JOURNAL OF HAZARDOUS MATERIALS
·
2025
·
IF 11.3
Xiaoxia Zhang,Xinyuan Zeng,Meng Rong,Mingchuan Yu,Hongtao Yu,Junfeng Niu
Short-chain perfluoroalkyl carboxylic acid (PFCAs) have been widely detected in aquatic systems, posing adverse threats to human health and the environment. However, the effective remediation of short-chain PFCAs in contaminated groundwater remains a major challenge. In this study, Zr-based metal-organic framework UiO-67—featuring tetrahedral cages (12 Å) and octahedral cages (14 Å)—was employed as a platform for precise pore microenvironment regulation. A new modulation strategy using glycine hydrochloride enabled the introduction of linker defects, thereby enhancing the surface positive charge and electrostatic interactions. By incorporating amine and fluorophilic CF 3 functional groups into the organic ligands, three UiO-67 series MOFs, UiO-67-X (X = H, NH 2 , 2CF 3 ), were synthesized for efficient removal of perfluorohexanoic acid (PFHxA) from aqueous solution. Among them, UiO-67–2CF 3 , with a hierarchical pore structure (0.89 nm, 1.14 nm), exhibited exceptional PFHxA adsorption capacity (1386 mg/g), rapid adsorption kinetics (4 min), and excellent selectivity and recyclability. Continuous column breakthrough experiments further demonstrated that UiO-67–2CF 3 effectively reduced PFHxA concentrations from 1 μg/L to below 10 ng/L. In addition, experimental characterizations and DFT theoretical calculations revealed that the adsorption mechanism involves electrostatic interaction, F···F interactions, Lewis acid-base interactions, anion–π interactions, CF 3 –π interactions and hydrogen bonding. These excellent adsorption performances highlight UiO-67–2CF 3 as a promising material for the remediation of short-chain PFCA-contaminated water. This study also provides new insights into the rational design of advanced adsorbents for short-chain PFCAs removal.
研究领域:
环境科学
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材料科学
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污染治理
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吸附技术
·
水处理
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DOI
PubMed
高影响因子
CATALYSIS LETTERS
·
2021
·Vol. 152
·期 4
·1160-1169
·
IF 3.186
Cheng Lin,Cao Liumei,Ren Hao,Guo Qiaoqiao,Deng Huifang,Li Yiming
The construction of a multifunctional catalyst for multistep sequential\tandem reactions at the molecular level faces a formidable challenge. Multivariate (MTV)-MOFs can provide a facile and tunable platform for rationally designing such multifunctional catalysts via grafting different catalytic groups on the bridging ligands. However, the related investigations are still limited. Here, Pd(II) and l -proline are metalated and decorated to organic linkers, respectively, to build a MTV-MOF, which is then successfully applied to sequential Suzuki Coupling/asymmetric Aldol reactions with satisfied coupling performance (yields up to 99%) and good enantioselectivities ( ee anti up to 98%). Inductively coupled plasma optical emission spectrometer (ICP-OES) measurements of the supernatant and hot leaching test suggest the heterogeneous nature of the catalyst. Macrosubstrate tests verify that the reaction occurs inside the pores of the MOF. The heterogeneous catalyst can maintain structural stability and catalytic activity within three cycles. Graphic Abstract Versatile Pd(II) and l -proline were metalated and decorated, respectively, into stable UiO-67 to construct bifunctional and heterogeneous multivariate MOF catalyst, which displayed efficient and recyclable catalytic activity in sequential Suzuki Coupling/asymmetric Aldol reactions.
研究领域:
化学
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材料科学
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催化领域
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DOI
高影响因子
FOOD CHEMISTRY
·
2020
·
IF 6.306
Yong Han,Xie He,Weixia Yang,Xueli Luo,Ying Yu,Wenzhi Tang,Tianli Yue,Zhonghong Li
A ratiometric fluorescent sensor was facilely fabricated using innate fluorescence of carbendazim (MBC) and fluorescent UiO-67 to sensitively and selectively detect MBC in food matrixes. The innate fluorescence of MBC provided a signal at 311 nm (F 311 ), and the fluorescent UiO-67 at 408 nm (F 408 ) could recognize MBC through π-π stacking inducing fluorescent quenching relied on photoelectron transfer (PET). The ratio (F 311 /F 408 ) of the fluorescence enhancement of MBC and the quenching of UiO-67 linearly responded to the MBC concentrations of 0–47.6 μmol/L with a low limit of detection (LOD) of 3.0 × 10 −3 μmol/L. The reverse response signals of the sensor enhanced the sensitivity toward MBC and presented remarkable anti-interference capability in complex matrices. The as-prepared sensor was applied to detect MBC residues in apple, cucumber and cabbage, obtaining satisfactory accuracy and precision with the recovery of 90.82–103.45% and RSDs of lower than 3.03%.
