JOURNAL OF SEPARATION SCIENCE
·
2020
·Vol. 44
·期 6
·1220-1230
·
IF 2.878
Yuan Wang,Shi-Jun Yin,Cong-Peng Zhao,Guo-Ying Chen,Feng-Qing Yang
In this study, a zirconium terephthalate metal-organic framework-coated magnetic nanoparticle (UiO-66@PA@PEI@Fe 3 O 4 ) was synthesized for the extraction of berberine prior to high-performance liquid chromatography analysis. The phytic acid, which could be grafted onto the magnetic nanoparticle through electrostatic interaction with the abundant amino groups of polyethylenimine, possesses outstanding metal ion coordination ability for the immobilization of metal-organic frameworks UiO-66. The physicochemical properties of the obtained nanoparticle were thoroughly investigated by a series of characterization techniques. Then, the factors that will affect the extraction efficiency and recovery of berberine were investigated. Results indicated that the material had good stability and reusability, and high adsorption capacity (50.01 mg/g) to berberine through single-layer adsorption. In addition, a molecular docking study indicated that the interactions between the material and berberine were mainly π-π stacking and hydrophobic interaction. Finally, the material was successfully applied to the extraction of berberine in Rhizoma Coptidis and Cortex Phellodendri extracts with the recoveries of 76.1% and 71.6%, respectively.
研究领域:
分析化学
·
材料科学
·
药学
✓ 已验证
DOI
PubMed
高影响因子
FOOD CHEMISTRY
·
2020
·
IF 6.306
Hai-Long Jiang,Na Li,Xia Wang,Xiang-Yu Wei,Ru-Song Zhao,Jin-Ming Lin
A zirconium-based metal-organic framework material (UiO-66-OH) was designed and applied for the first time as an adsorbent in food analysis for the solid phase microextraction of trace polybrominated diphenyl ethers (PBDEs) from milk. The materials were characterized by powder X-ray diffraction, scanning electron microscopy, Fourier transform infrared spectroscopy, and thermogravimetric analyses. Through response surface methodology, the optimal conditions for adsorption were determined to as follows: extraction time of 30 min, ionic strength of 15%, extraction temperature of 61 °C, and stirring speed of 880 r/min. Under the optimal conditions, the method showed excellent linearity with a high correlation coefficient ( r ≥ 0.9994), low limits of detection in the range of 0.15–0.35 ng L −1 , good interday precision ranging of 7.58%-9.48%, and satisfactory recoveries of 74.7%-118.0%. All these findings showed that the method was reliable and effective for detecting trace PBDEs in milk.
研究领域:
食品分析
·
环境化学
·
材料科学
✓ 已验证
DOI
高影响因子
INORGANIC CHEMISTRY
·
2025
·
IF 4.7
Hong-Bin Luo,Zhi-Xing Han,Kai-Xin Zhao,Xin-Ru Wu,Wei-Jie Cai,Yangyang Liu,Xiao-Ming Ren
Organophosphorus nerve agents are among the most hazardous chemical warfare agents, posing serious risks to human health. Developing efficient catalysts and composite materials for their detoxification remains a significant challenge. In this study, we present the first example of zirconium oxide (ZrOx) nanozyme derived from a zirconium-based metal–organic framework (Zr-MOF), which exhibits outstanding catalytic activity for the hydrolysis of a nerve agent simulant, dimethyl-4-nitrophenyl phosphate (DMNP). Moreover, ZrOx was incorporated into a poly(vinyl alcohol) (PVA) matrix with 1,4-diazabicyclo[2.2.2]octane (dabco) as a base, forming a hydrogel composite membrane, named ZrOx@PD. Notably, ZrOx@PD demonstrates superior catalytic efficiency for the solid-phase hydrolysis of DMNP under ambient conditions, outperforming many previously reported catalytic materials and highlighting its potential as a protective material against nerve agents.
