MICROCHIMICA ACTA
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2024
·Vol. 191
·期 3
·1-8
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IF 5.3
Yang Shuning,Tian Li,Song Guanying,Li Huiling,Li Chao,Wu Qian,Shan Xiangyu,Zhao Lun
An electrochemiluminescence (ECL) sensor for determining bisphenol A (BPA) was prepared based on titanium dioxide (TiO 2 ) and Co-MOF. TiO 2 is a co-reaction promoter that amplifies the ECL signal in the Ru(bpy) 3 2+ -trinpropylamine (TPrA) system. When the electrode is modified with Co-MOF the ECL signal is significantly enhanced. This is because Co-MOF can not only be used as a co-reaction accelerator but also as a carrier to adsorb more luminescent substances. Possible mechanisms for amplifying the original signal through the synergistic action of the two substances are investigated. The ECL strength decreases with increasing concentrations of BPA, and the amount of BPA can be determined by the change in ECL signal strength (Δ I ). Under optimal experimental conditions, the linear range of BPA was 2.0 × 10 −10 to 2.0 × 10 −5 M, with a determination limit of 6.7 × 10 −11 M (3 σ / m ). The relative standard deviation (RSD) of the signal for ten consecutive measurements was 1.5%. The sensor can be used to detect BPA in bottled samples with recoveries of 96 to 105%. Graphical
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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电化学
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传感器技术
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2015
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IF 3.368
Xiang Shen,Bing Yan
A series of luminescent Ln 3+ @bio-MOF-1 (Ln = Eu, Tb, bio-MOF-1 = Zn 8 (ad) 4 (BPDC) 6 O⋅2Me 2 NH 2 (ad = adeninate, BPDC = biphenyldicarboxylate)) are synthesized via postsynthetic cation exchange by encapsulating lanthanide ions into an anionic metal–organic framework (MOF), and their photophysical properties are studied. After loading 2-thenoyltrifluroacetone (TTA) as sensitized ligand by a gas diffusion (“ship-in-bottle”) method, it is found that the luminescent intensity of Eu 3+ is enhanced. Especially, when loading two different lanthanide cations into bio-MOF-1, the luminescent color can be tuned to close white (light pink) light output. Additionally, bio-MOF-1 and Eu 3+ @bio-MOF-1 are selected as representative samples for sensing metal ions . When bio-MOF-1 is immersed in the aqueous solutions of different metal ions , it shows highly sensitive sensing for Fe 3+ as well as Eu 3+ @bio-MOF-1 immersed in the DMF solutions of different metal ion. The results are benefit for the further application of functionalized bio-MOFs in practical fields.
研究领域:
无机化学
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材料科学
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分析化学
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纳米生物技术
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光物理学
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配位化学
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BIOSENSORS & BIOELECTRONICS
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2026
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IF 11.8
Yifei Chen,Mengxue Zhu,Zhengyi Chen,Yinjun Tang,Ruimin Li,Haifei Wan,Qie Fang,Wenhong Yang,Wenxuan Jiang,Miao Xu,Canglong Wang,Liuyong Hu,Chengzhou Zhu,Wenling Gu
Organophosphate esters (OPEs) are representative phosphate ester substrates, whose efficient hydrolysis critically depends on cooperative Lewis and Brønsted acid catalysis as observed in natural hydrolases. However, most artificial catalysts primarily emphasize Lewis acidic metal centers while the regulatory role of Brønsted acidity in hydrolysis nanozymes has rarely been systematically investigated or mechanistically validated. Here, we report a hydroxyl-modified metal-organic framework nanozyme (MOF-808-OH), in which the catalytic microenvironment is engineered by introducing hydroxyl groups into the organic linkers of MOF-808 to enhance Brønsted acidity. As a result, MOF-808-OH exhibits a 1.9-fold increase in phosphate ester hydrolysis activity compared with pristine MOF-808. Combined experimental investigations and density functional theory calculations reveal that strengthened Brønsted acid sites facilitate substrate activation and transition-state stabilization during P-O bond cleavage. Benefiting from this enhanced catalytic efficiency, MOF-808-OH enables reliable colorimetric quantification of p -nitrophenyl phosphate ( p -NPP) with a linear range of 5-1000 μg mL −1 and a limit of detection of 2.5 μg mL −1 . Furthermore, the hydrolyzed phosphate can be subsequently captured via Ca 2+ -induced precipitation, offering a feasible route for downstream phosphorus utilization. This work demonstrates the key role of Brønsted acidity in hydrolysis nanozymes, which differs from traditional studies that only focus on Lewis acid sites. The establishment of structure-activity relationship provides a new and transferable design principle for high-performance MOF-based hydrolytic nanozymes.
