APPLIED SURFACE SCIENCE
·
2015
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IF 2.711
Jian-Jian Zhou,Rong Wang,Xin-Ling Liu,Fu-Min Peng,Chuan-Hao Li,Fei Teng,Yu-Peng Yuan
CdS nanoparticles acting as photosensitizer was grown in situ upon UiO-66 metal-organic framework octahedrons through a hydrothermal process. The resultant CdS/UiO-66 hybrid photocatalysts show remarkably active hydrogen evolution under visible light irradiation as compared to CdS and UiO-66 alone. The optimum hybrid with 16 wt% CdS loading shows a hydrogen production rate of 235 μmol h −1 , corresponding to 1.2% quantum efficiency at 420 nm. The improved photocatalytic hydrogen production over hybrid CdS/UiO-66 is ascribed to the efficient interfacial charge transfer from CdS to UiO-66, which effectively suppresses the recombination of photogenerated electron-hole pairs and thereby enhancing the photocatalytic efficiency.
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INTERNATIONAL JOURNAL OF HEAT AND MASS TRANSFER
·
2024
·
IF 5
Yue Liu,Yan Ma,Wenjing Chen,Xiaowu Hu,Xiongxin Jiang
Modification of metal-organic frameworks (MOFs) with different functional groups can effectively improve the loading ratio of phase change materials (PCMs) as well as the thermal properties of composite phase change material (CPCM). However, the interaction mechanism between functional groups and PCMs is still unclear. Herein, molecular dynamics (MD) simulations and experimental tools were used to study the interaction mechanism between integrating amino-functionalized and unfunctionalized UiO-66-NH 2 , UiO-66 (UiO-66: Zirconium-centred MOF) and stearic acid (SA). The incorporation of amino groups enhanced the phonon vibrational coupling between UiO-66-NH 2 and SA, as well as the number of hydrogen bonds. Thermal resistance between PCM and the carrier was effectively reduced, exhibiting a 42.46% decrease compared to UiO-66, because the amino functional group can increase the number of hydrogen bonds between UiO-66 and SA, thereby increasing the overall thermal conductivity. From the experimental results in this paper, the amino-modified UiO-66-NH 2 can load more SA, and therefore the enthalpy is also well enhanced, with a maximum melting enthalpy of 71.3 J/g, and no leakage during the phase transition. The findings of the experimental study are in alignment with the results of the molecular dynamics simulations. In addition, the results of the thermal management experiment demonstrate that the CPCMs consisting of UiO-66-NH 2 and SA can effectively regulate the heating rate of the heating element. In conclusion, the present study offers novel experimental and MD simulation insights that may inform the future design of MOF-based CPCMs modified with diverse surface functional groups.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2025
·Vol. 172
·期 3
·036503
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IF 3.3
Xiaoyan Wang,Hao Zheng,Huiling Chen,Bin Qiu,Yunliang Liu,Qing Ye
Interleukin-6 (IL-6) is a common proinflammatory cytokine and can be adopted as an important biomarker for several diseases including nasopharynx cancer, pancreatitis, infections, and cardiovascular. It is thus necessary to design an effective method for monitoring IL-6. Herein, by preparing gold nanoparticles/graphdiyne (Au/GRD) nanohybrid with simple electroless deposition as the sensing substrate and UiO-66 metal–organic frameworks/ferrocene (UiO/Fc) as the signaling-amplifier, a highly efficient sandwich-type electrochemical immunosensing (SEI) platform was proposed for IL-6 determination. The superior electrical properties, easy preparation, high surface area, and stability of Au/GRD make it a desirable substrate to immobilize the primary antibody of IL-6. Meanwhile, the unique structure of UiO-66 is beneficial to immobilizing the Fc probe and the secondary antibody. By optimizing experimental conditions, the Fc current obtained at the as-designed SEI platform increases along with IL-6 increase, and the related linearity is 0.5 pg ml−1–1200.0 pg ml−1 coupled with a low detection limit of 0.2 pg ml−1. It is expected the as-designed SEI platform based on Au/GRD and UiO/Fc shows potential applications for IL-6 analysis.
