MICROCHEMICAL JOURNAL
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2024
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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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INTERNATIONAL JOURNAL OF HEAT AND MASS TRANSFER
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2024
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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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MICROCHEMICAL JOURNAL
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2024
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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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ACS Applied Nano Materials
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2024
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IF 5.3
Yahui Zhang,Xia Huang,Jiachang Chen,Jiyuan Li,Shen Zhou,Junying Chen
Quantitative analysis of harmful patina components on the surface of bronzeware is crucial as patina can corrode artifacts. Surface-enhanced Raman spectroscopy (SERS) has a common application in surface analysis. However, there exists an absence of documented investigations concerning the quantitative analysis of detrimental patina, particularly the chloride patina. To achieve high sensitivity in targeting harmful patina, we report a fabrication method for constructing Ag/Au alloys in the pores and on the surface of UiO-66 (zirconium 1,4-dicarboxybenzene metal–organic framework) nanomaterials, resulting in Ag/Au/UiO-66 nanoparticle monolayers formed by self-assembly at the oil–water interface. By incorporating them onto the surface of PVA hydrogel, we obtained SERS sensor devices with excellent flexibility, outstanding optical transparency, and ultrahigh activity. These sensor devices efficiently sample irregular surfaces and detect micrometer-scale specimen. They significantly enhance the Raman characteristic peaks of measured objects, facilitating precise analysis of the patina composition on the surface of bronze artifacts. The Raman peak at 118 cm–1 was boosted from 367 to 11,909 for detecting harmful patina, and the enhancement factor of the SERS substrate was calculated to be 3.6 ×1010 for detecting the Raman peak of rhodamine 6G (R6G), which could be easily detected at 610 cm–1 at a concentration of 10–13 mol/L (M). The Raman peaks at 610 cm–1 from the SERS substrate could also be readily detected. By grafting the organic fluorescent group amino-MQAE onto the surface of Ag/Au/UiO-66 nanoparticles (NPs), the content of harmful patina on the surface of bronze artifacts treated for different durations was indirectly determined. These results indicate the successful construction of the Ag/Au alloy on the surface of UiO-66 NPs, resulting in SERS sensor devices with excellent flexibility, optical transparency, and ultrahigh sensitivity.
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SENSORS AND ACTUATORS B-CHEMICAL
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2025
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IF 7.7
Shengqiao Gao,Qingyi Wei,Hongbin Pu
Heterojunction-like substrates have drawn significant attention in surface enhanced Raman spectroscopy (SERS) owing to their multi-enhancement characteristics. In this study, the core-shell architectures of UiO-66@ TiO 2 were fabricated for capture and enrichment of organophosphorus pesticides (OPs) in solution. After absorption of OPs, the SERS-active nanoparticles of Au were assembled on the core-shell architectures to form UiO-66@TiO₂/Au substrate via Au-S bonding between OPs molecule and AuNPs and electrostatic interactions between UiO-66@TiO 2 and Au, resulting in adsorption-induced aggregation of Raman signal for OPs. The proposed method of adsorption-induced aggregation could be used for detecting thiamethoxam and triazophos in apple juice with detection limit of 3.51 μg/L and 0.66 μg/L, respectively. Furthermore, the satisfactory recovery rates, ranging from 91.98 % to 104.31 % for thiamethoxam and from 91.47 % to 116.47 % for triazophos, indicated that the prepared heterojunction-like substrate could be potentially used for trace detecting OPs in foods.
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Research
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2025
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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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PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
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IF 3.9
Yiwen Gui,Ao Chen,Yiting Liu,Ning Cai,Jumei Li
A sensitive and stable substrate is crucial in Raman spectroscopic techniques for the effective detection of environmental contaminants. In this study, a novel core–shell composite, Ag@UiO-66, was developed by coating Ag nanospheres with a porous metal–organic framework (MOF), UiO-66-NH2. This composite combines high stability with selective enrichment capabilities for Cr(VI). Leveraging the unique properties of UiO-66-NH2, such as its porosity, abundant amine groups, and Zr nodes, Ag@UiO-66 effectively enriches Cr(VI) through pore-filling, electrostatic interactions, and Zr–O coordination. Direct analysis of water samples spiked with Cr(VI) showed detection limits of 6.53 × 10–8 M in pond water and 7.52 × 10–8 M in lake water. The composite also exhibited excellent signal uniformity and reproducibility, with a low relative standard deviation of 6.78% across 30 batches. Additionally, it demonstrated outstanding recyclability under simulated sunlight irradiation due to the solar photocatalytic properties of UiO-66-NH2. Ag@UiO-66 also showed superior stability compared to pristine Ag nanospheres when exposed to strong acids, bases, or oxidative environments (e.g., 1% H2O2 solution). Overall, Ag@UiO-66 shows great potential as a reliable substrate for the trace detection of chemical analytes via SERS.
