JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2022
·Vol. 169
·期 2
·027504
·
IF 4.386
Zaiqiong Liu,Jinpeng Tao,Zhenyu Zhu,Yanli Zhang,Hongbin Wang,Pengfei Pang,Haibo Wang,Wenrong Yang
An ultrasensitive electrochemical assay for T4 polynucleotide kinase (T4 PNK) activity and inhibition was developed based on magnetic Fe3O4@TiO2 core–shell nanoparticles and gold nanoparticles hybrid probe (Fe3O4@TiO2-dsDNA-AuNPs) modified magnetic gold electrode (MGE). Fe3O4@TiO2-dsDNA-AuNPs hybrid probe was formed via DNA hybridization between phosphorylated DNA S1 modified Fe3O4@TiO2 and complementary DNA S2 assembled AuNPs. [Ru(NH3)6]3+ was used as an electrochemically active indicator to enhance the electrochemical signal. The proposed method is sensitive for T4 PNK activity assay with a linear range of 0.0001 to 10 U ml−1 and low detection limit of 0.00003 U ml−1. This strategy can be used to screen the T4 PNK inhibitors, holding a great potential for discovery of nucleotide kinase-target drug and early clinical diagnosis of cancer.
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ACS Applied Nano Materials
·
2022
·
IF 6.14
Hongzhi Lu,Shoufang Xu
Nanoparticles are effective tools for signal amplification in chemical sensor construction. Herein, we present molecularly imprinted polymer (MIP)-based sandwich-structured fluorescence sensors for ultrasensitive detection of trace carcinoembryonic antigen (CEA) based on MnO2 nanosheet and MoS2 nanoflower dual signal amplification. MIPs were used as synthetic antibodies and prepared by a surface imprinting method using MnO2 nanosheet-loaded magnetic carbon fibers (CF/Fe3O4/MnO2) as solid supports by the self-polymerization of dopamine. The obtained CF/Fe3O4/MnO2/MIPs can specifically absorb the target CEA from complex samples, which can then be specifically labeled with boronic acid-modified MoS2-curcumin nanotags (BA-MoS2-CUR). Under alkaline conditions, CUR was detached from MoS2 and used as a fluorescence reporter molecule. Due to the high binding capacity of the MnO2 nanosheets and the high loading capacity of the MoS2 nanoflowers, the detection sensitivity of the molecularly imprinted fluorescence sensors was remarkably improved. Specific detection of CEA in the linear range of 0.01 ng/mL–10 μg/mL with a low LOD of 3.5 pg/mL (S/N = 3) was achieved. In addition, based on the MIPs and boronic affinity dual specific recognition ability, the detection selectivity was also improved. Finally, the concentration of CEA in human serum was determined by this approach.
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TALANTA
·
2023
·
IF 6.1
Zichen Yang,Guoqing Chen,Chaoqun Ma,Jiao Gu,Chun Zhu,Lei Li,Hui Gao
Quinolone antibiotics have good antibacterial properties and are commonly used antibiotics in the dairy industry. Currently, the problem of excessive antibiotics in dairy products is very serious. As an ultra-sensitive detection technology, Surface-Enhanced Raman Scattering (SERS) was applied to the detection of quinolone antibiotics in this work. In order to classify and quantify three antibiotics (Ciprofloxacin, Norfloxacin, Levofloxacin) with highly similar molecular structures, a combination of magnetic COF-based SERS substrate and machine learning algorithms (PCA-k-NN, PCA-SVM, PCA-Decision Tree) was used. The classification accuracy of the spectral dataset could reach 100% and the results of LOD calculation were: CIP: 5.61 × 10 −9 M, LEV: 1.44 × 10 −8 M, NFX: 1.56 × 10 −8 M. This provides a new method for the detection of antibiotics in dairy products.
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NANOTECHNOLOGY
·
2021
·Vol. 33
·期 9
·095601
·
IF 3.874
Lulu Yu,Min Liu,Yanling Zhang,Yun Ni,Shaobo Wu,Ruijiang Liu
A magnetically induced self-assembly DNAzyme electrochemical biosensor based on gold-modified α-Fe2O3/Fe3O4 heterogeneous nanoparticles was successfully fabricated to detect Nickel(II) (Ni2+). The phase composition and magnetic properties of α-Fe2O3/Fe3O4 heterogeneous nanoparticles controllably prepared by the citric acid (CA) sol–gel method were investigated in detail. The α-Fe2O3/Fe3O4 heterogeneous nanoparticles were modified by using trisodium citrate as reducing agent, and the magnetically induced self-assembly α-Fe2O3/Fe3O4–Au nanocomposites were obtained. The designed Ni2+-dependent DNAzyme consisted of the catalytic chain modified with the thiol group (S1-SH) and the substrate chain modified with methylene blue (S2-MB). The MGCE/α-Fe2O3/Fe3O4–Au/S1/BSA/S2 electrochemical sensing platform was constructed and differential pulse voltammetry was applied for electrochemical detection. Under the optimum experimental parameters, the detection range of the biosensor was 100 pM–10 μM (R2 = 0.9978) with the limit of detection of 55 pM. The biosensor had high selectivity, acceptable stability, and reproducibility (RSD = 4.03%).