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ELECTROCHIMICA ACTA
·
2023
·
IF 6.6
Rui Zhao,Huimin Ren,Yubing Si,Gang Li,Yongzhu Fu
Phenyl tetrasulfide (PTS) is a high-capacity cathode material for lithium batteries. However, it also suffers the shuttle effect of polysulfides to the lithium anode in the charge because some lithium polysulfides are still formed due to the middle sulfur atoms in the structure of PTS. The separator modification is considered as a convenient and effective strategy to reduce the shuttle effect. In this report, metal-organic framework (MOF)-801(Ce) is synthesized and coated on a polypropylene separator (MOF-801(Ce)−PP) as a polysulfide barrier. MOF-801(Ce) has a pore size of 6 Å, which is smaller than the sizes of lithium thiophenolate and lithium polysulfides. Therefore, the MOF-801(Ce)−PP can effectively inhibit the migration of active species to the lithium metal anode without affecting the passage of lithium ions. Consequently, the Li/PTS cell with the MOF-801(Ce)−PP exhibits a discharge capacity of 340.8 mAh g −1 at 0.5 C after 250 cycles, which is better than the control cell. Even when the PTS areal mass loading is 5.4 mg cm −2 , the cell with the MOF-801(Ce)−PP can still deliver a high specific capacity of 430 mAh g −1 at 0.5 C rate. This study proves a feasible strategy to overcome the polysulfide shuttle issue of organosulfide cathode materials.
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Sustainable Chemistry and Pharmacy
·
2023
·
IF 6
Qiuyun Zhang,Yanting Lei,Luyan Li,Jiao Lei,Mengmeng Hu,Taoli Deng,Yutao Zhang,Peihua Ma
A novel Bi-based metal-organic framework impregnated phosphomolybdic acid (PMA@Bi-MOF) catalyst has been fabricated via a simple hydrothermal procedure, and successfully applied in the preparation of biodiesel using oleic acid (OA) as the raw material. The PMA@Bi-MOF composites were exhaustively characterized with the help of FTIR , XRD, TPD-NH 3 , SEM-EDX, N 2 -physisorption, TGA , and XPS analyses. Experimental findings showed that the PMA@Bi-BTC exhibited a higher activity than that of PMA@Bi-BDC and Bi-BTC, attributed to its textural property, the presence of more acid sites with higher strength, and synergistic catalytic effects between PMA and Bi-BTC. The optimum conditions for esterification of OA, with a conversion of up to 92.5%, were found to be a molar ratio of methanol to OA of 20:1 and 0.15g PMA@Bi-BTC catalyst at 160 °C in 3 h. Meanwhile, reused studies indicated that the OA conversion reached more than 80% after seven reaction cycles. Furthermore, the activation energy of esterification catalyzed by PMA@Bi-BTC was also calculated as 54.8 kJ/mol. It is expected that our study provides an efficient route to biofuel production involving polyoxometalates/MOF synergistic catalysts.
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CARBON
·
2023
·
IF 10.9
Tianwen Xie,Shuaizhen Li,Lin Ma,Jian Li,Shengyang Pang,Chenglong Hu,Rida Zhao,Sufang Tang
With widespread requirements of electromagnetic wave absorption in 5G era, the advanced wave-absorbing materials with corrosion resistance are urgently required. Herein we have synthesized a bimetallic NiZn-MOF-derived composite with broad electromagnetic wave absorption and strong excellent corrosion resistance using a facile hydrothermal method . Based on the composition modulation of the produced Ni/Ni 3 ZnC 0.7 particles, dense and continuous carbon shell can be formed and eventually encapsulate the particles. The resulting composite has an optimum reflection loss of −56.8 dB at 2.40 mm and an effective absorption bandwidth of 5.9 GHz at 2.34 mm. Besides, it remains stable after 6-month immersion in the corrosive mediums, suggesting its long-term corrosion resistance. This work provides a way to prepare MOF-derived wave absorbing materials with anti-corrosion function.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Haifei An,Weijian Tian,Xin Lu,Huanmei Yuan,Liyun Yang,Hao Zhang,Haoming Shen,Hao Bai