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APPLIED SURFACE SCIENCE
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2024
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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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Journal of Cleaner Production
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2021
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IF 9.297
Peng Shi,Xingkang Hu,Ming Duan
The water-soluble pollutant including dye and heavy metal was a challenge to the water and environment. Adsorption was among one of the most promising technique for the recycle of dye but it usually required a long contact time. A membrane-like adsorbent was fabricated by mixing and depositing tannic acid, chitosan and metal organic framework (MOF, UIO-66) on polyethersulfone (PES) membrane in this study. The material was dense enough to conduct filtration like a membrane to remove both the anionic and cationic dye (acid brilliant scarlet and methylene blue), as well as Cr(VI) from water. When the ratio of MOF/Chitosan was 30% and the pH for mixing was 3.5, the pollutant removal reached 99% in the filtration for 200 min. The adsorbent in the dynamic filtration showed a pollutant loading capacity 3 times of the capacity in the static adsorption, which was caused by the enhanced driving force brought by the concentration polarization in the filtration. The particle size of the TA/CS/MOF mixture were characterized by dynamic light scattering as well as Zeta potential , FTIR, XRD , TEM and XPS . The morphology of membrane was observed by SEM. The result showed that the MOF played as core to disperse the tannic acid-chitosan mixture to improve the pollutant removal. TEM showed the TA/CS mixture formed an uniform coating outside the MOF particle at the pH of 3.5. The pseudo 1st order and pseudo 2nd order model fitted the adsorption kinetics well, while the Elovich model did not fit very well.
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ANALYTICA CHIMICA ACTA
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2020
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IF 5.977
Tianjiao Meng,Ningzhao Shang,Anaclet Nsabimana,Huimin Ye,Huan Wang,Chun Wang,Yufan Zhang
MicroRNA-21 (miR-21) has been widely investigated as important biomarkers for cancer diagnosis and treatment. Herein, a highly sensitive nonenzymatic electrochemical biosensor based on [email protected] frameworks ( [email protected] ) and target-catalytic hairpin assembly (CHA) with target recycling approach has been proposed for the detection of miR-21. The proposed biosensor integrates the efficient CHA strategy and excellent electrocatalytic performance of [email protected] nanocomposites. The concentration of miRNA-21 is related to the amount of the adsorbed electrocatalyst , leading to the different electrochemical signals for readout towards paracetamol (AP). This biosensor shows a low limit of detection of 0.713 fM with the dynamic range of 20 fM −600 pM under the optimal experimental conditions, providing a powerful platform for detecting miR-21. Furthermore, the designed biochemical self-assembly strategy of this electrochemical biosensor is promising candidate for potential applications in the analysis of other important genetic biomarkers for early diagnosis of cancers.
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PubMed
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APPLIED SURFACE SCIENCE
·
2022
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IF 7.392
Xiaoqian Zhang,Qing Dong,Yuping Wang,Ze Zhu,Zhenfeng Guo,Jichao Li,Ying Lv,Yuk Tak Chow,Xinqiang Wang,Luyi Zhu,Guanghui Zhang,Dong Xu
Water-soluble pollutants including pharmaceuticals and personal care products (PPCPs) and inorganic arsenic have posed challenges to water and the environment. In this work, the water-stable metal–organic framework UiO-66 was loaded on electrospinning zirconia nanofibers membrane via the in-situ solvothermal method. This novel composite membrane had increased surface area, good adsorption performance, and could dynamically remove contaminants from polluted water. Adsorption performance of the composite membrane for tetracycline (TC) and As(III) were investigated using batch experiments. The maximum adsorption capacities were 59.27 mg/g for TC and 143.95 mg/g for As(III). The membrane’s dynamic removal efficiency for TC and As(III) could reach over 90% and 80%, respectively, at a relatively high flux of 60 L/(m 2 ·h), and could be generated and reused. pH values had strong impacts on the electrostatic interaction force, thus influenced the absorption efficiency. The adsorption mechanisms were studied by experimental characterizations and DFT calculations, and the results showed that direct interaction, hydrogen bond and ligand exchange were the main driving forces, and Zr O bond played a significant role in this process. Based on the self-supporting structure and good adsorption performance, we believe this novel composite membrane could find notable applications in wastewater decontamination.
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ACS Applied Nano Materials
·
2021
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IF 5.097
Haojie Zhao,Beili Yi,Xiaomeng Si,Lei Cao,Longxing Su,Yanli Wang,Lien-Yang Chou,Jin Xie
Perfect crystals do not exist; however, the introduction of defects can tailor the physical and chemical properties of materials. Defects in metal–organic frameworks (MOFs) have been demonstrated to be important in many applications, including but not limited to catalysis, gas separation, and energy storage. While a few liquid-phase synthesis methods have been reported to prepare defect-rich UiO-66, the heavy use of organic solvents may cause irreversible environmental problems. Here, we present a green, rapid, and facile solid-state synthesis approach to prepare UiO-66. All UiO-66 crystals remain in the nanometer size due to the limited diffusivity of growth species in solid-state synthesis without a large quantity of the solvent. The defect concentrations can be fine-tuned by the content of ethanol addition. Defect-rich UiO-66 shows excellent catalytic activity to the ring opening of epoxides with alcohols. This work provides insights into the large-scale production of defect-rich MOFs.
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