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Xu Shi,Peidong Hong,Hongqi Huang,Dandan Yang,Kaisheng Zhang,Junyong He,Yulian Li,Zijian Wu,Chao Xie,Jinhuai Liu,Lingtao Kong
Fenton-like catalysts have usually superior catalytic activities, however, some drawbacks of ion leaching and difficult-to-recovery limit their applications. In this work, a hierarchical porous Fe 3 O 4 /Co 3 S 4 catalyst was fabricated via a simple phase change reaction to overcome these shortcomings. The introduced iron cooperates with cobalt achieving high-efficiency activation of peroxymonosulfate (PMS) to eliminate Rhodamine B (RhB). The results showed that 0.05 g/L Fe 3 O 4 /Co 3 S 4 and 1 mM PMS could quickly remove 100% of 200 mg/L RhB within 20 min, and the removal rate of RhB remained above 82% after 5 cycles. Moreover, the as-prepared Fe 3 O 4 /Co 3 S 4 possessed a great magnetic separation capacity and good stability of low metal leaching dose. Radical quenching experiments and electron paramagnetic resonance (EPR) techniques proved that sulfate radicals (SO 4 •− ) were the dominant reactive oxygen species responding for RhB degradation. X-ray photoelectron spectroscopy (XPS) pointed out that the synergism of sulfur promoted the cycling of Co 3+ /Co 2+ and Fe 3+ /Fe 2+ , boosting the electron transfer between Fe 3 O 4 /Co 3 S 4 and PMS. Moreover, the degradation pathways of RhB were deduced by combining liquid chromatography-mass spectrometry (LC-MS) analysis and density functional theory (DFT) calculations. The toxicities of RhB and its intermediates were evaluated as well, which provided significant assistance in the exploration of their ecological risks.
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APPLIED BIOCHEMISTRY AND BIOTECHNOLOGY
·
2017
·Vol. 183
·期 3
·1035-1048
·
IF 1.751
Zhang Li-Shuang,Fang Yue,Zhou Ying,Ye Bang-Ce
Protocatechuate 3,4-dioxygenase (P34O), which is isolated from Rhizobium sp. LMB-1, catalyzes the ring cleavage step in the metabolism of aromatic compounds, and has great potential for environmental bioremediation. However, its structure is very sensitive to different environmental factors, which weaken its activity. Immobilization of the enzyme can improve its stability, allow reusability, and reduce operation costs. In this work, the relative molecular mass of the native P34O enzyme was determined to be 500 kDa by gel filtration chromatography on Sephadex G-200, and the enzyme was immobilized onto (3-aminopropyl) triethoxysilane-modified Fe 3 O 4 nanoparticles (NPs) by the glutaraldehyde method. The optimum pH of immobilized and free P34O was unaffected, but the optimum temperature of immobilized P34O increased from 60 to 70 °C, and the thermal stability of immobilized P34O was better than that of the free enzyme and showed higher enzymatic activity at 60 and 70 °C. In addition, with the exception of Fe 3+ , most metal ions and organic chemicals could not improve the activity of free and immobilized P34O. The kinetic parameters of the immobilized P34O were higher than those of the free enzyme, and immobilized P34O on Fe 3 O 4 NPs could be reused ten times without a remarkable decrease in enzymatic activity.
