TALANTA
·
2018
·
IF 4.244
Sihua Qian,Li’na Qiao,Wenxiang Xu,Kai Jiang,Yuhui Wang,Hengwei Lin
Antibiotics play important roles in the treatment and prevention of bacterial infections. However, the over-use of antibiotics can lead to a lot of adverse side-effects like nerve damage, anaphylaxis and drug tolerance. Herein, we report an inner filter effect (IFE)-based near-infrared (NIR) fluorescent probe for highly sensitive and selective detection of tetracyclines (TCs) and quinolones (QNs), of which being the most frequently applied antibiotics. NIR emissive carbon-dots (NIR-CDs) that displayed broad excitation range, stable and strong emission were selected as label-free fluorophores. In the presence of TCs or QNs, efficient IFE from CDs to the two types of antibiotics occurred because of the good spectrum overlap between the ultraviolet absorption of TCs/QNs and the excitation of NIR-CDs. As a result, fluorescence emission of the NIR-CDs was obviously quenched, and this builds the foundation of TCs and QNs quantification. The probe provides linear detection ranges, i.e. 1–80 nM and 0.01–0.2 μM for oxytetracycline (OTC, an example for TCs) and norfloxacin (NOR, an example for QNs) with detection limits of 0.5 nM and 6.3 nM, respectively. To the best of our knowledge, this is the first report on NIR fluorescent probe for antibiotics assay. Moreover, the probe has been demonstrated to be very robust, and was successfully adopted for the determination of OTC and NOR in milk samples.
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ACS Applied Nano Materials
·
2019
·
IF 0
Xian Fang,Xiaoyan Chen,Ying Liu,Qiuju Li,Zhongrun Zeng,T. Maiyalagan,Shun Mao
Rapid determination of trace antibiotics is critical for environmental monitoring and the ecosystem. In this study, a sensitive and selective electrochemical sensor for ciprofloxacin (Cip) detection by anodic stripping voltammetry of Cu2+ is designed. Zr(IV)-based metal–organic framework (MOF) NH2–UiO-66 and reduced graphene oxide (RGO) composites are used as working electrodes, which have a large surface area with porous structure and high electrical conductivity. Because Cip can form a stable composite with Cu2+ due to the complexation reaction, the anodic stripping voltammetry method is used for Cip determination with Cu deposition on the NH2–UiO-66/RGO-modified electrode. When Cip is present, the oxidization current of Cu2+ decreases significantly due to the formation of Cu2+–Cip complex. The prepared NH2–UiO-66/RGO sensor can detect trace levels of Cip down to 6.67 nM with a sensitivity of 10.86 μA μM–1, and a linear working range from 0.02 to 1 μM, which is superior to other electrochemical Cip sensors reported previously. The sensor also shows high selectivity, reproducibility, and stability in Cip sensing. Meanwhile, the electrochemical sensor is capable to detect Cip in real water samples with satisfactory recoveries. The ultrasensitivity, rapid detection, and easy operation of the reported sensors present significant potentials for real-time analysis and monitoring of trace antibiotic contaminants in water.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2019
·
IF 2.931
Yang-Zi Ouyang,Hai-Long Wu,Huan Fang,Tong Wang,Xiao-Dong Sun,Yue-Yue Chang,Yu-Jie Ding,Ru-Qin Yu