研究领域:
材料科学
·
生物化学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2024
·
IF 4.9
Ping Tan,Niling Zou,Jiakang Sun,Liangjun Long,Yuhan Li,Jiayuan Yu
Zirconium-based Metal-Organic Frameworks (Zr-MOFs) have attracted significant attention for phosphate removal due to their large specific surface area and abundant active sites. In this study, amino-modified Zr-MOFs were synthesized and used for phosphate removal, with a focus on investigating the relationship between the physicochemical structure of the amino-modified Zr-MOFs and phosphate adsorption, as well as the role of the amino groups. A series of amino-modified Zr-MOFs (UiO-67) were synthesized and characterized, with particular emphasis on the variant with one amino group functionalization on a defect-rich framework, designated as DUN. The results reveal that amino modification of defective UiO-67 (DUN) increases the number of phosphate adsorption sites per unit mass and specific surface area, thereby enhancing phosphate adsorption capacity, which is significantly higher than that of other synthesized UiO-67 variants. The role of amino group not only enhances the affinity for phosphate and the adsorption efficiency at low phosphate concentrations but also accelerates the phosphate adsorption rate. Through comprehensive characterization and DFT simulations, the superior performance of DUN is primarily attributed to the synergistic effects of its structural defects, carboxyl groups, and introduced amino functionalities. The defects at Zr nodes in DUN contribute significantly to phosphate adsorption by providing Zr-OH groups and oxygen vacancies. Concurrently, the carboxyl groups present in the DUN's ligand linkers engage in hydrogen bonding interactions with phosphate. The amino groups, a novel addition to the DUN structure, not only provide additional adsorption sites but also significantly enhance the strength of the existing hydrogen bonds and the Zr-O-P coordination interactions. This study sheds light on the intricate relationship between the physicochemical structure of Zr-MOFs and their phosphate adsorption capacity, providing a theoretical basis and practical approach for developing efficient Zr-MOF-based adsorbents for water purification.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ADSORPTION SCIENCE & TECHNOLOGY
·
2024
·
IF 2.8
Yinghao Zhuang,Shuai Sun,Kai Jia,Lei Shi,Xiangshan Yang
Thorium is a promising nuclear fuel; however, even a small amount in nuclear wastewater can cause significant radioactive pollution. Therefore, it is urgent to develop effective adsorbents for the efficient removal of thorium to solve this problem. Herein, the phytic acid modification of carboxylated Zirconium-based metal-organic framework materials (UiO-66-COOH-PA) has been obtained by rapid high-temperature carbonization, which exhibits excellent performance in removing thorium (IV) in acidic aqueous solutions. The maximum adsorption capacity of UiO-66-COOH-PA-2 (with 40% mass ratio of phytic acid) in solution reaches 315.5 mg/g at a pH of 4, which is more than twice that of the unmodified Zr-based metal organic framework (MOF) material. The adsorption kinetics of UiO-66-COOH-PA on thorium has been analyzed using two different isothermal adsorption models, the Langmuir and Freundlich isotherm adsorption models. It turns out that the Freundlich model is more suitable for the data. The thorium adsorption process reaches dynamic equilibrium very quickly, while the adsorption dynamics of UiO-66-COOH-PA on thorium follows the pseudo-second-order adsorption kinetic model. The excellent adsorption performance of UiO-66-COOH-PA-2 at low pH values indicates that adsorption material containing phosphorus is suitable for the removal of thorium especially in acidic systems. It also exhibits excellent selectivity (up to 90.2%) for Th(IV) adsorption in the presence of several coexisting rare-earth ions. Overall, the integration of phosphorus-modified in Zr-MOFs represents a significant advancement in thorium adsorption technology, offering a pathway toward more effective management of radioactive acidic waste liquid.
研究领域:
环境科学
·
核化学
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Qiyue Zhao,Hong-Man Hou,Gong-Liang Zhang,Hongshun Hao,Bei-wei Zhu,Jingran Bi
The platform of isostructural crystalline metal-organic frameworks (MOFs) with structural defects and additional pores is an emerging technology for rapidly removing hazardous small molecules. Herein, this paper designed a series of Zr-based MOFs (UiO-66) with different mesopore ratios by inducing linker/cluster missing through monocarboxylic acid modulators; besides their adsorption capacity and mechanism for heterocyclic aromatic amines (HAAs) were investigated. The UiO-66 defected with lauric acid (UiO-66-12A) showed the best adsorption performance and its adsorption capacity and rate for HAAs were 1.25–5.63 and 1.74–5.82 times higher than UiO-66, respectively. The zeta potentials of adsorbents in the presence of HAAs aqueous solutions underscore the pivotal role of electrostatic interactions during adsorption. Fourier Transform Infrared (FT-IR) and X-ray photoelectron spectroscopy (XPS) demonstrated that π-π stacking, coordination and hydrogen bonding interactions were also critical factors in promoting adsorption. Moreover, simulation calculations revealed that UiO-66 with missing clusters can provide more active sites and stronger interactions. These findings provided a novel and feasible strategy for the rapid removal of hazardous small molecules from complex food environments, which could improve the adsorption capacity and convenient processes of MOFs through building appropriate inherent microporous structures. The comprehensive and systematic understanding of the adsorption mechanism in this paper is conducive to the future advancement of nanomaterials.
