TALANTA
·
2022
·
IF 6.556
Xiaodi Zhu,Jingkai Shan,Li Dai,Feifei Shi,Jinshen Wang,Huan Wang,Yuyang Li,Dan Wu,Hongmin Ma,Qin Wei,Huangxian Ju
Photoelectrochemical (PEC) immunoassays exhibiting high sensitivity and decent operability have considerable potential in areas such as cancer diagnostics. In particular, cathodic PEC configurations can prevent interference from reductive substances, which can occur in biological samples; however, challenges remain in terms of sensitivity and operability. In this study, separate-type PEC immunoassays were developed for carcinoembryonic antigen (CEA) by combining microplate-based immune recognition and off–on cathodic PEC detection. Polydopamine (PDA)-coated Prussian blue (PB) nanoparticles (PB@PDA NPs) were used as signal tags to label the detection antibody. The PB NPs and PDA captured on the microplates both disassembled under strongly alkaline conditions to generate redox-active electron acceptors . The disassembled products were quantitatively transferred to PEC detection cells and synergistically enhanced the PEC current with microstructured BiOI , which operated as a cathodic semiconductor electrode. As proof of principle, carcinoembryonic antigen (CEA) was applied to elucidate the potential application of PEC immunoassay in clinical diagnosis, and the obtained linear range of the sensor was 0.001–100 ng mL −1 with the detection limit of 54.9 fg mL −1 (S/N = 3). The proposed separate-type off–on PEC strategy showed high sensitivity and decent operability for CEA detection, indicating its potential for the identification of other tumor markers.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Wei Yang,Mingli Cao
The removal of heavy metal ions from the aqueous environment is an important topic as heavy metal pollution is widely distributed in water bodies, causing serious damage to aquatic ecosystems and worsening the already scarce freshwater resources. In this work, we report the synthesis of novel ZIF-8@GO-COOH composite nanosorbent materials by in situ self-assembly. The physicochemical properties of the composites were investigated using relevant characterisation techniques, and the adsorption capacity of ZIF-8@GO-COOH for copper and lead ions in aqueous solution was tested by batch adsorption experiments. The adsorption behaviour was analysed by combining adsorption kinetics, adsorption isotherm model and Van't Hoff model. The results showed that the adsorption capacities of ZIF-8@GO-COOH for Cu(II) and Pb(II) were 93.26 mg/g and 95.875 mg/g, respectively, when the initial heavy metal ion concentration was 100 mg/L, the adsorption time was 60 min, the temperature was 293 K and the pH conditions were suitable. The high adsorption performance of ZIF-8@GO-COOH was attributed to its surface with abundant oxygen-containing functional groups and excellent specific surface area, which gives it a significant advantage in the removal of heavy metal ions from aqueous solutions.
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ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
·
2021
·
IF 6.291
Yelin Zhu,Xinzhong Wang,Ping Wang,Jian Zhu,Yingnan He,Xiuxiu Jia,Fengqin Chang,Huaisheng Wang,Guangzhi Hu
In the present work, hematite–boron-carbonitride (Fe 2 O 3 –BCN) nanosheets were synthesized by a simple hydrothermal reaction and the following high temperature treatment. The morphology, structure and chemical composition of the as-prepared material were carefully characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). The Fe 2 O 3 –BCN nanosheets were used to modified on the surface of the glassy carbon electrode to fabricate an electrochemical sensor for lead ions (Pb(II)) via differential pulse anodic stripping voltammetry (DPASV). At the same time, the influence of the modification concentration, solution acidity, deposition potential and deposition time on response peak current of Pb(II) at the Fe 2 O 3 –BCN-based electrochemical sensor was well investigated. Under the optimized conditions, the electrochemical signal and concentration of Pb(II) show two-stage linear relationship in the range of 0.5 – 40 μg/L and 40 –140 μg/L, with a limit of detection (LOD) of 0.129 μg/L. The Fe 2 O 3 –BCN-based electrochemical sensor shows excellent selectivity and anti-interference ability in the anti-interference experiments and actual sample analysis experiments, revealing its broad application in environmental monitoring of Pb(II).
