JOURNAL OF ALLOYS AND COMPOUNDS
·
2020
·
IF 4.65
Jingjing Yang,Le Shao,Xun Wang,Yan Yang,Zhanyuan Tian,Weixing Chen,Gai Zhang,Chao Shen
Solid composite polymer electrolytes have been proposed as high-performance solid electrolytes for next-generation energy storage devices. In particular, UiO-66 with monodispersed size (400 nm) and morphology and outstanding stability was introduced as a functional filler to modify the electrochemical properties of poly(ethylene oxide) (PEO) solid electrolytes with LiClO 4 as the lithium salt. The desired physicochemical properties and electrochemical properties of the electrolyte was improved through microstructure regulation and the intermolecular interactions, as confirmed by X-ray diffraction, differential scanning calorimetry , optical microscopy and electrochemical characterisation. Owing to the intermolecular interactions, crystallisation of PEO was inhibited, and the ionic conductivity of the solid composite polymer electrolyte increased to 4.8 × 10 −5 S cm −1 at 25 °C. Electrochemical stable window and lithium ion transference number (t + ) were also observably enhanced. The assembled LiFePO 4 /PEO-LiClO 4 -UiO-66/Li solid-state lithium batteries exhibited excellent cycling and C-rate performances. The initial discharge capacity reached to 160 mAh g −1 , and superior cycle stability with a capacity retention ratio of 83% after 200 cycles at 1C current and 80 °C was achieved. The discharge capacity at 5C was improved by 232%. This work provides new insights into boosting the performances of solid composite polymer electrolytes through intermolecular interactions.
研究领域:
材料科学
·
电化学
·
能源存储
·
高分子物理
·
纳米复合材料
·
固态电池
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DOI
高影响因子
Catalysis Science & Technology
·
2025
·
IF 4.2
Kai Yan,Zhihao Yu,Yingqing Li,Mengyan Guo,Yuanyu Wang,Xuebin Lu
The efficient dehydration of fructose to 5-hydroxymethylfurfural (HMF) is a crucial step in biomass valorization, requiring solid acids with precisely balanced Brønsted acidity. Defect engineering in Zr-based metal–organic frameworks (MOFs), such as UiO-66, is well known to enhance Lewis acidity; however, its impact on tailoring Brønsted acid sites remains insufficiently understood. Here, we demonstrate that defective UiO-66 possesses a dual-origin Brønsted acid system, comprising intrinsic μ3–OH groups and water molecules coordinated to defect-generated Lewis acidic Zr centers (Zr–H2O). The concentration of these Brønsted acid sites can be finely regulated by thermal activation treatment. A volcano-shaped dependence of catalytic activity on activation temperature is observed, with an optimum at 200 °C. At moderate activation temperatures below 200 °C, the removal of physisorbed water exposes both μ3–OH and Zr–H2O sites, maximizing Brønsted acid density and HMF yield. Activation beyond 200 °C reduces both types of Brønsted acid sites, resulting in diminished catalytic performance. This study reveals the cooperative effect of defect engineering and thermal activation in tuning the Brønsted acidity of MOFs, providing a rational strategy for designing highly selective catalysts for the sustainable production of platform chemicals.
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高影响因子
ANALYST
·
2021
·Vol. 146
·期 9
·3052-3061
·
IF 4.616
Jie Min,Xiang-Long Qu,Bing Yan
By means of post-synthetic treatment on the UiO-66 derivative with –SO3H, a novel luminescent hybrid material named Tb3+@UiO-66–SO3H has been prepared simply and efficiently. Given its wonderful luminescence properties like intense green emission, a long lifetime, a robust structure and photostability, it is further developed as a fluorescent probe for the sensing of trans,trans-muconic acid (tt-MA, a biomarker of benzene) and Fe3+, which are closely related to human health. Notably, Tb3+@UiO-66–SO3H shows an outstanding recognition ability for Fe3+ among common cations with a low detection limit (0.11 μM, 0.006 ppm). More importantly, Tb3+@UiO-66–SO3H can realize highly sensitive and selective detection of tt-MA (detection limit, 0.58 μM, 0.083 ppm). Besides, this rapid response probe is facilely prepared, non-toxic and reusable, showing the potential of Tb3+@UiO-66–SO3H in the practical monitoring of tt-MA and Fe3+.