研究领域:
材料科学
·
环境科学
·
食品科学
✓ 已验证
产品关联
DOI
高影响因子
Nanomaterials
·
2018
·Vol. 8
·期 9
·655
·
IF 3.504
Xue-Qing Zhan,Fang-Chang Tsai,Lei Xie,Ke-Deng Zhang,Huan-Li Liu,Ning Ma,Dean Shi,Tao Jiang
Isostructural zirconium-based metal–organic frameworks (Zr-MOFs) have attracted the attention of researchers because of their remarkable stability at high temperatures and high pressures and their chemical stabilities against acids and bases. Due to this stability, Zr-MOFs can be utilized in adsorption research, and the adsorption performance of a Zr-MOF depends on the pore size and the surroundings of the MOF. In this study, as the dimensions changed and the adsorption was carried out, the Zr-MOF material remained stable, and the adsorption of the best state was achieved at 235 mg/g. Through the simulation of theoretical kinetic models of Zr-MOFs, we initially postulated that the adsorption capacity is proportional to the pore size and that acid orange 7 (AO7) was adsorbed by the MOFs. Afterwards, we verified our hypotheses through a series of Brunauer–Emmett–Teller (BET) data analysis; non-local density function theory (NLDFT) was mainly used to analyze the data. Moreover, we determined that physical adsorption occurs on the surface of the MOFs during the adsorption process, while chemisorption occurs in the form of dye molecules combining with active sites. Ultimately, we concluded that the larger the pore size, the stronger the adsorption capacity, and this contribution casts a new light on the issue of wastewater treatment.Keywords:Zr-MOF;adsorption;dye;NLDFT;BET
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INORGANIC CHEMISTRY
·
2018
·
IF 4.7
Yingfan Zhang,Bo Gui,Rufan Chen,Guiping Hu,Yi Meng,Daqiang Yuan,Matthias Zeller,Cheng Wang
Metal–organic frameworks (MOFs) assembled from linkers of identical length but with different functional groups have gained increasing interests recently. However, it is very challenging for precise control of the ratios of different functionalities. Herein, we reported a stable azide- and alkyne-appended Zr-MOF that can undergo quantitative tandem click reactions on the different functional sites, thus providing a unique platform for quantitative loading of bifunctional moieties. As an added advantage, the same MOF product can be obtained via two independent routes. The method is versatile and can tolerate a wide variety of functional groups, and furthermore, a heterogeneous acid–base MOF organocatalyst was synthesized by tandemly introducing both acidic and basic groups onto the predesigned pore surface. The presented strategy provides a general way toward the construction of bifunctional MOFs with a precise control of ratio of different functionalities for desirable applications in future.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2021
·Vol. 31
·期 42
·2104629
·
IF 18.808
Li Xin,Dezhu Zhang,Kai Qu,Yuqin Lu,Yixing Wang,Kang Huang,Zhaohui Wang,Wanqin Jin,Zhi Xu
Membrane with ordered channels is the key to controlling ion sieving and proton conductivity in flow batteries. However, it remains a great challenge for finely controlling the nanochannels of polymeric membranes. Herein, two types of acid-stable Zr-metal organic framework (MOF-801 and MOF-808) with variable pore structures and channel properties are introduced as fillers into a non-fluorinated sulfonated poly (ether ether ketone) (SPEEK). The membrane incorporated with MOF-801 of a smaller triangular window (≈3.5 Å) successfully translates the molecular sieving property into the flow battery membrane, resulting in enhanced coulombic efficiency (98.5–99.2%) at 40–120 mA cm −2 compared with the pristine SPEEK membrane (97.1–98.5%). In contrast, more protophilic internal interconnected channels of MOF-808 yield faster proton highway, leading to a significant increase of voltage efficiency (93.7–84.1%) at 40–120 mA cm −2 compared with the pristine SPEEK membrane (91.7–78.9%). By regulating the ion sieving and proton conductivity, MOF-801/MOF-808 binary composite membrane exhibits synchronously improved performance in the vanadium redox flow battery system. The revealed structure–property relationship in the Zr-MOFs-based membranes provides a general guideline to design new proton exchange membranes with ordered channels for flow battery application.