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高影响因子
Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Shenwan Wang,Dao Xiao,Xiaoyan Zheng,Lili Zheng,Yang Yang,Haide Zhang,Binling Ai,Zhanwu Sheng
Halloysite/biochar was prepared by co-pyrolysis at different temperatures using coconut shell and halloysite as raw materials. Magnetic adsorbents were prepared through ball-mill extrusion with Fe 3 O 4 and the halloysite/biochar and the capacity of the adsorbents to adsorb Pb(II) from water was evaluated and compared. The effects of pH, contact time, and initial Pb(II) concentration on the adsorption capacity of the magnetic adsorbents for Pb(II) were investigated. The pseudo-second-order ( R 2 =0.9999) and Langmuir isothermal models ( R 2 =0.9906) fit the experimental data well. The prepared samples denotes as MBM-HBC700 exhibited the highest Pb(II) adsorption capacity (833.33 ± 16.71 mg·g -1 ), and the removal efficiency of Pb(II) by the magnetic adsorbents was above 90% after four adsorption–desorption cycles. Complexation, cation exchange, cation–π interaction, precipitation, pore filling and electrostatic adsorption have been proposed as the main removal mechanisms. After applying MBM-HBCs to simulated electroplating wastewater, the contents of Pb(II), Cu(II), Zn(II), and Cr(VI) were significantly lower than the discharge standard of China. The magnetic adsorbents prepared in this study have wide application prospects in the treatment of Pb(II) in wastewater, thus providing a new approach for promoting waste recycling and utilization.
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高影响因子
CHEMOSPHERE
·
2021
·
IF 7.086
Da Wang,Shiwen Dong,Lingsha Wen,Weiting Yu,Zhiqiao He,Qingqing Guo,Xiaohui Lu,Lizhang Wang,Shuang Song,Jun Ma
A metal oxide electrode has been developed for the electrochemical CO 2 reduction reaction (eCO 2 RR). It exhibits superior activity and product selectivity towards eCO 2 RR by circumventing the previously encountered problem of self-reduction with high-valence metals. Specifically, a hydrocerussite [Pb 3 (CO 3 ) 2 (OH) 2 ] thin film has been synthesized in situ on a Pb substrate (denoted as ER-HC) by an electroreduction method using a lead-based metal–organic framework (Pb-MOF) as a precursor. The ER-HC electrode exhibits a high selectivity of 96.8% towards HCOOH production with a partial current density of 1.9 mA cm −2 at −0.88 V vs. the reversible hydrogen electrode (RHE). A higher HCOOH partial current density of 7.3 mA cm −2 has been achieved at −0.98 V vs. RHE. Physicochemical and electrochemical characterization results demonstrate that the defective hydrocerussite surface exhibits appropriate adsorption free energy of formate (HCOO − ) and a lower reaction free energy for HCOOH production from CO 2 , which greatly boosts the eCO 2 RR activity and HCOOH production selectivity. The structure and eCO 2 RR performance of the hydrocerussite thin film remain stable in 0.1 M KHCO 3 as electrolyte, ensuring its durability. Overall, this work not only provides a metal oxide electrode (metal hydroxide, to be more precise) with excellent eCO 2 RR performance, but also expands the in situ electrochemical derivatization strategy for the fabrication of metal oxide electrodes.
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高影响因子
MICROCHEMICAL JOURNAL
·
2021
·
IF 4.821
Hui Li,Jie Zhao,Shifan Zhao,Guofeng Cui
Developing a reliable, sensitive and portable electrochemical sensor for precise determination of trace heavy metal ions in water is an attractive challenge. In this work, an integrated three-electrode sensor based on screen–printed gold working electrode (SPAuE) ex-situ electroplated bismuth film was developed via a facile and simple process for the determination of trace Pb(II), Cd(II), and Zn(II) by square wave anodic stripping voltammetry (SWASV). The bismuth film was deposited on SPAuE at a potential of −0.08 V (Bi/SPAuE −0.08V ). The results exhibited the sensor with a wide linear range (from 1 to 120 μg L -1 ) for the simultaneous detection of these three heavy metal ions. Besides, the detection limits of Pb(II), Cd(II), and Zn(II) for the sensor were respectively found to be 0.04 μg L −1 , 0.02 μg L −1 , and 0.05 μg L −1 (S/N = 3). The proposed sensor revealed good anti-interference ability, satisfactory repeatability with RSDs of less than 2.5% (n = 12), excellent reproducibility with RSDs of less than 2.5% (n = 6), and considerable stability. The detection accuracy of the Bi/SPAuE −0.08V based sensor was further evaluated via atomic absorption spectroscopy (AAS). Due to its simplicity in process, high detection performance and excellent reliability, such sensors are expected to find utility in portable heavy metal detection applications.