The matter of fluoroquinolone residues in various foods still arouses wide public concern nowadays. In the present work, the strategy of excitation-emission matrix (EEM) fluorescence data coupled with second-order calibration method based on alternating normalization-weighted error (ANWE) algorithm was used to determine ofloxacin , lomefloxacin and ciprofloxacin in milk powder, milk and beef. Owning the unique “second-order advantage”, the ANWE-assisted analytical method was proved to successfully and eco-friendly resolve the overlapped fluorescence spectra of multi-component in complex food matrixes without tedious pretreatment steps and sophisticated high-cost instrumentations. The feasibility of the proposed method was validated by experiments. The average spiked recoveries of three fluoroquinolones range from 82.6% to 110.5% with relative standard deviations lower than 7.4%, and the limits of detection range from 0.18 and 2.41 ng mL −1 . For further evaluation, analytical figures of merit such as sensitivity and selectivity, as well as the RSDs of intra-day (≦10.6%) and inter-day (≦9.4%) were calculated. The satisfactory analytical results demonstrated that the proposed strategy could be a competitive alternative for simple, rapid and simultaneous determination of multiple fluoroquinolones in animal-derived food samples.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2018
·
IF 3.909
Lin Wang,Yu Du,Yi Yuan,Ruo-Jun Mu,Jingni Gong,Yongsheng Ni,Jie Pang,Chunhua Wu
Intelligent hydrogels are attractive biomaterials for various applications, however, fabricating a hydrogel with both adequate self-healing ability and mechanical properties remains a challenge. Herein, a series of novel intelligent konjac glucomannan (KGM)/microcrystalline cellulose (MCC) hydrogels were prepared vis the mussel-inspired chemistry. MCC was firstly functionalized by the oxidative polymerization of dopamine, and the intelligent hydrogels were obtained by mixing aqueous solutions of KGM and functionalized MCC (PDMCC). By introducing PDMCC, a more compact interconnected porous structure formed for the resulting hydrogels. The self-healing ability and mechanical properties of intelligent hydrogels were dependence on the PDMCC content. Compared with KGM hydrogels, KGM/PDMCC hydrogels exhibited a more distinct pH sensitivity and a lower initial burst release, which was attributed to the compact structure and strong intermolecular hydrogen bond interaction between PDMCC and KGM. These results suggest that the KGM/PDMCC intelligent hydrogels may be promising carriers for controlled drug delivery.
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MICROCHIMICA ACTA
·
2018
·Vol. 185
·期 2
·1-9
·
IF 5.705
Hua Jianhao,Jiao Yang,Wang Meng,Yang Yaling
The authors describe a method for the determination of norfloxacin (NOR) or ciprofloxacin (CIP). It is making use of a combination of fluorescence enhancement and magnetic solid-phase extraction (MSPE). Sulfur-doped carbon dots (S-CDs) are used as a fluorescent probe. They were prepared by a one-pot method using poly(4-styrenesulfonic acid-co-maleic acid) (PSMA) as a source for carbon and sulfur. NOR or CIP act as sensitizers of fluorescence (with excitation/emission maxima at 324/412 nm), probably due to strong hydrogen bond interaction and charge transfer with the S-CDs. The S-CDs were characterized by using TEM, XRD, XPS, FT-IR, UV-Vis and fluorescence spectroscopies. Response is linear in the 0.02–1.25 μM NOR concentration range, and the detection limit is 4.6 nM. The respective data for CIP are 0.02–1.0 μM and 6.7 nM. The average recoveries of NOR and CIP residues from spiked bovine raw milk are 96.2%~105.2% and 92.3%~102.5%.