研究领域:
材料科学
·
分析化学
·
环境健康
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DOI
PubMed
高影响因子
COMPOSITES PART B-ENGINEERING
·
2020
·
IF 7.635
Shuangjiang He,Yingqing Zhan,Jiaxin Hu,Guiyuan Zhang,Shumei Zhao,Qingying Feng,Wei Yang
Multi-component pollutant-oil-water emulsion from the fast-growing industry seriously threatens the human health and ecological environment, which poses a huge challenge to membrane technology. Recently, 2D MXene materials have shown promising and potential candidates for functional separation membranes . Herein, for the first time, a multitasking hierarchical MXene@UIO-66-(COOH) 2 composite membrane supported on nylon 66 microporous substrate was designed via a facial strategy, which possessed high chemical stability and efficient multi-component pollutant-oil-water emulsion separation performance. The promising synergistic separation performance of various oil-in-water emulsions and dye, high antifouling resistance, and excellent recyclability of MXene@UIO-66-(COOH) 2 composite membrane originated from the inherent hydrophilicity , low oil adhesion feature, and hierarchical intercalation structure of membrane. Furthermore, the chemically stable MXene@UIO-66-(COOH) 2 composite membrane exhibited outstanding corrosion resistance under strong acid (3 M HCl), alkali (1 M NaOH) and salty (Saturated NaCl) solutions. Therefore, this work provides a powerful platform for designing stable and functional 2D membrane materials for multi-component pollutant-oil-water emulsion separation in harsh chemical environments.
研究领域:
材料科学
·
环境工程
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DOI
高影响因子
Journal of Materials Chemistry A
·
2024
·
IF 10.7
Wen Lu,Chen Wang,Wenhui Song,Zhixiong Zhang,Chengde Xie,Jianjun Wang
The heavy metal ion hexavalent chromium (Cr(VI)) in wastewater significantly threatens public health. Heterojunction photocatalysts typically demonstrate high reduction efficiency in water for Cr(VI) contamination. Overcoming the drawbacks of single metal organic frameworks (MOFs) or covalent organic frameworks (COFs), MOF@COF heterostructures inherit the advantages of large porosity, high surface area, and multiple active sites of single components. Herein, we report novel hybrid UiO-66-NH2@HDU-25 heterojunctions based on a condensation reaction. The optimal ratio of UiO-66-NH2@HDU-25 presented significantly superior photocatalytic activity to most reported MOFs and COFs due to heterojunction formation, which promoted charge separation. Under identical conditions, the optimally formulated UiO-66-NH2@HDU-25 could remove over 99% of Cr(VI), approximately 1.8 and 2.6 times the original UiO-66-NH2 and HDU-25 levels. Furthermore, the UiO-66-NH2@HDU-25 (8 : 1) heterojunction demonstrated favorable reusability and stability over five reaction cycles. Various experiments and density functional theory (DFT) calculations investigated the charge carrier transport pathways and possible photocatalytic mechanisms. The Z-scheme mechanism for the photocatalytic Cr(VI) reduction by UiO-66-NH2@HDU-25 was proposed and validated. This work aims to open new horizons for preparing novel photocatalyst heterojunctions with excellent visible light responsiveness for environmental water remediation.
研究领域:
环境科学
·
材料科学
·
化学工程
·
光化学
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DOI
高影响因子
ANALYTICAL CHEMISTRY
·
2025
·
IF 6.7
Chengli Xie,Longcheng Gong,Tong Xu,Lianzhe Hu,Zhining Xia,Min Wang
To overcome the limitation of low catalytic activity in nanozyme labels for immunoassay, this study proposed a heterovalent Co-doping strategy to construct the bimetallic Zr/Co-UiO-66-NH2 nanozyme. Compared to the undoped UiO-66-NH2, the resulting nanozyme exhibited a 14-fold enhancement in phosphatase-like catalytic efficiency (kcat/Km). Mechanistic investigations revealed that the activity enhancement was not only dependent on the high specific surface area and increased defects introduced by heterovalent Co doping, but also was attributed to the electronic synergy between Zr and Co. Furthermore, a fluorescent immunoassay method utilizing highly efficient Zr/Co-UiO-66-NH2 as the nanozyme label was developed for the ultrasensitive detection of carcinoembryonic antigen (CEA). This method achieved a broad linear detection range spanning 6 orders of magnitude (1 × 10–12 g/mL to 1 × 10–6 g/mL) and a detection limit as low as 0.74 × 10–12 g/mL. The high recovery rates (95.89%–99.31%) in serum samples demonstrate great potential for the detection of CEA in complex biological matrices.
