APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Fajie Hu,Rushuo Li,Danfeng Zhao,Xiubing Huang,Ge Wang
The hydrogenation of dicyclopentadiene (DCPD) to synthesize tetrahydrodicyclopentadiene (THDCPD) is one of the key processes for the preparation of high-energy–density fuels, and the development of low-temperature and high-activity Ni catalysts is still challenging. In this work, hierarchical porous (HP) Ce-UiO-66 loaded Ni nanoparticles (NPs) catalysts were prepared based on the soft template method and liquid-phase in situ reduction method. The introduction of mesopores into Ce-UiO-66 can effectively enhance the transfer and adsorption of the substrate, and Ni NPs act as the main active centers. Furthermore, the modulation of the electronic structure of Ni NPs and the promotion of Ce-Ni interaction were effectively achieved by changing the in-situ deposition conditions. With a low loading of 3 wt% Ni NPs, the prepared 3Ni/HP-UiO-66 catalysts could achieve the observed complete DCPD conversion and 100 % selectivity of THDCPD within 1 h and retained good cycling stability. The results demonstrated preferential adsorption and hydrogenation of the norbornene ring, confirming the reaction pathway of the 3Ni/HP-UiO-66 catalyst for the hydrogenation of DCPD. The present work provides a guidance for exploring and designing non-noble metal catalysts for the hydrogenation of olefins and aromatics.
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CARBOHYDRATE POLYMERS
·
2024
·
IF 10.7
Yuan Gao,Peng He,Jingwen Yang,Bo Liu,Qiong Zhang,Qi Zhou,Hanlu Xu,Rongli Jiang,Zhongran Dai,Shaorong Wang
We focus on optimizing acid-base interactions and hydrogen bonding networks to achieve enhanced proton conductivity under low relative humidity (RH) and high temperature. By functionalizing UiO-66-(COOH) 2 with glutamic acid (Glu) and lysine (Lys), we generate Glu-UiO-66-(COOH) 2 and Lys-UiO-66-(COOH) 2 . These modified materials are subsequently incorporated into chitosan (CS) to produce the composites Glu-UiO-66-(COOH) 2 @CS and Lys-UiO-66-(COOH) 2 @CS. The successful incorporation of amino acids and cross-linking between -COOH and -NH 2 groups in the composites, confirmed by FTIR and PXRD analyses, significantly enhances the structural integrity and durability by strengthening the network, and reducing polymer chain mobility. Proton conductivity assessments reveal that Lys-UiO-66-(COOH) 2 @CS-7 exhibits a remarkable conductivity of 0.022 S/cm at 100 % RH and 363 K, outperforming Glu-UiO-66-(COOH) 2 @CS-7. The lower activation energy ( E a ) of 0.28 eV for Lys-UiO-66-(COOH) 2 @CS-7, compared to 0.336 eV for Glu-UiO-66-(COOH) 2 @CS-7, highlights the significant improvement in intramolecular acid-base interactions and hydrogen bonding. Furthermore, Lys-UiO-66-(COOH) 2 @CS-7 maintains notable proton conductivity at 43 % RH, with an E a of 0.216 eV, demonstrating its efficacy in low-humidity conditions. These findings underscore the profound impact of amino acid modifications and cross-linking on proton conductivity by reinforcing acid-base interactions, hydrogen bonding networks, and proton transfer efficiency.