研究领域:
食品科学
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分析化学
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产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Shuting Liu,Ziyu Zengcai,Jingyao Yang,Tianhao Wang,Wenting Lin,Yunhong Pi,Tiejun Wang
To achieve highly efficient in situ hydrogen release from methanol/water reforming at lower temperature, integrating solar-energy provides a promising strategy to activate methanol/water while significantly reducing the activation energy. Herein, we report a series of novel MOF-based photothermal catalysts, mUiO-67-bpy-CuX, featuring enhanced H 2 O affinity and spatially isolated Cu-pyridine active sites for photothermal-driven reforming process of methanol solutions (PTRM). These catalysts exhibit distinct active sites that separately adsorb and activate H 2 O and CH 3 OH, with synergistically photothermal effect leading to an exceptional H 2 evolution activity of 121.1 mmol‧g cat −1 ‧h −1 within 80 min at 210 ℃ and an overall turnover number (TON) of 25904 over 68 hours without significant deactivation, with a high apparent quantum efficiency (AQE) of 54 %. Notably, the activation energy is reduced by 44 % compared to thermal-only systems, and the H 2 production is initiated even at 100 °C. The photothermal H 2 evolution activities of mUiO-67-bpy-CuX correlate with the lability of X counteranions, suggesting open coordination environments of Cu sites generated by labile X groups facilitate Cu + -N intermediate formation upon photoexcitation. Additionally, the Zr 6 nodes and increased mesoporosity in the modulated MOF enhance H 2 O adsorption and dissociation at low temperatures, promoting OH‧ generation. While Cu + -N interfaces are responsible for effective cleavage of the C-H bonds in CH 3 OH. This work highlights the design of MOF-based photothermal catalyst with isolated metal sites for enhanced H 2 production from CH 3 OH/H 2 O reforming at low temperatures.
研究领域:
化学工程
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材料科学
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能源科学
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Qiangyu Zhao,Zhenyuan Zhao,Renzhi Rao,Yang Yang,Songyuan Ling,Fukun Bi,Xiaoyu Shi,Jingcheng Xu,Guang Lu,Xiaodong Zhang
In this paper, a simple solvothermal synthesis method was proposed for the preparation of metal organic framework/graphene oxide hybrid nanocomposite (UiO-67/GO). A series of UiO-67/GO composites were prepared by varying the addition forms and amounts of GO, and the optimal synthesis conditions were screened. The composites were characterized by X-ray diffraction (XRD), Fourier transform infrared (FTIR), transmission Electron Microscope (TEM), scanning electron microscopy (SEM), X-ray photoelectron spectroscopic (XPS), water contact angles (CA) and thermogravimetric analysis (TGA). The adsorption capacity and the adsorption process of toluene were investigated by dynamic adsorption and adsorption kinetics , respectively. The results indicated that 67/GO-0.5% reached the maximum adsorption capacity (876 mg g −1 ), which far exceeded the other adsorbents. Kinetic model and the Weber-Morris model correlated satisfactorily to the experimental data. The improved adsorption performance was attributed to GO, which enhanced π-π interaction, promoted defect generation and provided more adsorption sites. Finally, the excellent regeneration performance of the adsorbent was verified by temperature programmed desorption (TPD) and cyclic adsorption–desorption experiments. Moreover, the adsorption mechanism was further revealed. Combined with the related adsorption experiments and the density functional theory (DFT) analysis, the efficient removal of toluene by UiO-67/GO was attributed to the cooperation of defects, π-π interaction and hydrogen bonding .
研究领域:
材料科学
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环境科学
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DOI
高影响因子
WATER SCIENCE AND TECHNOLOGY
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2022
·Vol. 85
·期 5
·1636-1647
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IF 2.43
Jin Yuning,Wu Danping,Ma Na,Dai Wei
MOFs (metal-organic frameworks) significantly suffer from water- and heat instable issues, restricting their practical application, such as the capture of hazardous anionic dyes (e.g. Congo red, CR) from water. In the present contribution, a series of novel composites (UiO-67@CNTs) composed of microporous UiO-67 (Zr6O4(OH)4(CO2)12) and mesoporous CNTs (carbon nanotubes) have been innovatively synthesized by an in-situ hydrothermal reaction strategy. This UiO-67@CNT impressively retains structural integrity whether contacted with strong acid, distilled water, and strong alkali conditions even for 20 days. Due to the existence of CNT, its heat stability can reach up to 480 °C, which is superior to that of UiO-67. Open Zr(IV) sites, mesoporous, and high surface area in the structure of UiO-67@CNTs play associative effects for CR capture ability. CR uptakes over (5.0)UiO-67@CNTs can reach 1024 mg/g, exceeding some other previous adsorbents in literature. Importantly, UiO-67@CNTs could retain a remarkable CR capture ability even after the fifth cycle. This work expands views for water-heat resistant MOF-based composite with excellent ability of CR capture. UiO-67@CNTs exhibited outstanding hydrolytic stability, retaining intactness for 20 days even in strong acid and alkali. UiO-67@CNTs performed more excellent thermal stability until 480 °C. Novel UiO-67@CNTs have potential applications for CR capture.