Sulfur doped carbon dots (S-CDs) were synthesized by a hydrothermal method using poly(4-styrenesulfonic acid-co-maleic acid) (PSMA). Norfloxacin (NOR) or ciprofloxacin (CIP) was extracted by magnetic nanoparticles (MNPs), they were detected by carbon dots fluorescence enhancement.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2018
·Vol. 24
·期 18
·4703-4709
·
IF 5.16
Li'na Qiao,Sihua Qian,Yuhui Wang,Shifeng Yan,Hengwei Lin
Graphical A “lab-on-a-nanoparticle” approach for the detection and discrimination of antibiotics has been developed. The sensing platform is designed on the basis of the different channel's fluorescence recoveries of full-color emissive carbon dots and metal ion ensembles with the addition of antibiotics. Moreover, the proposed method can be successfully employed for the quantitative identification of antibiotic residues in real food samples. Fluorescent carbon dots (CDs) have received considerable attention in recent years due to their superior optical properties. To take further advantages of these unique features, herein, a CDs-based “lab-on-a-nanoparticle” approach for the detection and discrimination of antibiotics is developed. The sensing platform was designed based on the different channel's fluorescence recoveries or further quenching of the full-color emissive CDs (F-CDs) and metal ion ensembles upon the addition of antibiotics. The F-CDs exhibited unusually comparable emission intensity nearly across the entire visible spectrum even as the excitation wavelength is shifted, making it very suitable for the construction of multi-channel sensing systems. The sensing platform was fabricated on the basis of the competing interaction of metal ions with the F-CDs and antibiotics. Three metal ions (i.e., Cu 2+ , Ce 3+ and Eu 3+ ) can efficiently quench the fluorescence of the F-CDs. Upon the addition of antibiotics, the fluorescent intensities either recovered at different emission wavelengths or were further quenched to various degrees. The fluorescence response patterns at different emission wavelength were characteristic for each antibiotic and can be quantitatively differentiated by standard statistical methods (e.g., hierarchical clustering analysis and principal component analysis). Moreover, as an example, the proposed method was applied for quantitative detection of oxytetracycline with a limit of detection to be 0.06 μ m . Finally, the sensing system was successfully employed for residual antibiotics detection and identification in real food samples.
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CHEMICAL ENGINEERING JOURNAL
·
2018
·
IF 6.735
Kiran Gupta,Jiang-Bo Huo,Jia-Cheng E. Yang,Ming-Lai Fu,Baoling Yuan,Zhangxu Chen
We introduced (MoS 4 ) 2− moiety into the lamellar layers of Ca 0.66 Al 0.34 (OH) 2 (NO 3 ) 0.34 ⋅yH 2 O to fabricate Ca 0.66 Al 0.34 (OH) 2 (MoS 4 ) 0.17 ⋅yH 2 O (CA-MoS 4 ⋅LDH), a stable and efficient adsorbent for removal of two envoy Fluoroquinolones (FQs), Ciprofloxacin (CIP) and Ofloxacin (OFL), from contaminated aquatic sources. Various characterization tools, such as X-ray diffraction (XRD), Scanning electron microscopy, Energy dispersive X-ray spectrometer, transmission electron microscopy , X-ray photoelectron spectroscopy (XPS), Fourier transform infrared (FTIR) spectroscopy, Raman spectroscopy and Thermogravimetric analyses etc. were applied to confirm structural and compositional changes during the synthesis and adsorption properties of CA-MoS 4 ⋅LDH. The efficiency of adsorbent was investigated by evaluating different parameters including contact time, pH of solution, initial concentration of pollutant, and effect of temperature. By using CA-MoS 4 ⋅LDH as adsorbent, we found more efficient removal of CIP than that of OFL due to the steric hindrance. The highest uptake of 707.20 mg/g and 476.74 mg/g of CIP and OFL, respectively, was found at pH of 6 with improved kinetics and easily reusability for these representative antibiotics models so far. Removal kinetics of both FQs were found to better follow the pseudo-second-order kinetic model than the pseudo-first-order. The Langmuir adsorption isotherm was employed to understand the removal process, suggesting monolayer chemisorption mechanism. The adsorbate-adsorbent interaction revealed remarkable features originate from the combination of weak hydrogen bond interaction between thio group and NH 2 + group of antibiotic and electrostatic interaction between positive LDH layer and COO − group of antibiotic as well, and anion exchange mechanisms, which were also confirmed by XRD, FTIR, XPS and Raman spectrum etc. obtained after adsorption. It is proposed that all (MoS 4 ) 2− moiety offers stability to the CA-MoS 4 ⋅LDH structure to avoid its solubility under ambient environments.
