CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Ying Gao,Yong Liu,Lingling Gao,Jinxing Long
An effective strategy is proposed here for transfer hydrogenation of alkyl levulinate to γ-valerolactone (GVL) using a UiO-66 framework modified with phosphotungstate ionic liquid (UiO-66@IL(HPW)). Due to the intensive influence of ionic liquid fragment, the modification significantly enhances the catalytic activity of UiO-66@IL(HPW), leading to a complete conversion of ethyl levulinate with over 93.1% selectivity for GVL. Characterizations techniques, including XRD, N 2 absorption/desorption, SEM, FT-IR, pyridine FT-IR, NH 3 -TPD and CO 2 -TPD, confirm that while the basic structure of UiO-66-NH 2 is insignificantly changed, the introduction of the ionic liquid greatly improves the acidic/base properties of the catalyst. XAFS and XPS results reveal an intensive interaction between the N and W species in UiO-66@IL(HPW), and the formed W-N/O moiety is responsible for the enhanced catalytic activity. In addition, a plausible catalytic mechanism is proposed based upon in situ DRIFTS and density functional theory (DFT) calculations, highlighting the crucial role of ionic liquid fraction within the UiO-66 ligand. Therefore, this work would contribute to the valorization of biochemicals.
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Journal of Energy Storage
·
2024
·
IF 8.9
Bahaaudin M. Raffah,Haseebul Hassan,Muhammad Waqas Iqbal,Yas Al-Hadeethi,Bassim Arkook
The precisely defined nanostructures are used to develop highly efficient catalysts for processes like the hydrogen evolution reaction (HER) and energy storage. However, this endeavor remains a formidable challenge. The porous Zr-MOF and its composite with molybdenum disulfide were prepared using a straightforward hydrothermal technique. These materials were evaluated for their supercapacitor and hydrogen evolution reaction (HER) in a 1 M KOH electrolyte. The capacitance experiments indicated a noteworthy increase in the specific capacitances to 1392C/g for UiO-66/MoS 2 . The supercapattery was also formed using UiO-66/MoS 2 and activated carbon. The UiO-66/MoS 2 device demonstrates 66.87 Wh/kg energy density at a power density of 1100 W/kg. The findings revealed that UiO-66/MoS 2 exhibited a lower overpotential of 132 mV for HER. The superior HER catalytic performance of UiO-66/MoS 2 was due to the enhanced availability of active sites at the edges and vertices of nanocubes in the nanoflower architecture. This study highlights the UiO-66/MoS 2 can substantially enhance the storage and catalytic activity.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
·
IF 7.7
Shuo Li,Yawen Guan,Yunjie Li,Yuzhuo Tuo,Yakun Luo,Liang Si,Yingjie Hua,Fang Chai
As an early multi-purpose tumor marker of hepatocellular carcinoma, alpha-fetoprotein (AFP) plays a vital role in early diagnosis and treatment. To achieve the early and accurate determination of AFP, the POMOF was fabricated by embedding H 3 PW 12 O 40 (PW 12 ) into UIO-66-NH 2 , further immobilized on reduced GO (rGO) and fabricated an innovative POMOF nanocomposite (PW@UIO-Au/rGO) as an electrochemical immunosensor (ECI-sensor). The PW@UIO-Au/rGO achieved 17-fold signal enhancement owing to their synergistic effect, enabling PW@UIO-Au/rGO exhibit high oxidase-like catalytic activity, facilitating their sensing performance. Under optimal experimental conditions, the proposed PW@UIO-Au/rGO ECI-sensor presented excellent sensing performance over a wide range from 0.01 ng mL −1 to 500 ng mL −1 with ultra-low detection of 4.0 pg mL −1 . Notably, sensing results in real serum samples were verified by the clinical enzyme-linked immunosorbent assay (ELISA) and electrochemiluminescence immunoassay (ECL) methods with excellent accuracy and consistency, indicating the excellent environmental tolerance of the proposed ECI-sensor. This work provided a promising strategy for designing feasible ultra-sensitive probe for sensing AFP in clinical test.