研究领域:
材料科学
·
化学工程
·
能源技术
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Zhonghui Zhang,Bolun Yang,Yue Wu,Wenxiang Zhang,Heping Ma
The efficient capture of SO 2 after the combustion of fossil fuels is of great challenge as the low SO 2 concentration (<500 ppm) and coexisting with CO 2 , water, O 2 in flue gas . Robust zirconium-based MOFs possessing accessible polar sites usually have high SO 2 adsorption capacity but poor durably in adsorption desulfurization due to the acidic sulfate deposition on the Zr-O cluster. Herein, a Zr-O cluster post-modification method was introduced in a Zr-MOF (MOF-808) to form EDTA-MOF-808 (EDTA, ethylene diaminetetraacetic acid) for selective and durable removal of SO 2 . The introduction of EDTA not only improve their SO 2 adsorption capacity, but also sharply increase their SO 2 /CO 2 selectivity (57.2 vs 8.9) and SO 2 /N 2 selectivity (1915.8 vs 292.7) at low SO 2 partial pressure. Moreover, the synergistic effects of dipole and hydrogen bonding interaction between SO 2 and EDTA in EDTA-MOF-808 make the capture of SO 2 in a reversible manner, which can prevent the formation of S(VI) species in Zr-MOF. DFT calculation confirmed that SO 2 was interacted with EDTA through moderate dipole–dipole interaction (S(SO 2 ) with N(EDTA)) and hydrogen bonds (H(–COOH) with O(SO 2 )). Systematic investigations including thermodynamic SO 2 adsorption, dynamic breakthrough experiments, stability tests and DFT-calculations in both MOF-808 and EDTA-MOF-808 confirmed the efficient performance of post modification of Zr-O clusters with EDTA in Zr-MOFs for durable SO 2 capture.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Feipan Liang,Zhiyong Nie,Yuzheng Xia,Yutian Yan,Xiaonong Chen,Bo Liu,Lei Lei,Shuxian Shi
The usage of organophosphate esters as pesticides or nerve agents in chemical warfare caused vital environmental and safety issues. Although metal organic frameworks (MOFs) are often applied to remove the organophosphate esters by adsorption and catalytic degradation, a basic environment with N -ethylmorpholine buffer is essential. In this study, four kinds of zirconium-based MOFs (Zr-MOFs), labeled UiO-66, UiO-67, UiO-67-NH 2 , and UiO-67-2NH 2 , were prepared by the solvothermal method to decontaminate aqueous solutions containing organophosphate esters of paraoxon (POX) and sarin (a nerve agent) without adding any additional basic buffer. Effects of MOF/POX mass ratio and temperature on degradation kinetics and efficiency were investigated in detail. A possible mechanism for the POX decontamination by Zr-MOFs was proposed and verified. Results showed that the POX decontamination catalyzed by Zr-MOFs was a pseudo-first-order reaction. The introduction of amino groups in Zr-MOFs could increase the decontamination rate, which follows the order of “UiO-67-2NH 2 > UiO-67-NH 2 > UiO-67 > UiO-66”. The half-lives of POX and sarin with UiO-67-2NH 2 were 18 min and 5 min respectively, and more than 90% POX and 99% sarin could be decontaminated at room temperature. Compared with previous similar studies on POX degradation in N -ethylmorpholine buffer, UiO-67-2NH 2 performs significantly better in terms of catalytic efficiency and environment. This work would broaden the application scope for the decontamination of aqueous solutions containing organophosphate esters under mild conditions, and offer an effective approach for the treatment of chemical warfare agents in modern society.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
Chemosensors
·
2023
·Vol. 11
·期 8
·451
·
IF 4.2
Longsheng Jin,Huihui Yu,Weishuai Liu,Ziying Xiao,Haijian Yang,Bing Jin,Meisheng Wu
Fumonisin B1(FB1) is a toxin produced by the metabolism of Fusarium oxysporum, which can cause serious effects on the nervous, respiratory, digestive, and reproductive systems of humans or animals; it is known as one of the highly toxic epidemic contaminants. Herein, we report the visual inspection of FB1using bipolar electrodes (BPEs) with an array-based electrochemiluminescence (ECL) platform. The sensor consists of a PDMS cover and a glass substrate containing an array of 10 ITO electrodes. A specific sensing interface was constructed on the cathode of the BPE, which could modulate the ECL reactions that occurred at the anode of BPEs. To amplify the ECL signal, methylene blue (MB)-encapsulated Zr-MOFs (MB@Zr-MOFs) were synthesized and immobilized on the cathode of the BPE, which could amplify the ECL signal at the anode. By coupling the cyclic amplification effect of the DNA walker and nicking endonuclease (Nb.BbvCI), the biosensor can realize the visual measurement of FB1in the range of 5 × 10−5~0.5 ng/mL. In addition, the developed biosensor was used to monitor the concentration of FB1in maize and peanut samples. The recoveries were in the range of 99.2%~110.6%, which demonstrated the good accuracy of the designed BPE-ECL biosensor for FB1assay in food samples.Keywords:fumonisin B1;bipolar electrode-electrochemiluminescence;visualization;Zr-MOFs
研究领域:
食品科学
·
分析化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）