研究领域:
环境科学
·
材料科学
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DOI
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
·
2024
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IF 4
Zhiwei Wang,Guangyuan Hu,Changqing Xia,Xinliang Wang,Hongxing He,Zhifeng Nie,Shixing Wang,Weili Li
The recovery and utilization of precious metals from secondary resources are important owing to their pivotal role in modern technology. In this study, we successfully grafted diamine onto UiO-67, modulated its charge and functionalization, and developed a highly efficient adsorbent for the extraction of Au(III) from waste solutions. The recovery rate of UiO-67-(NH 2 ) 2 for trace gold is >99 % in the wide range of pH 3 to 9. The maximum adsorption capacity of UiO-67-(NH 2 ) 2 at a temperature of 298 K is 482 mg/L. In addition, UiO-67-(NH 2 ) 2 exhibits excellent selectivity to Au(III) in mixed metal ion waste solutions. After five cycles of adsorption–desorption experiments, the adsorption efficiency remains above 95 %. The identification of electrostatic interactions, coordination, and reduction as the primary adsorption mechanisms is supported by X-ray photoelectron spectroscopy (XPS) analysis of UiO-67-(NH 2 ) 2 and density functional theory (DFT) calculations.
研究领域:
化学工程
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材料科学
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产品关联
DOI
高影响因子
Journal of Inorganic and Organometallic Polymers and Materials
·
2024
·
IF 3.9
Pei Xiu,Bai Jinchuan,Li Yaming,Kong Xiangbo
In this paper, a luminescent metal-organic framework Tb 3+ @tartaric acid-functionalized Zr-MOF (Tb 3+ @UiO-67-bpy-TA, TA = tartaric acid) was prepared by post-synthetic modification (PSM) and used as a fluorescence sensor for the detection of the pesticide nitenpyram (NTP). The fluorescence sensing experiment verified that Tb 3+ @UiO-67-bpy-TA had exceptional sensitivity and selectivity for NTP detection, and the detection limit was calculated to be as low as 1.28 µM. The mechanism studies indicated that competitive UV absorption, photoinduced electron transfer (PET) and dynamic quenching contributed to the fluorescence quenching process. In addition, the detection of NTP in tap water and Yellow River water samples by the Tb 3+ @UiO-67-bpy-TA were also investigated using standard addition method, and satisfactory recoveries were achieved.
研究领域:
材料科学
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分析化学
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环境科学
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产品关联
DOI
高影响因子
RSC Advances
·
2022
·Vol. 12
·期 11
·6676-6682
·
IF 4.036
Jia Zhang,Xintong Gao,Wenbo Guo,Zengnan Wu,Yilin Yin,Zenghe Li
TiO2 has great potential in photocatalytic degradation of organic pollutants, but poor visible light response and low separation efficiency of photogenerated electron–hole pairs limit its wide applications. In this study, we have successfully prepared TiO2/UiO-67 photocatalyst through an in situ solvothermal method. The degradation rate of aflatoxin B1 (AFB1) is 98.9% in only 80 min, which is superior to the commercial P25, commercial TiO2 and most of reported photocatalysts under visible light irradiation. In addition, the TiO2/UiO-67 photocatalyst showed excellent recyclability. We demonstrated that the enhanced photocatalytic mechanism was owing to the heterojunction between TiO2 and UiO-67, which enhanced effectively the separation photogenerated charge carriers and visible light response. The free radical trapping tests demonstrated that superoxide radicals (˙O2−), holes (h+) and hydroxyl radicals (˙OH) were the main active species and then oxidized AFB1 to some small molecules.