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PubMed
高影响因子
TALANTA
·
2024
·
IF 5.6
Dandan Guo,Diya Zheng,Ding Zhou,Changlun Tong,Shaohua Huang
Lysine (Lys) is an essential nutrient that plays a crucial role in the growth and development of living organisms. Chiral analysis of Lys holds significant importance for ensuring the safety of food, pharmaceuticals, and health products. In this work, an achiral Zr-based metal organic frameworks (MOFs), UiO-66-NH 2 , was proposed as a fluorescent probe to achieve rapid response to l -lysine (L-Lys) in solution. Additionally, Zr 4+ in the skeleton of UiO-66-NH 2 framework exhibited different binding capacities towards Lys enantiomers, leading to distinct fluorescence responses for L-Lys and d -lysine (D-Lys). Leveraging these properties, the UiO-66-NH 2 probe enabled accurate determination of L-Lys concentrations in solution, as well as the enantiomeric excess (ee) values of Lys solutions. Notably, in the detection of Lys enantiomers, the achiral UiO-66-NH 2 acted as both a chiral selector and a fluorescent indicator, greatly improving the efficiency and stability of the detection system. The probable mechanism was further elucidated by pH titration experiments and density functional theory calculations. Additionally, the general applicability of this mechanism was validated by similar amino MOFs. The application of the UiO-66-NH 2 fluorescent probe in analysis of infant formula milk powders and liquid milk samples confirmed the reliability of the method. Moreover, the construction of fluorescence test paper by immobilizing UiO-66-NH 2 onto filler papers enabled the rapid identification of Lys enantiomers. Compared to previous fluorescent analyses of chiral amino acids assisted by additional metal ions, this study presented a novel approach and methodology that offers high efficiency, stability, reproducibility and reusability for the identification and detection of Lys enantiomers, highlighting the potential of the UiO-66-NH 2 fluorescent probe in advancing analytical techniques.
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高影响因子
CATALYSIS LETTERS
·
2025
·Vol. 155
·期 2
·1-18
·
IF 2.4
Xu Lingling,Pan Xiaomei,Gao Lijing,Wei Ruiping,Li Jihang,Wen Xiu,Li Yuanzhuang,Xiao Guomin
UiO–66–NH 2 (Ti/Zr) modified by Ti metal oxide (TiO 2 ) was used to catalyze the hydrolysis of cellulose to prepare 5-HMF. Under the optimal reaction conditions of H 2 O(NaCl)/THF(1/4 mL), 190 °C, 2 h and 50 mg UNT-3(Ti/Zr) (TiO 2 and UiO–66–NH 2 with mass of 1.5 and 0.1 g, respectively), the yield of 5-hydroxymethylfurfural reached 59.88%. UiO–66–NH 2 (Ti/Zr) nanocomposites with different mass ratios were successfully prepared by simple solvent evaporation method. SEM and TEM have shown that the modified UiO–66–NH 2 (Ti/Zr) are wrapped into sphere by TiO 2 densely attached to the surface of UiO–66–NH 2 , which provides favorable conditions for the uniform dispersion of TiO 2 and coordination of the Lewis acidic site of UiO–66–NH 2 . NH 3 –TPD results confirmed the existence of super-strong, strong, middle and weak acid sites in UiO–66–NH 2 (Ti/Zr), and Py-FTIR confirmed the existence of Brønsted and Lewis acids. After four cycles, the yield of 5-HMF and FUR decreased slightly from 59.88 to 51.89% and 9.11 to 7.66%, respectively, and the yield of 5-HMF could still remain above 50%. The results showed that the modified composite treatment of TiO 2 with rich Lewis acid/base and UiO–66–NH 2 could provide a certain idea for the extensive application of biomass research in the future. Graphic
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ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Xiaoyan Han,Shan Wang,Tingting Cui,Yumin Yang,Haixiang Li,Haiwen Zhang,Huanhuan Zhou,Xiaoxia Li
Aristolochic acid I (AA-I), a known nephrotoxin and carcinogen, is commonly found in certain medicinal plants, posing significant safety concerns. In this work, defect-engineered, molecularly imprinted UiO-66-NH2 was synthesized via a one-pot hydrothermal method using indomethacin (IND) as a green alternative template. The resulting imprinted metal–organic framework effectively mitigates matrix interference, enabling highly selective recognition and the efficient adsorption of AA-I. Structural characterization confirmed that the imprinting process and template removal did not compromise the framework integrity of UiO-66-NH2. Spectroscopic analysis revealed that AA-I recognition was governed by Zr coordination, electrostatic interactions, and spatially confined recognition sites within the porous framework. Density functional theory calculations further elucidated the interaction mechanisms involved in the adsorption process. The imprinted UiO-66-NH2 exhibited a maximum adsorption capacity of 42.74 mg/g and an imprinting factor of 2.48. In real sample analysis, the material achieved recovery rates of 96.7–103.5% and excellent selectivity in Clematis armandii extracts. The adsorption efficiency remained above 80% after five adsorption–desorption cycles, indicating good structural stability and reusability. This work offers a promising and sustainable strategy for improving herbal medicine safety through the rational design of ecofriendly MOF-based adsorbents.