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ELECTROCHEMISTRY COMMUNICATIONS
·
2025
·
IF 4.2
Jie Zhang,Yuanying Shi,Liming Liu,Bin Qiu,Yue Tian,Guodong Guo
In this work, a novel homogeneous electrochemical (HEC) sensing strategy was developed for carcinoembryonic antigen (CEA) detection, addressing limitations of traditional electrochemical platforms that necessitate complex electrode modifications and receptor immobilization protocols. This approach integrates platinum nanoparticle-loaded UiO-66 metal-organic frameworks (Pt/UiO) as an oxidase-like nanozyme with CEA-specific aptamer (Apt) as recognition element, establishing a target-responsive catalytic mechanism. In solution-phase operation, the Pt/UiO nanozyme facilitates the oxidation of 1,2-diaminobenzene into electroactive diaminophenazine (DAP), generating measurable reduction current at unmodified electrode. Apt adsorption onto Pt/UiO surfaces effectively inhibits this enzymatic activity through steric hindrance, resulting in current suppression proportional to Apt coverage. The presence of CEA induces specific Apt-CEA binding, resulting Apt away from the nanozyme surface and restoring catalytic activity in a concentration-dependent manner. Optimization of experimental parameters (e.g., nanozyme concentration, incubation time) enabled the sensor to achieve a detection limit of 3 pg mL −1 with a linear range spanning 0.01–11 ng mL −1 , demonstrating potential for point-of-care applications in tumor biomarker analysis.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2025
·
IF 7.7
Jiaqi Chang,Fengsen Wang,Peng Zhang,Jiaqi Li,Xi Zhang,Fanhong Chen,Qianrui Lv
The controllable pore structures and surface functionalization characteristics of metal-organic frameworks (MOFs) provide new ideas for the development of high-performance humidity sensors. In this study, a hierarchical porous IL/UIO-66-NH 2 material with well-defined microporous-mesoporous channels was successfully synthesized. This unique porous structure results from the steric hindrance effect and competitive coordination of a carboxylic acid-functionalized ionic liquid used as the MOF precursor. By combining the Kelvin equation with Fick's law of diffusion, we revealed how the synergistic interactions within hierarchical pore structures enhance water-molecule transport dynamics, resulting in ultrafast sensor performance with response and recovery times of 0.6 s and 0.9 s, respectively. The humidity sensing mechanism was systematically investigated using electrochemical impedance spectroscopy. The sensor can accurately distinguish respiratory states and recognize short speech signals, providing a new material design strategy for wearable health monitoring devices.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Jingling Gong,Bin Xiang,Ruirui Jin,Zhaoyang Li,Weimin Liu,Jian Li
Membrane fouling is a key challenge to the sustainable operation of oil–water separation membranes. Constructing a stable hydration layer on the membrane surface as an oil-fouling resistance barrier by modulating the physicochemical structure of the membrane is one of the most effective strategies. Herein, inspired by the petal structure in nature, Cu 3 (PO 4 ) 2 and UiO-66-NH 2 particles were combined by a self-assembly strategy to construct CUP (Cu 3 (PO 4 ) 2 /UiO-66-NH 2 /PVA) composite membranes with anti-fouling capability against viscous crude oil. Benefiting from the petal structure and abundant polar groups within the membrane, the as-prepared membrane could easily combine with water molecules to form a stable hydration layer, which acted as a barrier to hinder the oil contamination of the membrane. Further, the hierarchical flower-like structure was conducive to the improvement of the emulsion breaking rate and permeation flux of oil-in-water emulsions. After 60 min continuous cross-flow separation, the obtained CUP composite membrane still remained prominent separation efficiency (99.6 %) and permeate flux (4685.96 LMH/bar). In addition, the CUP composite membranes showed outstanding resistance to acid and alkali as well as abrasion. This study provides an effective method for the advancement of high-performance membranes with high flux and anti-fouling capability in the flied of oily wastewater treatment.