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2020
·
IF 7.183
Rong Rong,Yanwei Sun,Taotao Ji,Yi Liu
Zirconium-based MOF (Zr-MOF) membranes have attracted widespread attention due to their highly tailorable pore aperture and adsorption behavior achieved by functional group decoration and ligand/cluster-missing defect regulation as well as extraordinary chemical/thermal stability. Nevertheless, it has remained a great challenge to further improve the separation performance of Zr-MOF membranes due to very limited available zirconium sources and heating modes. In this study, we prepared polycrystalline UiO-66 membranes exhibiting unprecedented CO 2 /N 2 selectivity (31.3). The use of layered ZrS 2 , a representative of transition-metal dichalcogenides (TMDCs), as zirconium source during tertiary solvothermal growth was found to be indispensable for improving the separation performance of UiO-66 membranes. As far as we know, the CO 2 /N 2 selectivity reported in this study was the highest among all pristine polycrystalline MOF membranes measured under ambient conditions. More importantly, our study highlighted the importance of concurrent metal source and fabrication process innovation in performance enhancement of polycrystalline MOF membranes.
研究领域:
材料科学
·
化学工程
·
膜技术
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DOI
高影响因子
LANGMUIR
·
2022
·
IF 4.331
Bingying Jia,Liujie Bing,Bang Xu,Jihong Sun,Shiyang Bai
The amine (NH2)-functionalized UiO-66 was successfully anchored on disorderly layered clinoptilolite (CP) via surfactant (poly(ethylene glycol) (PEG) and poly(vinylpyrrolidone) (PVP))-assisted induction. The structural features and physicochemical parameters of the resultant UiO-66-on-CPs were characterized by powder X-ray diffraction (XRD) patterns, scanning/transmission electron microscopy (SEM/TEM) images, Fourier transform infrared (FT-IR) spectra, N2 sorption isotherms, and small-angle X-ray scattering (SAXS) patterns. The results demonstrated that the growth of UiO-66-NH2 nanoparticles facilitated the disorder degree of the crystal plane of CP along the a-axis, while the addition of PEG in the hydrothermal synthesis system of CP was conducive to the formation of a flower-like microstructure and the introduction of PVP was beneficial to the nucleation and growth of UiO-66-NH2 nanoparticles with a small size (40 nm) on the surfaces of the obtained CP-PEG lamellas. Finally, the gas-selective adsorption and separation performances of CO2 and CH4 were evaluated using the synthesized disorderly layered UiO-66-on-CP heterostructures as adsorbents, indicating that the NH2-functionalized UiO-66-on-CP exhibited a superior selective factor (3.66) of CO2/CH4. These results elucidated that the proposed approach is a promising strategy for constructing MOF-on-zeolite heterostructures, which may open an avenue to expand CP application and improve their performance.
研究领域:
材料科学
·
化学工程
·
环境科学
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DOI
高影响因子
Foods
·
2025
·Vol. 14
·期 18
·3264
·
IF 5.1
Yimeng Pang,Zehao Yang,Xiaohua Liu,Xing Shen,Hongtao Lei,Xiangmei Li
Gentamicin (GEN) is a broad-spectrum antibiotic widely used in livestock production, and its excessive residues in animal-derived foods pose potential health risks to consumers. However, conventional colloidal gold immunochromatographic assays (AuNPs-ICA) often suffer from low sensitivity and poor tolerance to sample matrices. Herein, a UiO-66-NH2framework decorated with gold nanoparticle (UiO-66-NH2@Au)-based ICA was employed to construct an ICA platform for GEN detection, combining the optical advantages of AuNPs with the protective and stable octahedral framework of the Metal-organic framework (MOF) to enhance antibody stability under extreme conditions. The method achieved limits of detection for GEN of 0.1 µg/kg in four tested matrices, with recoveries of 80.1–112.0% and coefficients of variation below 11.7%. Compared to traditional AuNPs-ICA, the sensitivity was improved by up to 30-fold, the pH tolerance range was expanded from 6–8 to 4–10, and the organic solvent tolerance to organic solvents expanded up to 40%. Verification with 40 real samples demonstrated excellent correlation (R2> 0.99) with results from commercial ELISA kits. This UiO-66-NH2@Au-ICA platform offers a new technical solution with high sensitivity, strong good anti-interference performance, and robustness for rapid field detection of GEN residues in products of animal origin and holds significant practical importance for advancing rapid food safety detection technologies.
