2 MPa, 90 min), superior to most high-loading Ni-based catalysts. This work reveals the synergistic mechanism of MOFs defect engineering and electronic structure of Ni NPs, providing effective guidance for the precise preparation of highly efficient and stable MNPs@MOFs heterogeneous catalysts.
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JOURNAL OF CHROMATOGRAPHY A
·
2014
·
IF 4.258
Hai-Bo Shang,Cheng-Xiong Yang,Xiu-Ping Yan
Effective solid-phase microextraction (SPME) of polar phenols from water samples is usually difficult due to the strong interaction between polar phenols and aqueous matrix. Here, we report the fabrication of a metal–organic framework UiO-66 coated stainless steel fiber via physical adhesion for the SPME of polar phenols (phenol, o -cresol, p -cresol, 2,6-dimethylphenol, 2,4-dichlorophenol and 2,6-dichlorophenol) in water samples before gas chromatographic separation with flame ionic detection. Headspace SPME of 10 mL sample solution with the fabricated UiO-66 coated fiber gave the enhancement factors of 160 (phenol) – 3769 (2,4-dichlorophenol), and the linear ranges of 1–1000 μg L −1 (2,6-dimethylphenol, 2,4-dichlorophenol and 2,6-dichlorophenol), 1–500 μg L −1 ( o -cresol and p -cresol) and 5–500 μg L −1 (phenol). The detection limits ranged from 0.11 μg L −1 (2,6-dimethylphenol) to 1.23 μg L −1 (phenol). The precision (relative standard deviations, RSDs) for six replicate determinations of the analytes at 100 μg L −1 using a single UiO-66 coated fiber ranged from 2.8% to 6.2%. The fiber-to-fiber reproducibility (RSDs) for three parallel UiO-66 coated fibers varied from 5.9% to 10%. The recoveries obtained by spiking 5 μg L −1 of the phenols in the water samples ranged from 80% to 115%.
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PubMed
高影响因子
MICROCHEMICAL JOURNAL
·
2025
·
IF 5.1
Yalong Cheng,Juan Qiao,Shidi Zhang,Li Qi
Metal-organic frameworks (MOFs) have attracted extensively interests for enzyme immobilization. However, their rigid structures remain a great challenge in improvement the catalytic performance of the carriers due to no nanoconfinement. Herein, carriers based on rigid UiO-66-NH 2 (U) modified with soft smart polymer were designed by surface engineering. A thermo-responsive polymer, poly(N-isopropylacrylamide) (PNP), was synthesized through an in-situ polymerization strategy, which was employed as a “soft tent” on the surface of rigid U. Glucose oxidase (GOx)-horseradish peroxidase (HRP) was chemically bonded on PNP-U using glutaraldehyde as a linker. Benefiting from the nanoconfinement via variation temperatures, PNP-U@GOx-HRP carriers exhibited 2.01-fold catalytic activity ( K cat value) at 37 °C higher than that at 25 °C. Furthermore, a colorimetric method for analysis of glucose in grape samples was developed. This study offers a strategy for construction of “soft tent” smart polymer-MOFs@enzyme carriers, which provides a pivotal nanoconfinement for boosting their catalytic performance, and broadens their applications in bio-molecules sensing.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Yulan Zheng,Peng Cheng,Zikuo Li,Chuhao Fan,Jinchao Wen,Yue Yu,Li Jia
To achieve the efficient removal of gaseous elemental mercury in coal-fired flue gas, the study successfully prepared the isostructural bimetallic MOFs-based biochar composite by introducing the transition metal Fe into the UiO-66 by solvothermal method and using in-situ growth method for structural design. In addition, the effect of doping the secondary metal Fe and biochar on the Hg 0 removal performance and the corresponding quantitative correlation mechanism was established. The results showed that the overall mercury removal performance of the samples after Fe modification was improved. The optimal Fe loading ratio was 10 %, which corresponded to the adsorption capacity of 127.65 μg·g −1 . The biochar promoted the electron transmission and transfer of the overall reaction system by exerting the carrier effect. The 10 %Fe-UiO-66@20 %BC composite showed the best Hg 0 removal performance, with the corresponding adsorption capacity of 150.74 μg·g −1 . Fe 3+ , lattice oxygen, and chemisorbed oxygen jointly participated in the oxidation process of Hg 0 and finally oxidized Hg 0 to HgO.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
·
IF 16.683
Fukun Bi,Xiaodong Zhang,Jinfeng Chen,Yang Yang,Yuxin Wang
The highly dispersed Pd nanoparticles supported UiO-66 catalysts were successfully prepared via ethylene glycol reduction method (Pd-U-EG). And their catalytic performances were evaluated by toluene degradation. A series of characterization methods were carried out to characterize the physicochemical properties of the samples. During the effect of high weight hourly space velocity, stability and reusability test, the catalytic activity of Pd-U-EG remains unchanged, which also indicated good catalytic performance. More importantly, water resistance test (10-20 vol.% water) indicated that Pd-U-EG had a great water resistance. The study of toluene-TPD, toluene-TPSR and in-situ DRIFTS at different temperatures under different conditions over Pd-U-EG indicated the role of H 2 O. The introduction of H 2 O at low temperature was conducive to the adsorption of toluene, but inhibited the degradation of toluene. Differently, the H 2 O presence at high temperature was favorable to toluene degradation. In addition, toluene degradation mechanism was also revealed.
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