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MOLECULES
·
2025
·Vol. 30
·期 15
·3130
·
IF 4.6
Jun Li,Jianlan Deng,Qian Tao,Chenyu Yan,Yuxuan Liu,Jianxiao Yang,Zhong Cao
Luminescent metal–organic frameworks (MOFs) are used for the detection of organophosphorus pesticides (OPs) due to their large surface area and pore volume as well as their special optical properties. However, most self-luminescent MOFs are not only complex to synthesize and unstable in water but also feature a “turn-off” sensing system, which has highly restricted their practical applications in OP detection. Herein, a “turn-on” fluorescence sensor based on the guest-induced luminescence MOF Ru(bpy)32+@UiO-66 was constructed, which realized the sensitive detection of OPs through a dual-enzyme system for the first time. Compared with self-luminescent MOFs, Ru(bpy)32+@UiO-66 was not only more easily synthesized but also had higher chemical and photostability in water. In this strategy, by means of the hydrolysis of AChE and ChOx, H2O2will be produced, which can oxidize Fe2+to Fe3+, thereby quenching the fluorescence of Ru(bpy)32+@UiO-66. In the presence of OPs, the activity of AChE can be inhibited, resulting in the inability to generate H2O2and Fe3+, which will turn on the fluorescence signal of Ru(bpy)32+@UiO-66. As a result, the Ru(bpy)32+@UiO-66 sensing system not only had high sensitivity for OPs detection but also possessed a satisfactory detection recovery rate for parathion-methyl in real samples, which provides a new approach for OP detection in food safety as well as environmental monitoring.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Xiaoxia Liang,Jiakang Duan,Yu Tian,Yue Han,Zewan Qin,Huixia Zhu,Yating Lu,Dongyu Nie,Yingna Guo,Xia Yang
AgCl/Ag 0 shows great promise for the removal of environmental pollutants, while its photocatalytic performance is still a great challenge on account of the agglomeration. Herein, orientational deposited and octahedral AgCl/Ag 0 were obtained by etching the UiO-66-NH 2 template for the first time. The 0.35:1–AgCl/Ag 0 exhibited outstanding efficiency in the degradation of Diazinon (DZN), which was closely 300 times than that of UiO-66-NH 2 and 0.35:1–AgCl@Ag 0 prepared without a template. Its bigger surface area provided more active sites to promote mass transfer efficiency and large amounts of •OH and 1 O 2 were fabricated to offense specific positions of DZN determined through Fukui function. Meanwhile, a high removal rate of 91.0 % was obtained after 5 recycles. Finally, the results of HPLC-MS, T.E.S.T., TOC and IC indicated all intermediates had less toxicity than DZN and were rapidly mineralized. Our work developed a new strategy for designing superb performance AgCl/Ag 0 photocatalysts.
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JOURNAL OF CHROMATOGRAPHY A
·
2012
·
IF 4.531
Na Chang,Xiu-Ping Yan
Metal-organic frameworks (MOFs) which offer a variety of topologies, porous networks and high surface areas are promising and have potential for the applications of specific adsorption, isomerization, catalysis and separation. UIO-66 is the first MOF that has been observed to have reverse shape selectivity. However, such reverse shape selectivity of MOFs has never been explored for capillary gas chromatographic separation. Here we report the fabrication of MOF UIO-66 coated capillary column and exploration of the reverse shape selectivity and molecular sieving effect of such column for capillary gas chromatographic separation of alkane isomers and benzene homologues with excellent selectivity and precision. The adsorption enthalpies and entropies on the interaction between hydrocarbons and UIO-66 were measured to illustrate the energy effect on the separation of alkane isomers and benzene homologues on the UIO-66 coated capillary column. UIO-66 coated capillary column gave preferential retention of branched alkane isomers over their linear isomer, showing reverse shape selectivity, making UIO-66 coated capillary column attractive for capillary gas chromatographic separation of alkane isomers. iso -Propylbenzene (branched) eluted after n -propylbenzene on the UIO-66 coated capillary column again shows reverse shape selectivity. However, much bulkier 1,3,5-trimethylbenzene eluted earlier than n -propylbenzene and iso -propylbenzene on the UIO-66 coated capillary column, exhibiting molecular sieving effect. The combination of reverse shape selectivity with molecular sieving effect makes the UIO-66 coated capillary column promising for the separation of structural isomers.