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Materials Today Chemistry
·
2025
·
IF 6.7
Liang Chu,Teng Zhao,Zhaokun Wang,Xinyu Zhao,Zhiyong Zhu,Mu Yang,Ge Wang
The development of efficient oxidative desulfurization (ODS) catalysts is of great importance for clean energy. In this study, we report a method for the preparation of defect-enriched UiO-66(Zr) materials via a high-energy ball-milling pretreatment-assisted followed by rapid ethanol crystallization. This method significantly enhances ligand deficiency (46.1 %) and average pore diameter (4.1 nm) without using toxic solvents or pre-synthesized clusters, distinguishing it from conventional solvothermal and one-step mechanochemical approaches. Under the optimal parameters, the resulting UiO-66-BM catalyst exhibits excellent ODS performance, achieving full conversion of dibenzothiophene (DBT, 1000 ppm) within 6 min at 50 °C and 20 min at 30 °C using only 20 mg of catalyst and an O/S molar ratio of 5. The turnover frequency (19.85 h −1 ) and mass specific activity (53 mmol g −1 h −1 ) surpass those of most reported pristine MOFs-based catalysts. Moreover, the catalyst reaction activity maintains high activity over six consecutive cycles, showing excellent stability. The superior performance is attributed to the synergistic effect of ball milling and ethanol crystallization, which generates the enriched structural defects and enlarged mesopores, facilitating mass transfer and active site accessibility. This work presents an effective and eco-friendly strategy for the scalable synthesis of high-performance MOF catalysts for deep desulfurization.
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NEW JOURNAL OF CHEMISTRY
·
2025
·Vol. 49
·期 23
·9663-9668
·
IF 2.5
Wenhui Yao,Yongkui Chen,Xiaowei Guo
With the wide application of gold as a high-value resource, the recycling of gold has received considerable attention. Owing to the functional active sites, tunable pore size and designable structures, metal–organic frameworks (MOFs) have aroused significant curiosity in gold-recycling. However, designing MOFs with both remarkable adsorption capacity and selectivity for Au(III) is highly desirable but challenging. In this work, two hydroxy-modified UiO-66-type MOFs: UiO-66-(OH)2 and UiO-66-OH have been prepared for rapid and selective adsorption of gold ions from aqueous solution. Significantly, UiO-66-(OH)2 was found to exhibit a remarkable gold adsorption capacity of 1570 mg g−1 (pH = 6) compared with UiO-66-OH (520 mg g−1) under uniform conditions. Furthermore, UiO-66-(OH)2 still exhibited excellent gold adsorption efficiency in the presence of other interfering ions. Mechanism analyses revealed that Au(III) was partly transformed to Au(0) by the reducing action of –OH on the framework in the gold adsorption process. Importantly, the MOF materials can be well regenerated by soaking in hydrochloric acid–thiourea aqueous solution.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Derui Zheng,Yu Wang,Jianhua Zu,Siyu Liu
This study developed a novel defective composite material (UiO-66/D-AMP) based on defect engineering and in situ synthesis of ammonium phosphomolybdate (AMP) for the highly selective capture of Cs + and Sr 2+ . The changes in adsorption capacity and surface functional groups of the composite before and after defect engineering were analyzed by adsorption experiment and FT-IR characterization. It was found that the defect-engineered composite had obvious carboxyl groups, and the adsorption efficiency of Sr 2+ was effectively improved. Several analytical methods were employed to verify the effective incorporation of AMP onto the UiO-66 framework. SEM-EDS was utilized to examine surface morphology and elemental composition. FTIR confirmed the presence of functional groups, while XRD analysis validated the crystalline structure. Additionally, TG assessed thermal stability, and BET measurements determined the material's surface area and porosity, collectively confirming AMP loading. The UiO-66/D-AMP composite exhibited significant adsorption affinity for both Cs + and Sr 2+ ions, demonstrating its potential for radioactive wastewater treatment. Under alkaline conditions (pH 10), the composite demonstrated exceptional removal efficiencies of 98.43% for Cs + and 99.54% for Sr 2+ . The maximum adsorption capacities were determined to be 104.3 mg/g for Cs + and 20.18 mg/g for Sr 2+ . Notably, the adsorption kinetics revealed rapid equilibration times of 5 min for Cs + and 60 min for Sr 2+ . The adsorption kinetics of Cs + and Sr 2+ followed the pseudo-second-order model, while the adsorption isotherms fitted well with the Langmuir model. In mixed solutions containing Cs + , Sr 2+ , and four competing ions, UiO-66/D-AMP exhibited excellent selectivity for both Cs + and Sr 2+ . Remarkably, the adsorption capacities for Cs + and Sr 2+ remained stable following exposure to various adsorbed doses. XPS provided direct evidence for the ion exchange mechanism between Cs + and NH 4 + during adsorption. Sr 2+ first exchanged with H + on UiO-66/D-AMP, then coordinated with the oxygen atom in the carboxyl group to be adsorbed.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2021
