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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ENVIRONMENTAL RESEARCH
·
2025
·
IF 7.7
Kaichun Lin,Jingjun Qin,Zhang Liu,Weicheng Xu,Meng Li,Yuanzhi Zheng,Wei Han,Guangying Zhou,Jianzhang Fang,Zhanqiang Fang,Feng Peng,King Lun Yeung
Pollutant removal through green photocatalysis combined with advanced oxidation processes (AOPs) is critical for efficient wastewater treatment but is limited by poor light harvesting and inefficient oxidant activation. This study addresses these challenges through developing a Co-incorporated UiO-bpydc MOF for enhanced visible-light-driven photocatalysis via peroxymonosulfate (PMS) bridged ligand-to-metal charge transfer (LMCT). The MOF was synthesized through direct cobalt complexation into the UiO-bpydc framework for enabling visible light absorption. The UiO-bpydc(Co) achieved 95.8% degradation of lomefloxacin (LOM) within 30 minutes in the presence of PMS, attributing to narrowed bandgap (i.e., 2.82 eV), improved charge transfer via Co centers, and increased pollutant affinity due to electron-rich ligand. Additionally, the generation of long-lifespan singlet oxygen ( 1 O 2 , 41.8%) was identified as the key reactive species. Theoretical calculations indicated a reduced HOMO-LUMO gap upon the formation of a -Co-OOSO 3 bridge, which promotes carrier separation and improves pollutant-catalyst interactions. The degradation pathways and toxicity evolution of intermediates were clarified, while the exceptional stability, recyclability, and broad pollutant applicability of UiO-bpydc(Co) demonstrate its potential for utilization in oxidative environments This work highlights the potential of transition metal doping to alter the electronic structure of MOFs for target-specific catalytic reactions, offering new opportunities for advanced environmental remediation technologies.
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PubMed
高影响因子
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
·
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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高影响因子
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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DALTON TRANSACTIONS
·
2022
·Vol. 51
·期 10
·4043-4051
·
IF 4.569
Yiming Wang,Xu Zhu,Xinyue Zhang,Jianwei Zheng,Hong Li,Nianyi Xie,Ying Guo,Hong-bin Sun,Gang Zhang
The treatment of mercury pollutants in water has been wide concern. Adsorption is a promising method for mercury removal that has been extensively studied. Nevertheless, the secondary application of the immobilized Hg is seldom investigated. In this paper, the Hg adsorption behavior of UiO-66 bearing sulfhydryl groups is studied. The research shows that the porous structure and sulfhydryl groups of UiO-66-SH can effectively promote the removal of mercury from water. In addition, this work also pushes forward the sequential application of the recovered adsorbent, which contains the adsorbed mercury that may cause secondary pollution. The recovered waste adsorbent, UiO-66-S-Hg, was successfully used as an efficient catalyst for transfer vinylation, which produces value-added products, vinyl benzoates. Eight vinyl esters have been successfully synthesized with a yield of up to 89%. This methodology provides a promising way for not only the treatment of mercury contamination, but also secondary pollution protection and the resource utilization of immobilized Hg.
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Journal of Cleaner Production
·
2021
·
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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ACS Applied Nano Materials
·
2021
·
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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APPLIED SURFACE SCIENCE
·
2022
·
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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