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CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Yihan Wu,Biyun Li,Xiangxue Wang,Shujun Yu,Hongwei Pang,Yue Liu,Xiaoyan Liu,Xiangke Wang
The water stable core-shell microspheres (Fe 3 O 4 @ZIF-8) with strong magnetism were successfully fabricated through a facile modification strategy. Concrete procedures included firstly pretreatment of Fe 3 O 4 core with anionic polyelectrolyte to acquire negatively charged Fe 3 O 4 particle surface, followed by nucleation through attracting Zn 2+ cation, and then growth of a thin layer of ZIF-8 (~25 nm). Various characterization techniques (SEM, TEM, FT-IR, XRD, VSM, BET and XPS) indicated that the Fe 3 O 4 @ZIF-8 microspheres were highly stable and magnetic with a large specific surface area (606.91 m 2 /g) and fairly sufficient functional groups ( NH , OH, COOH, Zn O, N O and C N ). Multi-factors affecting the radionuclides removal performance on Fe 3 O 4 @ZIF-8 was adequately explored, comprising contact time, temperature, pH, ionic strength, co-existing ions and extreme conditions. And the results showed that Fe 3 O 4 @ZIF-8 exhibited fast reaction kinetics (~30 min to achieve equilibrium), excellent uptake capabilities (539.7 mg U/g and 255.6 mg Eu/g), remarkable selectivity and favorable physicochemical stability. These researches suggested that Fe 3 O 4 @ZIF-8 could not only simultaneously achieve favorable stability and functionality, but also easily to be separated by external magnetic field after used in radioactive sewage treatment, which was of considerable practical utility in extracting radioactive wastes though in harsh circumstance.
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MICROCHEMICAL JOURNAL
·
2023
·
IF 4.8
Peifang Chen,Caiyun Jiang,Zhouping Wang,Hong-zhen Lian,Xiaoyuan Ma
As a virulent metabolite, aflatoxin B 1 (AFB 1 ) presented in various cereal grain is tightly implicated in severe human diseases. In this study, 3D plasmonic nanohybirds of Raman molecule 4-mercaptobenzoic acid (4-MBA)-embedded and AFB 1 aptamer-modified bimetallic nanostars as SERS probes bound to magnetic nanoflowers were fabricated and demonstrated as a high-performance SERS-active aptasensor to quantitatively analyze AFB 1 . Bimetallic Au@Ag SERS plasmonic nanoprobes with enhanced properties were capable of enhancing discriminative Raman peaks of 4-MBA. Then, the integration of iron tetroxide nanoparticles (Fe 3 O 4 NPs) and molybdenum disulfide nanosheets (MoS 2 NShs) with huge specific surface area constituted stable 3D Fe 3 O 4 @MoS 2 plasmonic nanoflowers, facilitating the bind of numerous aptamer-based SERS probes via the non-covalent interaction between MoS 2 NShs and aptamer, which were ideal candidates for SERS-active substrates. Additionally, Fe 3 O 4 NPs as magnetic core endowed 3D nanocomposites with specific magnetic separation characteristic that caused the collected SERS hotspots to exhibit superior signal response, and further strengthening the sensitivity in a complex food matrix. Aptamer-target AFB 1 specific recognition triggered linearly diminished 4-MBA signal intensity (I 4-MBA ) on the substrate to achieve a low detection limit of 58.9 pg/mL. Furthermore, the sensor has the potential to be a promising monitoring tool for other trace contaminants.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Tianyue Su,Chun Cai
Heterogeneous catalysts have recently regarded as a promising chose for the thermally-driven generation of the reactive oxygen species (ROS) through catalytic reactions with molecular oxygen , which can facilitate this process by specific geometric and electronic structure. However, the oxidative trifluoromethylation of alkenes to α-trifluoromethylated ketones by CF 3 SO 2 Na is rarely reported in this system. In this work, we report a one-pot polymerization ball milling strategy to construct precursor, and then pyrolyze it to obtain specific carbon nanotubes matrix with Fe/Fe 3 O 4 nanoparticles and single atoms Fe. Remarkably, the optimized catalyst (Fe 3 O 4 -Fe SAs - NPs @NC-1) displays excellent catalytic performance, broad substrates and recyclability for this fluorination reaction via radical pathway. Based on characterizations and mechanistic studies , we discover that the coexistence of Fe/Fe 3 O 4 and Fe-N x not only synergistically facilitates the catalytic efficiency in altering the electronic structure of Fe sites, but also benefits the absorption of O 2 and the ability of the thermally-driven generating ROS which can activate CF 3 SO 2 Na to CF 3 radical. This work offers a method of designing Fe-based catalysts and also opens up a new thermal-heterogeneous catalysis way for the oxidative trifluoromethylation of alkenes .