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BIOSENSORS & BIOELECTRONICS
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2018
·
IF 8.173
Xiaoqiang Liu,Peipei Liu,Yunfei Tang,Liwei Yang,Lele Li,Zhichong Qi,Deliang Li,Danny K.Y. Wong
In this work, a sensitive photoelectrochemical aptasensor was developed for kanamycin detection using an enhanced photocurrent response strategy, which is based on the surface plasmon resonance effect of gold nanoparticles deposited on a 3D TiO 2 -MoS 2 flower-like heterostructure . A significant aspect of this development lies in the photoelectrochemical and morphological features of the unique ternary composite, which have contributed to the excellent performance of the sensor. To develop an aptasensor, mercapto-group modified aptamers were immobilised on the photoactive composite as a recognition unit for kanamycin. The TiO 2 -MoS 2 -AuNP composite was demonstrated to accelerate the electron transfer , increase the loading of aptamers and improve the visible light excitation of the sensor. Under optimal conditions, the aptasensor exhibited a dynamic range from 0.2 nM to 450 nM of kanamycin with a detection limit of 0.05 nM. Overall, we have successfully synergised both the electrical and the optical merits from individual components to form a ternary composite, which was then demonstrated as an effective scaffold for the development of PEC biosensors.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2018
·
IF 11.698
Fengliang Wang,Yiping Feng,Ping Chen,Yingfei Wang,Yuehan Su,Qianxin Zhang,Yongqin Zeng,Zhijie Xie,Haijin Liu,Yang Liu,Wenying Lv,Guoguang Liu
The occurrence of fluoroquinolones (FQs) in the ambient environment has raised serious concerns. In this study, the photocatalytic degradation kinetics and mechanism of ciprofloxacin (CIP) was investigated in ordered mesoporous g-C 3 N 4 (ompg-C 3 N 4 ). Under simulated sunlight irradiation, ompg-C 3 N 4 exhibited a 2.9 fold more rapid reaction for CIP degradation than bulk g-C 3 N 4 . This enhancement may be attributed to the large specific surface area and effective charge separation of ompg-C 3 N 4 . The eradication of CIP followed the Langmuir–Hinshelwood (L–H) kinetics model, and surface reactions played a significant role during the photocatalysis process. Further study of reactive species (RSs) by both ESR technology and RSs scavenging experiments revealed that the superoxide anion radical (O 2 − ) and photohole (h + ) were primarily responsible for the degradation of CIP. Based on the identification of intermediates using liquid chromatography with tandem mass spectrometry (HPLC-MS/MS), and the prediction of reactive sites via Frontier Electron Densities (FEDs), the degradation pathways of CIP were proposed. A comparison of the degradation among FQs revealed that the piperazine moiety showed a dramatic effect on the degradation of FQs during the photocatalysis process. A residual antibiotic activity experiment revealed that ompg-C 3 N 4 provided a very desirable performance for the reduction of antibiotic activity. The sufficient photocatalytic degradation of CIP in ambient water revealed that a sunlight-driven ompg-C 3 N 4 photocatalytic process may be efficiently applied for the remediation of CIP contaminated natural waters.
