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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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
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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Journal of CO2 Utilization
·
2025
·
IF 8.4
Zhongqi Zhang,Yingjie Shen,Aosen Zhang,Yuan Zhai,Ziqing Wang,Kun Jiang,Heyun Wang
In this study, imidazole carboxylate was introduced into the structure of UiO-66 as a secondary ligand. Subsequently, a novel imidazole ligand zirconium-based UiO-66-Im- X material was prepared, which was used to catalyze the direct synthesis of dimethyl carbonate (DMC) from carbon dioxide (CO 2 ) and methanol. The influence of imidazole carboxylate content on the physicochemical properties and catalytic performance of the UiO-66-Im- X catalyst was studied. The results showed the addition of imidazole carboxylate increased the number of ligand defects in the Zr 6 formula unit, which significantly enhanced the α-acidic sites of the UiO-66-Im- X catalyst. UiO-66-Im-0.2 with a good crystal structure exhibited the highest surface area, pore volume, and acidic sites and demonstrated the best catalytic activity. At 3.5 MPa, 140 °C, and a reaction time of 8 h, the DMC yield reached 0.9335 %. In addition, the catalytic effect of UiO-66-Im-0.2 exceeded 90 % after four recycling iterations, demonstrating excellent reusability. The in-situ infrared spectroscopy results and density functional theory (DFT) calculations demonstrated that the incorporation of the imidazole ring significantly enhanced the adsorption capacity of CO 2 molecules and reduced its adsorption energy on the UiO-66-Im-0.2 catalyst.
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INORGANIC CHEMISTRY
·
2025
·
IF 4.7
Ying Gao,Ruibin Yang,Qinqin Chen,Xinhao Shen,Dapeng Li,Juanhong Li,Feng Liu,Jianhua Wu,Sanjian Ma,Guoliang Dai,Dongmei Wang,Lei Xie,Zixia Lin,Xin Liu
The large-scale production of iron sludge and the safety issues of H2O2 usage are two limitations in the promotion and application of the Fenton reaction. To further solve the problems, an active hydrogen reduction strategy was proposed. Herein, the reducing property of active hydrogen was utilized to simultaneously generate H2O2 in situ and accelerate the regeneration of ferric in the reaction process. The composite metal–organic frameworks (MOFs) Pd@UiO-66(Zr) and Pd@UiO-66(Zr)-2OH, which were stable under acidic conditions, were synthesized for hydrogen activation. Under the condition of only trace amounts of ferrous and hydrogen added, both catalysts showed excellent performance in the degradation experiments of trimethoprim. The kobs of the Pd@UiO(Zr)-66-mediated system is 0.0487 min–1, which is 1.67 times that of Pd@UiO-66(Zr)-2OH. In the pollutant degradation reaction system constructed by these two materials, both of the hydroxyl radicals and singlet oxygen play a dominant role. The Bader charge analysis showed that the charge transfer from Pd to the MOF host was higher on Pd@UiO-66(Zr) than Pd@UiO-66(Zr)-2OH, which could be a key factor in distinguishing the catalytic activity of the catalysts. In addition, both catalysts showed excellent stability over six cycles. Nearly 100% degradation of trimethoprim could be achieved. This study provides some reference for the control of emerging pollutants by UiO-66(Zr) series materials.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2025
·
IF 8.5
Ziyao Mi,Xuzhen Liu,Yue Zhang,Bo Wang,Hongyu Guo,Yufeng Chen,Yanyan Du,Xinyu Wang,Xiaojun Hu,Jingxian Jiang
The discharge of industrial effluents containing heavy metal ions and organic dyes has laid heavy burdens on ecosystem, meanwhile, drawing extensive scientific attention globally. In this work, CdS/UiO-66-NH 2 heterojunction was uniformly loading on the aerogel skeleton composed of cellulose (CNF), chitosan (CS) and montmorillonite (MMT). The fabricated composite aerogel noted as CUN-CCMA was equipped with light density, a large specific area and a robust three-dimensional interpenetrating network. The MMT not only reinforced the mechanical stability of the aerogel, but also regulated the distribution of the heterojunction. The CUN-CCMA could adsorb various organic dyes and heavy metal ions, and the maximum adsorption capacities for methylene blue (MB) and Cu 2+ were 111.5 mg/g and 45.1 mg/g, respectively. The corresponding adsorption processes were in better consistence with the pseudo-second-order kinetic model and the Freundlich isotherm. The hydrogen bonding, electrostatic interaction, π-π stacking and chelating effect might be attributed to the adsorption mechanism. Most importantly, the removal efficiency of MB with a high concentration of 300 mg/L could reach 94 % when synergistic effect of adsorption and visible light photocatalytic degradation was exerted. The active species that played vital roles during the photodegradation process were recognized as ·OH and · O 2 − . Furthermore, the CUN-CCMA demonstrated an excellent reusability. These outstanding characteristics of CUN-CCMA broadened its application prospects in complicated sewage treatment.
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ANALYTICA CHIMICA ACTA
·
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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Catalysts
·
2025
·Vol. 16
·期 1
·33
·
IF 4
Yao Li,Zaixiao Ren,Juan Bai,Keju Sun,Ziwei Song,Shaotong Song
This study systematically investigates how organic ligand modifications—chain length adjusting and functional group incorporation—regulate the catalytic performance of UiO-66 derivatives for CO2-to-dimethyl carbonate (DMC) conversion. Through multi-technique characterization (Py-IR, TGA, FT-IR, XPS, etc.) and catalytic tests, Lewis acid/basic sites (LAS/LBS), bulk defects and electron density effects were identified as the three key factors to govern the catalytic activity. The bulk defects were believed to enhance mass transfer. Notably, MOF-801 (shortest ligand) and UiO-66-Br (electron-withdrawing-Br) achieved the highest TOFs of 0.86 h−1and 1.10 h−1, respectively. While LAS/LBS and electron-rich Zr clusters promote methanol activation, defect-enhanced mass transfer dominated over electronic effects in boosting DMC yield. These insights highlight the tunability of MOFs for CO2utilization via rational ligand design.
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Nano Research
·
2024
·
IF 9.5
Li Rushuo,Ban Tao,Zhao Danfeng,Lin Jing,Liu Zhiyuan,Wang Linmeng,Huang Xiubing,Tao Zhiping,Wang Ge
Olefin hydrogenation under mild condition is crucial and challenging for industrial applications. Herein, defective UiO-66(Ce) was constructed by using cyanuric acid as the molecular etching “scissors” and further to synthesize heterogeneous catalyst with highly dispersed RuNi nanoparticles (Ru 1 Ni 1.5 @UiO-66(Ce)-12 h). The construction of Ce-O-Ru/Ni heterogeneous interfaces and Ni–Ru bonds provide electron transfer channels from Ce-oxo clusters and Ni species to Ru species. Furthermore, the microenvironment and electronic structure of Ru 0 active sites were synergistically regulated by adjusting the content of metal-organic frameworks (MOFs) defects and Ni promoter, thereby enhancing the adsorption and activation ability of H–H and C=C bonds. Therefore, Ru 1 Ni 1.5 @UiO-66(Ce)-12 h achieved dicyclopentadiene saturated hydrogenation (100% conversion) to tetrahydrodicyclopentadiene (∼ 100% selectivity) under mild condition (35 °C, 1 MPa) with only 25 min. Meanwhile, the sample exhibited excellent structural stability after 6 cycles test. This study provides a promising strategy for the rational design of remarkable noble metal-based catalysts for practical applications.
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