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DOI
PubMed
高影响因子
ANALYST
·
2020
·Vol. 145
·期 9
·3245-3256
·
IF 3.978
Liping Xu,Jiebin Li,Jiajia Zhang,Junyong Sun,Tian Gan,Yanming Liu
In this work, a disposable molecularly imprinted electrochemical sensor was developed towards the highly sensitive and selective detection of the organophosphorus insecticide phosalone (PAS), employing a home-made carbon paste microelectrode (CPME) modified with a Zr-based metal–organic framework catalyst (Pt-UiO-66) and a mesoporous structured conductive molecularly imprinted polymer (MIP). Pt-UiO-66 octahedra with isolated dispersed Pt nanoparticle active sites were firstly incorporated into the CPME to provide a remarkably amplified signal for voltammetric determination. The mesoporous MIP was then synthesized onto the Pt-UiO-66/CPME via electropolymerization and a subsequent sol–gel process, which could bind the PAS template molecules through hydrogen bond, coordinate bonding, hydrophobic interaction, and π–π stacking interaction. Morphological, structural, and electrochemical characterization studies revealed that this nano-sized MIP provided excellent features for PAS detection, including high porosity, large surface area, enhanced electron-transport ability, greatly improved diffusion capacity, and strong recognition specificity. Therefore, the resulting sensor exhibited an outstanding linearly proportional concentration domain of 0.50 nM–20 μM, low detection limit of 0.078 nM, marked selectivity over certain interferences with similar configurations, considerable repeatability, reproducibility, and stability for the analysis of PAS. Moreover, the sensor was successfully applied for the determination of PAS in agricultural products and environmental samples with results in good compatibility with a chromatographic method, indicative of the high reliability and practicability. Such an electrochemical sensor might open a novel window for the investigation of selective sensing of small organic species from their analogues coupled with the molecular imprinting technique.
研究领域:
分析化学
·
环境科学
·
农业科学
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DOI
PubMed
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2022
·
IF 10.53
Jiang Fan,Wufeng Wu,Zong Lu,Yanying Wei
The Metal-Organic Framework (MOF) materials are ideal molecular sieving membrane materials due to the regular pores with high-density and good designability, which have been widely studied in gas separation, desalination, and nanofiltration , etc. However, most preparation methods of MOF polycrystalline membranes are always time-consuming and the as-synthesized MOF membranes are thick. Here in this work, the ultrathin 210 nm-UiO-66 polycrystalline membranes are rapidly synthesized in 1 h, where sonication is utilized to generate massive tiny nucleation followed with rapid microwave-assisted membrane growth. The Na + rejection of the UiO-66 membrane maintains at 99.6% for 700 h long-term experiment with 0.16 L/(m 2 h bar) of water flux in forward osmosis, indicating the good quality and excellent stability of the as-synthesized membrane. This strategy is also expected to synthesize many other continuous defect-free MOF membranes with ultrathin thickness rapidly.
研究领域:
材料科学
·
化学工程
·
膜技术
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Xianjie Wang,Yaning Zhao,Hengsheng Wei,Yi Wang,Jingdong Gou,Jinhui He,Xue Ma,Louwei Cui,Liuyi Pan,Jiaojiao Liu,Dong Li
The separation of coal-derived C8 cyclohexane isomers, particularly cis-1,3-dimethylcyclohexane (cis-1,3-DMCH) and ethylcyclohexane (ECH), remains challenging due to their similar molecular structures and physicochemical properties, while research on cycloalkane isomer separation is limited. A series of functionalized UiO-66 derivatives (UiO-66, UiO-66-(CH 3 ) 2 , UiO-66-OH, and UiO-66-NO 2 ) were synthesized via solvothermal methods and systematically evaluated for their adsorption and separation performance toward C8 cyclohexane isomers through single-component and competitive batch adsorption experiments, dynamic breakthrough tests, and molecular simulations. Among the investigated materials, UiO-66-NO 2 demonstrated superior selectivity (α = 5.10) for cis-1,3-DMCH over ECH, with excellent regeneration stability over multiple cycles, significantly outperforming commercial activated carbons and zeolites. Mechanistic studies revealed that the enhanced selectivity arises from a dual mechanism combining geometric confinement effects and electronic recognition, where the oblate geometry and larger dipole moment of cis-1,3-DMCH enable preferential adsorption through strengthened C-H···O and C-H···NO 2 interactions, as confirmed by calculated binding energies (−37.15 kJ/mol for cis-1,3-DMCH vs. -22.13 kJ/mol for ECH) and diffusion coefficients. This work demonstrates rational MOF functionalization for efficient cycloalkane isomer separation, providing a promising strategy for coal-derived naphtha valorization.
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高影响因子
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