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CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Jiaxing Huang,Daguang Li,Ruobai Li,Qianxin Zhang,Tiansheng Chen,Haijin Liu,Yang Liu,Wenying Lv,Guoguang Liu
Non-metal doping has been frequently used in g-C 3 N 4 (CN) as a feasible and economical technique for maintaining its metal-free properties, while improving its photocatalytic performance. In this study, a novel phosphorus and oxygen co-doped graphitic carbon nitride (POCN) was successfully synthesized through a one-step thermal polymerization method and exhibited remarkable photocatalytic activity for the photocatalytic degradation of fluoroquinolones (FQs). The degradation rate of enrofloxacin (ENFX) was 6.2 times higher than that of CN. Based on the results of X-ray photoelectron spectroscopy (XPS) and nuclear magnetic resonance spectroscopy (NMR), P atoms replaced the corner and bay carbon sites, whereas O atoms replaced the nitrogen sites in the g-C 3 N 4 framework. The improvement of the photocatalytic effect of POCN0.01 was attributed to its narrow bandgap, effective charge separation and enhanced specific surface area. This is the first report to describe the use of phosphorus doping to promote the generation of reactive oxygen species (ROS). ROS scavenging tests revealed that O 2 − was the primary active species during the degradation of ENFX. Furthermore, pathways for the degradation of ENFX were proposed via the detection of intermediate products via HRAM LC–MS/MS and the prediction of active sites using the Fukui function.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2018
·
IF 4.61
Suyu Ren,Jing Tao,Feng Tan,Ying Cui,Xiaona Li,Jingwen Chen,Xin He,Yi Wang
Diffusive gradients in thin films (DGT) can achieve the time-weighted-average (TWA) concentrations of analytes in the period of deployment. Here we developed an approach based on DGT with a novel binding gel using porous carbon material (PCM) derived from metal-organic framework (MOF) for in-situ measurement of antibiotics in water samples. The diffusion coefficients of 20 antibiotics (nine sulfonamides, ten fluoroquinolones, and trimethoprim) in agarose diffusive gel were 1.41 × 10 −6 cm 2 /s to 4.75 × 10 −6 cm 2 /s at 25 °C. The capacity of PCM binding gel toward the antibiotics was ~100 μg per gel disc. The masses of the antibiotics accumulated by PCM-based DGT increased linearly with time, and they were almost independent of pH (4.2–8.4) and ionic strength (1–500 mM). The performance of the novel DGT was evaluated using freshwater and synthetic seawater spiked with the antibiotics in laboratory. The results showed good agreement with the theoretical predications except sulfacetamide. The detection limits achieved by the DGT with three devices together for deploying up to seven days were 1.0–18.0 ng/L. Field deployment in municipal wastewater treatment plant effluent and seawater showed that the TWA concentrations of antibiotics were 3.8–1342.5 ng/L and 5.6–43.3 ng/L, respectively, which were comparable to those measured by grab sampling. The proposed DGT was an efficient tool for the measurement of antibiotics in environmental waters.
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DALTON TRANSACTIONS
·
2017
·Vol. 47
·期 4
·1284-1293
·
IF 4.029
Yingfei Wang,Fengliang Wang,Yiping Feng,Zhijie Xie,Qianxin Zhang,Xiaoyu Jin,Haijin Liu,Yang Liu,Wenying Lv,Guoguang Liu
The development of facile and efficient synthetic approaches of carbon quantum dots loaded with mesoporous g-C3N4 (mpg-C3N4/CQDs) is of critical urgency. Here, a facile strategy was developed to synthesize the mpg-C3N4/CQDs by using calcinations of the mixture of CQDs, cyanamide, and silica colloid. The obtained composite still retained a considerable total surface area, which could offer a larger population of adsorption sites; therefore enhance the capacity for the adsorption of fluoroquinolones antibiotics (FQs). Under visible light irradiation, mpg-C3N4/CQDs demonstrated a higher photocatalytic activity for FQs degradation than did bulk g-C3N4 or mpg-C3N4. This enhancement might have been ascribed to the high surface area of the mpg-C3N4, unique up-converted photoluminescence (PL) properties, and the efficient charge separation of the CQDs. The eradication of FQs followed the Langmuir–Hinshelwood (L–H) kinetic degradation model and absorption pseudo-second-order kinetic model, indicating that surface reactions and chemical sorption played significant roles during the photocatalysis process. The results of electron spin resonance (ESR) technology and reactive species (RSs) scavenging experiments revealed that the superoxide anion radical (O2˙−) and photo-hole (h+) were the primarily active species that initiated the degradation of FQs. Based on the identification of intermediates and the prediction of reactive sites, the degradation pathways of ofloxacin (OFX) were proposed. A residual antibiotic activity experiment revealed that mpg-C3N4/CQDs provided very desirable performance for the reduction of antibiotic activity.
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