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MICROCHIMICA ACTA
·
2024
·Vol. 191
·期 4
·1-13
·
IF 5.3
Yang Peixun,Zhu Xiaoyan,Lan Hangzhen,Wu Yichun,Pan Daodong
A solid-phase microextraction (SPME) Arrow and high-performance liquid chromatography-UV detector (HPLC-UV, detection at 225 nm) based method was developed for the selective determination of nine alkylphenols (APs) in milk. The functionalized mesoporous UiO-66 (4-meso-UiO-66) was utilized as the new coating material, which was synthesized by post-modification of pore-expanded UiO-66-NH 2 by an esterification reaction with 4-pentylbenzoic acid. It was fully characterized by X-ray photoelectron spectroscopy (XPS), fourier transformation infrared spectrometry, nitrogen sorption-desorption test, scanning electron microscopy, transmission electron microscopy, and X-ray diffractometer. The characterization results showed the ester groups and benzene rings were introduced into the 4-meso-UiO-66, and the mesoporous structure was predominant in the 4-meso-UiO-66. The extraction mechanism of 4-meso-UiO-66 to APs is the synergistic effect of Zr-O electrostatic interaction and the size exclusion effect resulting from XPS, selectivity test, and nitrogen sorption-desorption test. The electrospinning technique was utilized to fabricate the 4-meso-UiO-66 coated SPME Arrow and polyacrylonitrile (PAN) was used as the adhesive. The mass rate of 4-meso-UiO-66 to PAN and the electrospinning time were evaluated. The extraction and desorption parameters were also studied. The linear range of this method was 0.2–1000 μg L –1 with a coefficient of determination greater than 0.9989 under the optimal conditions. The detection limits were 0.05–1 μg L –1 , the inter-day and intra-day precision (RSD) were 2.8–11.5%, and the recovery was 83.6%–112%. The reusability study showed that the extraction performance of this new SPME Arrow could be maintained after 80 adsorption-desorption cycles. This method showed excellent applicability for the selective determination of APs in milk. Graphical abstract
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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.
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ENVIRONMENTAL RESEARCH
·
2025
·
IF 7.7
Yuxuan Zhao,Yueli Wen,Xiaonuo Xu,Maohong Fan,Shiyun Guo,Zhiju Chen,Xiaoxiao Zhao,Bin Wang,Wei Huang
The heavy metals discharged from electroplating wastewater, represented as copper and chromium ions, is harmful to aquatic lives and human beings, and will break the ecological balance. In this work, magnetic hybrid porous structure adsorbent of Fe 3 O 4 @SiO 2 -UiO-66-EDTA is prepared for recycling copper and chromium ions. The adsorbent exhibits a maximum adsorption capacity of 212.10 mg/g for Cu(II) and 118.10 mg/g for Cr(VI). Notably, it shows excellent regenerability of 87.12% after 5 cycles. The adsorption of Cu(II) and Cr(VI) on Fe 3 O 4 @SiO 2 -UiO-66-EDTA follows the pseudo-second-order model, where chemical adsorption is dominant and it occurs spontaneously and exothermally. Based on XRD, FTIR, XPS, and DFT calculations, the adsorption mechanisms are driven by electrostatic attraction, chelation, and redox reactions. This work provides a novel and promising strategy for designing highly efficient adsorbents, paving the way for more effective treatments of electroplating wastewater contaminated with Cu(II) and Cr(VI).
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Biofabrication
·
2025
·Vol. 17
·期 3
·035012
·
IF 8
Mengyuan Li,Jiaming Ge,Jingwen Yao,Yuanhao Zhang,Lin Ma,Zheng Li,Xiangli Han,Ming Liu,Fei Tian,Jing Zhao
Oral squamous cell carcinoma (OSCC) is the most common malignant tumor in the head and neck. Due to low bioavailability and passive targetability of anticancer drugs show great limitations in cancer therapy, the treatment of OSCC faces major challenges. Folic acid (FA) targeting can deliver anticancer drugs efficiently into the tumor environment, further enhance the anti-cancer efficacy. Herein, the nanoplatform based on UiO-66 that encapsulated with an effective FA targeting ligands and the pH-responsive polyethylene glycol (PEG) layer for the targeted delivery of berberine (Ber) is constructed for fighting against OSCC. The FA modification and controlled pH-responsiveness enable the targeted delivery of UiO-66/PEG-FA, which promotes the release of Ber and increases the cumulative intracellular Ber concentration, which both promote consumption of glutathione (GSH) and induced generation of reactive oxygen species (ROS), further stimulate the secretion of inflammatory factors (TNF-α and IL-1β). A comprehensive evaluation of in vitro and in vivo experiments show that UiO-66@Ber/PEG-FA promote autophagy and apoptosis of tumor cells by regulating the expression of Beclin-1, ATG13, BAX and Bcl-2, and effectively inhibit tumor growth. Overall, UiO-66@Ber/PEG-FA exhibit superior pH-responsiveness and targeted therapeutic efficiencies in vitro and vivo, it can serve as an approach for OSCC therapy.
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