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REACTIVE & FUNCTIONAL POLYMERS
·
2025
·
IF 5.1
Yipeng Zhang,Yani Wang,Kewei Wang,Xiaopeng Xiong
The persistent presence of antibiotic contaminants, such as fluoroquinolones (FQs), in aquatic environments poses significant environmental risks. In this study, a porous poly(glycidyl methacrylate) (PPGMA) microsphere adsorbent was designed for the efficient removal of FQs. Acrylate monomers were dispersed in water to prepare an oil-in-water high internal phase emulsion, which was subsequently subjected to ultraviolet (UV) irradiation for 3 min to prepare the microsphere with high yield. To template the porous structure, cyclohexane, a poor solvent for the polymer, was introduced into the initial monomer oil phase, and its influence on the evolution of porous morphology was systematically investigated. Thereafter, the porous microsphere was modified through grafting with polyethyleneimine to facilitate the in-situ growth of a metal-organic framework, UiO-66-NH 2 . The modification progress was monitored, and the final UiO@PPGMA microspheres were comprehensively characterized. Based on adsorption kinetics and thermodynamics, the microsphere containing only 2.78 % UiO-66-NH 2 exhibits significantly enhanced adsorption rate and capacity, which can be attributed to the in-situ grown UiO-66-NH 2 nanoparticles. Furthermore, the UiO@PPGMA microsphere can be easily regenerated, allowing it to be packed in a column for cyclic fixed-bed adsorption. Consequently, our results demonstrate a facile strategy for preparing porous microsphere adsorbents, which may have promising applications in the removal of antibiotic contaminants from water sources.
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Journal of Materials Chemistry A
·
2024
·Vol. 12
·期 37
·25465-25474
·
IF 10.7
Yalin Niu,Peng Jiang,Tianying Guo
Developing high-performance artificial enzyme materials with practical applications in efficient catalytic hydrolysis detoxification of organophosphate (OP) nerve agents remains a formidable challenge. Herein, UiO-66-NH2-stabilized Pickering high internal phase molecularly imprinted polymer systems (MOFs@PHIPMIPs) were developed using OPs as template molecules. Thus, UiO-66-NH2-doped high-internal-phase MIP composites were obtained, which integrate MIPs and MOFs successfully, showing remarkable catalytic hydrolysis activity towards OPs. In addition, by introducing methyl methacrylate (MMA) during copolymerization, the MOFs@PHIPMIPs would effectively acquire pH buffering properties. The multi-porous composite catalysis system exhibits an exceptionally high detoxification efficiency towards dimethyl-4-nitrophenyl phosphate (DMNP) in pure water (kobs = 0.9162 min−1, t1/2 = 0.76 min). This work presents a new strategy for the preparation of artificial phosphatase materials with high-performance catalytic detoxification of OPs with great application prospects.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2024
·
IF 7.7
Xin Yuan,Jia-Hui Liao,Gui-Jia Du,Yi Hou,Song-Qing Hu
Kinsenoside is a rare and valuable glycoside with extensive bioactivities. However, the enzymatic synthesis of kinsenoside has been a challenging task due to the limited enzyme toolbox and unsatisfactory yield. Herein, the β-glucosidase from Dictyoglomus thermophilum (DtBGL) was heterologously expressed, purified and enzymatically characterized. The purified DtBGL was successfully immobilized on the metal-organic frameworks of UiO-66-NH 2 . The DtBGL@UiO-66-NH 2 was fully characterized using SEM, XRD, TGA and FTIR. The studies on enzymatic properties demonstrated that DtBGL@UiO-66-NH 2 exhibited increased catalytic activity and stability compared to the free DtBGL. Particularly, DtBGL@UiO-66-NH 2 could catalyze the synthesis of kinsenoside via the reverse hydrolysis reaction and the kinsenoside yield was 34.12 % under the optimized catalytic system, which was 1.9-fold higher compared with the free DtBGL. Moreover, DtBGL@UiO-66-NH 2 displayed good reusability with a kinsenoside yield of 27.02 % after reuse for 3 times. The present work not only identifies and characterizes a highly active β-glucosidase with reverse hydrolysis activity, but also proposes the immobilized enzyme as an effective catalyst for the industrial production of glycosides.