研究领域:
环境科学
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材料科学
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化学工程
·
食品安全
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产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 24
·11337-11345
·
IF 9.931
Wei-Ming Liao,Jian-Hua Zhang,Zheng Wang,Shao-Yun Yin,Mei Pan,Hai-Ping Wang,Cheng-Yong Su
Electron-deficient Ru/Rh half-sandwich units are optoelectronical, stereochemical, and redox and catalytically active in nature. Four different species of these units were designed and successfully incorporated into UiO-67 frameworks by post-synthetic exchange (PSE) method and employed for photocatalytic H2 evolution and CO2 reduction. Among them, the PSE-MOF catalysts containing [M–OH2] (M = Rh or Ru) groups show higher photocatalytic activity than those with [M–Cl], providing a new example of the exploitation of H2O molecules as small ancillary ligands for the construction of Ru/Rh half-sandwich units and subsequent incorporation into MOFs as photocatalytic centers. The application of TEOA (triethanolamine) and DMA (N,N-dimethylaniline) as sacrificial agents leads to different catalytic mechanisms and durations. A long-term hydrogen evolution lasting for 174 h without significant decrease in efficiency was achieved in the RhOH2@UiO-DMA system, showing the advantage of PSE-MOFs as highly stable photocatalytic platforms with superior self-protective properties.
研究领域:
材料科学
·
催化化学
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产品关联
DOI
高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
·
2024
·
IF 3.2
Rui Cao,Xinxin Li,Teng Zhang,Hanxiao Tang,Ying Song,Zhijuan Zhang,Weisheng Feng
The development of metal ion detection probes with high sensitivity and selectivity is of utmost importance for the promotion of public health and environmental sustainability. In this work, a series of ratiometric fluorescent probes (RhB@UiO-67-NH 2 ) were successfully prepared using a one-pot method for the detection of metal ions, particularly As 5+ and Fe 3+ . Notably, the ratiometric fluorescent probe RhB@UiO-67-NH 2 (1:4) demonstrates dual functionality as a Fe 3+ turn-off probe and an As 5+ turn-on probe. The limits of detection (LODs) for As 5+ and Fe 3+ using RhB@UiO-67-NH 2 (1:4) were determined to be 0.521 μM (39.03 ppb) and 0.107 μM (5.97 ppb), respectively, which were the lowest records of reported LMOFs so far. The fluorescence quenching of Fe 3+ can be attributed to various mechanisms such as fluorescence resonance energy transfer (FRET), photoinduced electron transfer (PET), and competitive absorption (CA). Additionally, the fluorescence enhancement of As 5+ is primarily due to absorbance-caused enhancement (ACE) and PET. Moreover, the composite material RhB@UiO-67-NH 2 (1:4) exhibited excellent anti-interference capability and reproducibility for detecting Fe 3+ and As 5+ . The removal efficiency of As 5+ by RhB@UiO-67-NH 2 (1:4) exceeded 50.9 % when the initial concentration of As 5+ was below 20 mg/L. This work presents a valuable reference for future investigations and utilization of As 5+ and Fe 3+ sensing.
研究领域:
分析化学
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环境科学
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材料科学
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产品关联
DOI
高影响因子
TALANTA
·
2016
·
IF 4.035
Lijie Liu,Lian Xia,Chuanxiang Wu,Fengli Qu,Guoliang Li,Zhiwei Sun,Jinmao You
A stable zirconium (Ⅳ)-based metal organic frameworks (UIO-67) material possessing good chemical, thermal and water stability was synthesized and applied as a sorbent for the dispersive solid phase extraction (DSPE) of 8 plant growth regulators (PGRs) in fruit samples. Fluorescence labeling combined with high performance liquid chromatography fluorescence detection (HPLC-FLD), was used to quantify the target analytes. Characterization of the UIO-67 material was performed by X-ray diffraction(XRD) and scanning electron microscopy (SEM). The experimental parameters, such as amount of UIO-67, type and volume of eluting solvent, adsorption and desorption time, were optimized. Under the optimized conditions, good linearity was observed in the range of 10–1000 pmol/mL with R 2 >0.9989. The limits of detection and limits of quantification were in the range of 0.21–0.57 ng/mL and 0.81–1.91 ng/mL, respectively. The intra-day and inter-day precisions (based on the relative standard deviation, n =3) of the PGR derivatives were under 3.1% and 5.3% respectively and the accuracies of the method for the PGRs were in the range from 89.3% to 102.3%. The developed method was successfully applied to analyze PGRs residues in fruit samples. The proposed method is proved to be simple, environment-friendly and inexpensive and it is feasible to directly use UIO-67 as sorbent to extract targets by varying conditions.
研究领域:
分析化学
·
食品科学
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DOI
高影响因子
危险品化学品经营许可证（带存储）