·
IF 6.953
Bin Wang,Jin Zhou,Xiang-Yang Zhang,Yu-Shun Yang,Chang-Hong Liu,Hai-Liang Zhu,Qing-Cai Jiao
Enzyme reaction has been accepted widely in numerous applications owing to the high efficiency and stereo-selectivity, as well as simple preparation by gene engineering. However, the fragility and complex purification process of the enzyme are long-standing problems which limit the large-scale application. One possible solution may be the enzyme immobilization. As one type of porous material with high loading capacity and designable functionality, Metal-Organic Frameworks (MOFs) are ideal choices for the immobilization of enzyme with a considerable interest in recent years. In this study, d -amino acid transaminase ( DAT ), an important enzyme for industrial synthesis of d -Ala, was covalently immobilized on the surface of a star MOFs material, UiO-66-NH 2. Interestingly, we found that the nanoscale hybrid enzyme UiO-66-NH 2 -Gd- DAT not only maintained the high catalytic efficiency but also got rid of the interference of polluting enzymes, which meant that we could obtain efficient and stereo-selective immobilized enzyme without complex purification process. In general, our findings demonstrated that using UiO-66-NH 2 might be a promising strategy to immobilize enzyme and produce effective biocatalyst with high activity and stereo-selectivity.
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高影响因子
Catalysts
·
2025
·Vol. 15
·期 3
·220
·
IF 4
Jiani Chen,Yanxuan Wang,Jianghua Huang,Shuting Ma,Yiyang Zhang,Fukun Bi,Xiaodong Zhang
Nowadays, volatile organic compounds (VOCs) increasingly jeopardize ecosystem sustainability and human well-being. In this study, UiO-66 and its different electron beam (EB) irradiation doses (100, 300, 500 kGy) modified materials supported Pt catalysts, Pt/UiO-66 and Pt/UiO-66-X (X = 100, 300, and 500, representing the irradiation doses), were synthesized, and a series of characterizations were conducted on the samples. On this basis, the effectiveness of these catalysts was evaluated through the degradation of ethyl acetate. The study findings indicated that the sample irradiated at 100 kGy demonstrated superior catalytic performance. Thereafter, extensive tests with regard to water resistance, stability, and cycle performance indicated that the Pt/UiO-66-100 catalyst was characterized by satisfactory reusability and catalytic stability, even when faced with high heat and humidity. Further work with in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and thermal desorption–gas chromatography–mass spectrometry (TD-GC–MS) uncovered the process of degradation of ethyl acetate. This research provides a guideline for the design of high-performance VOC degradation catalysts through EB modification.
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Journal of CO2 Utilization
·
2024
·
IF 7.2
Heming Deng,Haoshuang Gu
Two-dimensional membranes are considered the next generation separation membrane with great application potential due to their excellent separation performance, good mechanical strength and thermal stability compared with traditional membrane materials. In this work, the flexible NH 2 -UIO-66@MXene membrane was successfully prepared for gas separation by loading NH 2 -UIO-66 particles onto Ti 3 C 2 nanosheets based on an in-situ growth strategy. A LiF-HCl mixed solution was used as the etchant to obtain the Ti 3 C 2 nanosheets. The loading of NH 2 -UIO-66 particles can regulate the interlayer spacing of Ti 3 C 2 nanosheets, improving the specific surface area of Ti 3 C 2 and the adsorption capacity for specific gases. The -NH 2 group in NH 2 -UIO-66 enabled preferential adsorption of CO 2 over H 2 , and the CO 2 molecules adsorbed in the channel can even block the molecules passing through, increasing the resistance of CO 2 diffusion. As a result, the NH 2 -UIO-66@Ti 3 C 2 hybrid membrane realizes the selective separation of H 2 /CO 2 mixed gas, and the separation selectivity is as high as 155. The gas separation selectivity and permeation of the final prepared NH 2 -UIO-66@MXene were enhanced and exceeded the upper limit of Robeson upper bound (2017).
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