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ACS Applied Polymer Materials
·
2024
·
IF 4.4
Kuirong Feng,Lingxin Meng,Jingmei Xu,Pengyun Zhao,Na Li,Jinxuan Lei
In this paper, UiO-66-NH2 was successfully modified with a phosphate group by a Schiff base reaction. The phosphate and amine bifunctionalized UiO-66-NH2 (PUIN) was successfully prepared. A series of composite membranes were prepared by adding PUIN fillers to sulfonated poly(aryl ether ketone sulfone) (FSPUIN-X) containing fluorene groups. The introduction of PUIN containing both phosphate and amino bifunctional groups increased the number of proton transport sites within the membrane and facilitated the construction of continuous proton transport channels. The addition of PUIN resulted in a significant increase in the proton conductivity of FSPUIN-X due to the introduction of more proton transport sites. The conductivity of FSPUIN-5 (174.22 mS cm–1) was 1.46 times higher than that of pure membranes (119.32 mS cm–1) at the same condition. And the open-circuit voltage and power density of FSPUIN-5 also reached 0.957 V and 0.54 W cm–2, respectively. The structure and morphology of PUIN and membranes were characterized by Fourier infrared (FT-IR), X-ray polycrystalline diffraction (XRD), nuclear magnetic resonance hydrogen spectrum (1H NMR), and scanning electron microscopy (SEM). Meanwhile, the PUIN also strengthened the mechanical properties of FSPUIN-X series membranes. All of the results indicated that the introduction of phosphate and amine bifunctionalized UiO-66-NH2 promoted the comprehensive performance of the composite membranes.
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Catalysis Science & Technology
·
2024
·
IF 4.4
Jianghui Lin,Jiamei Luo,Mengjia Zhang,Lei Zhang,Guohui Cai,Jiahua Zou,Ling Li
Incorporation of ionic liquids into metal–organic frameworks (MOFs) offers a new platform to construct heterogeneous bifunctional catalytic systems for the chemical capture and conversion of CO2 with epoxides. Herein, an imidazolium-based ionic liquid decorated UiO-66 type MOF (P3[BCMIm]Br@UiO-66) was successfully constructed via solvothermal assembly of the carboxyl-functionalized imidazolium ionic liquid ligand, terephthalic acid ligand and Zr(IV) ions. It exhibits the highest catalytic activity upon the cycloaddition of CO2 (98.2% conversion of propylene oxide and 99% selectivity to propylene carbonate) under optimized conditions (2.2 Mpa CO2, 1.0 wt%, 110 °C, reaction time 2 h). Notably, P3[BCMIm]Br@UiO-66 outperformed the original UiO-66 materials and [BCMIm]Br. P3[BCMIm]Br@UiO-66 retained its good catalytic performance for up to five recycling runs with only a little loss in catalytic activity. Furthermore, several additional coupling reactions were investigated with other epoxides as substrates.
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MICROCHEMICAL JOURNAL
·
2024
·
IF 4.9
Peixun Yang,Senwei Jiang,Zhen Wu,Daodong Pan,Hangzhen Lan
Metal-organic frameworks (MOFs) hold significant potential for sample preparation, but single-MOF materials often face limitations in selectivity and extraction efficiency. To overcome these, a mesoporous MIL-53(Al)–NH 2 @UiO-66 composites with a core–shell structure was synthesized using an epitaxial growth strategy. This composite leverages the complementary properties of both MOFs, offering enhanced active sites and interaction forces for analytes. The structure and integration of the composite were characterized using Fourier-transform infrared spectroscopy, scanning electron microscopy, and X-ray diffraction, confirming their successful integration. To address the challenge of detecting alkylphenols (APs) in food matrices, known for their endocrine-disrupting properties and low concentrations, a new solid-phase microextraction (SPME) Arrow was fabricated using the MIL-53(Al)–NH 2 @UiO-66 composite combined with polyacrylonitrile as a binder. APs were detected using ultra-performance liquid chromatography and quadrupole time-of-flight tandem mass spectrometry (UPLC-ESI-Q-ToF/MS). The developed SPME Arrow-UPLC-ESI-Q-ToF/MS method exhibits good linearity (R 2 ≥ 0.9958), wide linear range (0.01–1000 μg L –1 ), and high sensitivity (limits of detection ranging from 0.005 to 0.01 μg L –1 ) for APs determination. This method was validated for determining nine APs in milk samples from various packing materials, with spiked recoveries ranging from 85.2 % to 115 % and relative standard deviations from 3.4 % to 13.6 %. This study demonstrates the potential of MOF-on-MOF composites in enhancing the performance of adsorbents for SPME pretreatment, offering a promising approach for improving analytical methodologies in food safety.