Adsorbents with high adsorption capacity and high selectivity are crucial for carbon capture, utilization and storage (CCUS) technology applied to industrial flue gas to reduce carbon emissions. In this paper, a defect-rich hierarchical porous Mg-MOF-74 was synthesized successfully with MgCl 2 ·6H 2 O used as a metal source considering that the weak coordination of Cl − may interfere with the normal coordination process of metal centers and organic ligands, which causes the formation of crystal defects. Through the analysis of a series of characterizations, ligand deletion of Mg-MOF-74 prepared with MgCl 2 ·6H 2 O was confirmed, and the deleted ligand was estimated to be approximately 20% compared with the traditional Mg-MOF-74 prepared with Mg(NO 3 ) 2 ·6H 2 O, which led to mesopores accounting for 36.9%, and the width of mesopores reached 13.1 nm. Compared with traditional Mg-MOF-74, the adsorption heat of CO 2 at zero load of the defect-rich hierarchical porous Mg-MOF-74 increased from 36 kJ·mol −1 to 46 kJ·mol −1 , and the saturated adsorption capacity of CO 2 under ambient pressure was improved by 15%. Interestingly, the IAST selective adsorption performance of CO 2 /N 2 was increased by 20 times. Compared with the saturated adsorption capacity for traditional Mg-MOF-74, the equivalent adsorption capacity of hierarchical porous Mg-MOF-74 only needs 17 kPa, indicating that it is suitable for carbon capture operation in a real flue environment. Calculations of density functional theory (DFT) confirmed that the active site of the hierarchical porous Mg-MOF-74 has a lower adsorption energy with CO 2 due to the presence of defects, which is regarded to play a key role in improving the CO 2 capture performance.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2023
·
IF 3.8
Jitong Deng,Yongjun Zhang,Xiaopeng Wang,Wei Zhang,Hongjing Han,Haiying Wang,Huimin Yuan,Yanan Zhang,Yanguang Chen
The effective utilization of natural gas resources is a promising option for the implementation of the “dual carbon” strategy. However, the capture of carbon dioxide with relatively lower concentration after the combustion of natural gas is the crucial step. Fortunately, the lattice oxygen is used for chemical cycle conversion of methane to overcome the shortcomings mentioned above. A method was proposed to synthesize perovskite for methane cycle conversion using meatl organic framework as a precursor. Morphology and pore structure of Fe 2 O 3 -LaFeO 3 composite oxides were regulated by precursor synthesis conditions and calcination process. Moreover, the chemical looping conversion performance of methane was evaluated. The results showed that the pure phase precursor of La[Fe(CN) 6 ]·5H 2 O was synthesized with the specific surface area of 23.91 m 2 ·g −1 under the crystallization of 10 h and the pH value of 10.5. Fe 2 O 3 -LaFeO 3 was obtained by controlled calcination of La[Fe(CN) 6 ]·5H 2 O and Fe 2 O 3 with variable mass ratio. The selectivity of CO 2 can reach more than 99% under the optimal parameters of methane chemical looping conversion: m (Fe 2 O 3 ): m (LaFeO 3 ) = 2:1, the reaction temperature is 900 °C, the lattice oxygen conversion is less than 40%. Fe 2 O 3 -LaFeO 3 still has good phase and structure stability after five redox reaction and regeneration cycles.
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CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2023
·Vol. 39
·期 6
·976-984
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IF 3.1
Hou Huipeng,Tang Shanshan,Wang Wei,Liu Miao,Liang Axin,Xie Bingteng,Yi Yue,Luo Aiqin
I n this work, an electrochemical chiral sensor of a nanowire-like chiral metal-organic framework/multiwalled carbon nanotube-chitosan/glassy carbon electrode( D -MOF/MWCNTs-CS/GCE) was proposed for the enantiorecognition of L / D -tryptophan( L / D -Trp). The asymmetrical spatial structure of D -MOF provides the feasibility for the enantiorecognition of Trp enantiomers. Moreover, differential pulse voltammetry(DPV) was carried out to be the detection method and the DPV peak potential difference(Δ E p ) between L -Trp and D -Trp was referred as the index of the enantiorecognition performance. Several parameters, such as mass ratios and drop-coated volume of MWCNTs-CS, drop-coated volume and concentration of D -MOF, pH and detection temperature of D -MOF/MWCNTs-CS/GCE were optimized for the largest Δ E p value. And the molecular dynamics(MD) simulation was used to elucidate the enantiorecognition mechanism. Furthermore, the proportions of D -Trp( D -Trp%) in Trp mixtures were detected in a good linear relationship with the DPV peak potentials( E p ), and the proposed electrochemical chiral sensor exhibited good reproducibility, stability and enantiorecognition ability. Additionally, the proposed electrochemical chiral sensor( D -MOF/MWCNTs-CS/GCE) has a good application prospect in the fields of biomedicine, clinical diagnosis, chemical production, pharmaceuticals safety and so on.