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2023
·
IF 8.7
Zhengjie Peng,Shikai Li,Hao He,Yujiao Wen,Haolong Huang,Lezhu Su,Zhigang Yi,Xing Peng,Nan Zhou
Advanced oxidation processes (AOPs), based on sulfate radical (SO 4 ·- ) produced by peroxymonosulfate (PMS), can effectively mineralize refractory organic pollutants. However, the coexistence of anions and natural organic matters in actual wastewater prevents the application of AOPs. A simple one-step method was used to prepare FeS/Fe 3 O 4 co-modified biochar materials (FFB) that could activate PMS to degrade quinclorac (QNC) with a removal rate of 100%, even exhibiting optimum degradation of QNC reached 99.31% in irrigation water, demonstrating excellent anti-interference performance for co-existing anions and natural organic matter. Meanwhile, ecotoxicity analysis showed that the toxicity of degradation intermediates was lower than that of QNC. Characterization results demonstrated the even distribution of FeS and Fe 3 O 4 onto biochar, supplying abundant Fe 2+ to activate PMS producing reactive oxygen species (ROS), while the generated Fe 3+ after reactive continue to be reduced with sulfur species to promote the cycle of Fe 2+ /Fe 3+ . The coexistence of ·OH, SO 4 ·- , 1 O 2, and O 2 ·- in the FFB/PMS-QNC system suggest the possession of two pathway with free radical and non-free radical pathways to degrade QNC. The density functional theory (DFT) was used to analyze the adsorption sites and adsorption energy of PMS, as well as the differential charge density, which further proved the generation of SO 4 ·- , O 2 ·- and 1 O 2 . In addition, the electrochemical test results showed that electron transfer also played an important role in the degradation of QNC. This study provides a feasible approach for the removal of organic pollutants in actual water.
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RADIATION PHYSICS AND CHEMISTRY
·
2023
·
IF 2.9
Shizong Wang,Jianlong Wang
This study firstly reported the in-situ preparation of nitrogen-doped graphene oxide-supported nano Fe 3 O 4 (Fe 3 O 4 @NRGO) by ionizing radiation . The conversion of Fe(II) to iron oxide was modulated by absorbed dose in solution, which regulated the catalytic activity of Fe 3 O 4 /NRGO. When the initial concentration of Fe(II) was 0.5 mM and the absorbed dose was 10 kGy, the as-prepared catalyst (Fe 3 O 4 @NRGO-10) showed superior catalytic activity for activating peroxymonosulfate (PMS) to degrade phenol. In the presence of 0.4 mM PMS and 0.5 g/L Fe 3 O 4 @NRGO-10, the pseudo first-order kinetic rate of phenol degradation reached 0.0286 min −1 . Sulfate radicals, hydroxyl radicals and high-valent iron oxo made major contribution to phenol degradation. The superior catalytic activity of Fe 3 O 4 @NRGO-10 might be attributed to the synergistic effect of NRGO and Fe 3 O 4 , in which NRGO promoted the conversion of Fe(III) to Fe(II). Fe 3 O 4 @NRGO-10 exhibited good stability in the cycling experiments. In addition to phenol, the Fe 3 O 4 @NRGO-10/PMS system could degrade sulfamethoxazole, bisphenol A and atrazine, indicating the wide applicability. This study reported a facile way to prepare carbon-supported metal oxide catalysts and convenient way to modulate the catalytic activity by absorbed dose.
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ACS Applied Nano Materials
·
2023
·
IF 5.9
Jiawei Lu,Ying-Nan Li,Youran Li,Huilin Zhu,Guiyang Shi
The reusability of immobilized lipases, including their hydrolysis activity, is greatly affected by lipase leakage, mass transfer channel blockage, and compound deposition on the outside surface. In this study, Candida antarctica lipase B (CALB) was immobilized on Fe3O4 nanoparticle-polyacrylonitrile (PAN) composite magnetic beads through phase inversion (L/FP). The hydrolysis activity of lipase was investigated using p-nitrophenyl palmitate (p-npp) as a model ester. To overcome the limitations of immobilized lipase in ester hydrolysis, three modification strategies were employed. First, lipase was covalently immobilized on Fe3O4 nanoparticles modified with methallyl (M9) and chloro (M13) silane modifiers, which exhibited faster immobilization with reduced lipase leaching and higher activity expression and stability. Second, poly(ethylene glycol) (PEG6000) and polylactic acid (PLA) were added to the precursors to physically modify the composite structures of L/FP, resulting in modified beads with larger specific surface area (15.26 m2·g–1) and smaller average pore size (19 nm). The modified beads, L/FP-9-M and L/FP-13-M, demonstrated superior reusability in long-term hydrolysis activity over 250 cycles. L/FP-9-M retained 63 and 34% of the initial activity at the 100th cycle and the 250th cycle, respectively. L/FP-13-M retained 55 and 36% of the initial activity at the 100th cycle and the 250th cycle, respectively. Furthermore, even after 250 repeated uses, the unit activities (U·gsupport–1) of both L/FP-9-M and L/FP-13-M remained higher than the initial activity of Novo 435.
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