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MICROCHEMICAL JOURNAL
·
2024
·
IF 4.9
Tianyu Wang,Yonghui Xia,Xuan Wan,Yafeng Zhang,Nayu Chen,Yuan Jin,Guangli Li
Improper and persistent use of marbofloxacin (MAR) is prone to produce residues that deteriorate the surrounding environment and endanger our health. Hence, it is urgent to stablish a facile and efficient detection technique for the detection of MAR . Herein, a highly efficient electrochemical platform was constructed for sensitive determination of MAR using zirconium-based metal–organic framework (UiO-66)/nitrogen-doped graphene (NG) nanocomposites (UiO-66/NG). The surface morphology, crystalline phase, elemental composition, and electrochemical behavior of UiO-66/NG were characterized by various spectroscopic and electrochemical techniques. Owing to the synergistic interaction of UiO-66 MOFs and NG nanosheets, the UiO-66/NG exhibited remarkable catalytic activity for MAR oxidation. As consequently, the UiO-66/NG demonstrated a wide linear response range (0.01 − 10 μM), high sensitivity (1.80 μM μA −1 cm −2 ) and low detection limit (0.002 μM). The proposed UiO-66/NG/GCE demonstrated robust voltammetric responses even in the presence of excess potential interfering species and retained stable response signals for at least two weeks. More importantly, the proposed UiO-66/NG/GCE displayed highly consistent sensitivity toward MAR detection in both aquaculture water and milk matrices and PBS buffer, and achieved accurate and sensitive detection of MAR with good recovery. Together with its low cost and facile operation, the UiO-66/NG/GCE shows great prospects for trace detection of MAR from complex matrices.
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Ming Fang,Zhenfei Yang,Yang Guo,Shuqin Yuan,Xinnian Xia,Shuaijun Pan
High-performance photocatalytic H 2 evolution materials require strong light absorption capability, excellent photogenerated charge separation ability and efficient charge carrier migration capability. In this study, we designed a piezoelectric photocatalytic heterojunction composed of UiO-66-NH 2 and ZnIn 2 S 4 nanosheets with sulfur vacancies. The Sv-UZ-45 heterojunction achieved piezoelectric photocatalytic H 2 evolution performance of 3886.4 μmol·g -1 ·h -1 , with a 4.6 times enhancement due to the synergistic effect of piezoelectric effect and defect engineering. The introduction of sulfur vacancies enables the heterojunction to obtain stronger light absorption, while the higher CB position of rich-sulfur vacancies ZnIn 2 S 4 is more favorable for the photocatalytic reduction reaction. In addition, the heterojunction with rich-sulfur vacancies exhibits a stronger piezoelectric effect than without vacancies, thus providing a powerful driving force for the separation of photogenerated charge carriers. Finally, ESR was used to explain the potential photocatalytic mechanism and showed that Sv-UZ-45 adheres to the Z-scheme carrier migration pathway. This work elucidates the synergistic interaction between piezoelectric effect and defect engineering, providing new insights for the further development of high-performance piezoelectric photocatalysts.
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Research
·
2025
·
IF 10.7
Yuening Wang,Xiangyu Meng,Wenxiong Shi,Yujiao Xie,Aochi Liu,Lei Xu,Lin Qiu,Xiaoyu Song,Mingjian Zhang,Jiahao Zhang,Jian Yu,Aiguo Wu,Xiaotian Wang,Jie Lin
Volatile organic compounds (VOCs) serve as critical biomarkers in exhaled breath for early-stage cancer patients, and their rapid, trace-level detection holds marked implications for cancer screening. Surface-enhanced Raman scattering (SERS) technology demonstrates strong potential for trace VOC gas detection due to its ultra-high sensitivity and immunity to water interference. However, while surface plasmon resonance (SPR)-free semiconductor substrates offer superior spectral stability and selectivity, their sensitivity toward VOC detection remains suboptimal. This study introduces a novel semiconductor-based SERS substrate composed of copper single atoms anchored on UiO-66 (Cu 1 /UiO-66), achieving a record-low detection limit of 10 parts per billion for VOC gases with a rapid 2-min response time, thereby elevating the gas-sensing performance of SPR-free substrates to unprecedented levels. The exceptional SERS activity originates from the highly delocalized electron properties of single-atomic copper, which effectively facilitates single-atom charge transfer processes. Concurrently, the incorporation of copper single atoms modulates the band structure of UiO-66, substantially enhancing the coupling resonance between the substrate and target molecules. In simulated breath tests mimicking lung cancer patients’ exhalations, Cu 1 /UiO-66 exhibits remarkable VOC recognition capability and robust anti-interference performance. This work pioneers a new paradigm for ultra-sensitive, rapid detection of trace VOCs in exhaled breath, holding substantial promise for early cancer diagnostics and clinical translation.
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