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Frontiers in Bioengineering and Biotechnology
·
2023
·
IF 5.7
Liang Zixing,Li Xiaofeng,Chen Xiaofang,Zhou Jiawei,Li Yanan,Peng Jianhui,Lin Zhousheng,Liu Gai,Zeng Xiancheng,Li Cheng,Hang Lifeng,Li Hailiang
Introduction: Photodynamic therapy (PDT) and photothermal therapy (PTT) are widely used in the treatment of tumors. However, their application in the treatment of clinical tumors is limited by the complexity and irreversible hypoxia environment generated by tumor tissues. To overcome this limitation, a nanoparticle composed of indocyanine green (ICG) and Fe-MOF-5 was developed.Methods: We prepared F-I@FM5 and measured its morphology, particle size, and stability. Its enzyme like ability and optical effect was verified. Then we used MTT, staining and flow cytometry to evaluated the anti-tumor effect on EMT-6 cells in vitro. Finally, the anti-tumor effect in vivo has been studied on EMT-6 tumor bearing mice.Results: For the composite nanoparticle, we confirmed that Fe-MOF-5 has the best nanozyme activity. In addition, it has excellent photothermal conversion efficiency and generates reactive oxygen species (ROS) under near-infrared light irradiation (808 nm). The composite nanoparticle showed good tumor inhibition effect in vitro and in vivo, which was superior to the free ICG or Fe-MOF-5 alone. Besides, there was no obvious cytotoxicity in major organs within the effective therapeutic concentration.Discussion: Fe-MOF-5 has the function of simulating catalase, which can promote the decomposition of excessive H2O2 in the tumor microenvironment and produce oxygen to improve the hypoxic environment. The improvement of tumor hypoxia can enhance the efficacy of PDT and PTT. This research not only provides an efficient and stable anti-tumor nano platform, but also has broad application prospects in the field of tumor therapy, and provides a new idea for the application of MOF as an important carrier material in the field of photodynamic therapy.
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Frontiers in Chemistry
·
2023
·
IF 5.5
Chen Danyang,Zhang Yixuan,Long Wei,Chai Langjie,Myint Thazin Phoone,Zhou Wei,Zhou Ling,Wang Min,Guo Liang
Photodynamic therapy (PDT) is widely used for the treatment of hypertrophic scars in clinical practice. However, the low transdermal delivery of photosensitizers in scar tissue and protective autophagy induced by Photodynamic therapy greatly reduces the therapeutic efficiency. Therefore, it is necessary to deal with these difficulties for overcoming obstacles in Photodynamic therapy treatment. In this study, a photosensitizer with photocatalytic performance was designed and synthesized using innovative MOFs (metal-organic frameworks). Additionally, the MOFs, together with an autophagy inhibitor chloroquine (CQ), was loaded in a high mechanical strength microneedle patch (MNP) for transdermal delivery. With these functionalized MNP, photosensitizers and chloroquine were delivered deep inside hypertrophic scars. Inhibition of autophagy increases the levels of reactive oxygen species (ROS) under high-intensity visible-light irradiation. Multiprong approaches have been used to remove obstacles in Photodynamic therapy and successfully enhance its anti-scarring effect. In vitro experiments indicated that the combined treatment increased the toxicity of hypertrophic scar fibroblasts (HSFs), downregulated the level of collagen type I expression as well as transforming growth factor-β1 (TGF-β1)expression, decreased the autophagy marker protein LC3II/I ratio, increased the expression of P62. In vivo experiments showed that the MNP had good puncture performance, and significant therapeutic effects were observed in the rabbit ear scar model. These results indicate that functionalized MNP has high potential clinical value.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2023
·
IF 8.4
Wen-Ting Li,Jia-Si Wang,Meili Pang,Yue Li,Wen-Juan Ruan
The incorporation of multiple sensing elements to a single sensor has been proposed by our group as an improvement for the array sensing technique with retaining the high selectivity of traditional multi-sensor based sensor array but largely simplifying the analytical operation. How to select reasonable sensing elements to construct the sensor is the key to improve the analytical performance. Herein, we propose a concept to solve this issue, that is, using the components which test different properties of analytes to discriminate them from various aspects. As a proof-of-principle trial, a MOF based composite sensor was designed to analyze tetracycline type antibiotics. The porphyrin-containing main ligand, naphthyl auxiliary ligand and rhodamine B guest were installed to response to the redox property, adsorption affinity and absorption/exchanging capability of the analyte, respectively. Six tetracycline homologous were clearly identified by this sensor, and it also exhibited good quantification performance. This method was successfully applied to the analysis of practical milk sample.
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