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高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2021
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IF 4.539
Yanru Zhang,Mingzhu Xia,Fengyun Wang,Jianzhe Ma
Amino trimethylposphonate(ATMP) functionalized HAP were synthesized with different ATMP addition (0, 5%, 10%, 15%) and the adsorption performance towards Pb 2+ and Cd 2+ were studied in an aqueous solution. Under the optimum condition, HAP with ATMP addition of 10% (10AT-HAP) displayed the most efficient adsorption performance with the adsorption capacity of 1458.79 mg/g and 321.26 mg/g towards Pb 2+ and Cd 2+ , respectively, which improved 76% and 92% than that of the artificially prepared HAP in the laboratory, respectively. For both heavy metal ions , the adsorption mechanism also included ion exchange and surface complexation, in which the surface complexation played a predominant role. In addition, XRD showed that a new crystal phase was formed after Pb 2+ adsorption, while no new phase appeared after Cd 2+ adsorption, indicating that the adsorption mechanism of Pb 2+ involved dissolution-precipitation. The fitting results of adsorption isotherm and kinetics showed that the adsorption of Pb 2+ and Cd 2+ on HAP and 10AT-HAP were well fitted by the Langmuir isotherm model and Pseudo-second model. Moreover, Multiwfn wavefunction program based on density functional theory (DFT) was applied to deeply probe and vividly visualize the interaction sites, interaction types, interaction strength and the essence of interactions between HAP and ATMP or ATMP-HAP composite and heavy metal ions.
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高影响因子
Journal of Environmental Sciences
·
2021
·
IF 5.565
Wen Zhou,Jiale Deng,Zhen Qin,Ruihua Huang,Yi Wang,Shanshan Tong
Toxic heavy metal ions, valuable noble metal ions and organic dyes are significant concerns in wastewater treatment. In this work, MoO 3 nanobelts (MoO 3 NBs) prepared by solvothermal method and MoS 2 nanoarrays (MoS 2 NAs) constructed using MoO 3 NBs precursor were proposed to effectively remove heavy/noble metal ions and organic dyes, such as Pb (II) , Au (III) and Methylene Blue (MB). The two adsorbents exhibited the excellent adsorption capacity towards Pb (II) , Au (III) and MB. The maximum removal capacity of Pb (II) and MB on MoO 3 NBs was 684.93 mg/g and 1408 mg/g, respectively, whereas that of Au (III) and MB on MoS 2 NAs was 1280.2 mg/g and 768 mg/g, respectively. Furthermore, the thermodynamic parameters were calculated from the temperature-dependent curves, suggesting that the removal of Pb (II) and Au (III) on both adsorbents was spontaneous and endothermic. The new adsorbents introduced here were high adsorption activity, ease of fabrication, high scalability, good chemical stability, great repeatability and abundant and cheap supply, which were highly attractive for wastewater treatment.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2021
·
IF 4.539
Xiangke Han,Peng Li,Maowa Zhang,Jingtao Wang,Yijun Cao,Tong Zhang,Guoli Zhou,Fengli Li
The agglomeration of nanoscale carbon-based material with excellent large specific surface area and numerous active sites remains a challenging, which decreases the adsorption efficiency. Herein, a three-dimensional (3D) half-embedded architecture adsorbent membrane (ES-PAN/AHCNs) was designed to address this weakness by combining the small-sized activated hollow carbon nanospheres (AHCNs) with polyacrylonitrile (PAN) fiber. The 3D architecture precludes the agglomeration of AHCNs, while the half-embedded of AHCNs ensures structural stability of fiber adsorbents. The adsorption capacity and mechanism of ES-PAN/AHCNs membrane were investigated by using metal ions (Pb(Ⅱ), Cu(Ⅱ), Cr(Ⅲ)). Concretely, the adsorption capacity of ES-PAN/AHCNs membrane to Pb(Ⅱ), Cu(Ⅱ) and Cr(Ⅲ) were 192, 186 and 179 mg g −1 , respectively, which was more than two times than that of AHCNs. Noticeably, the significant increase of adsorption capacity mainly benefits from the 3D half-embedded architecture, owing to that pure PAN fiber has negligible adsorption capacity. Moreover, the adsorption capability of ES-PAN/AHCNs membrane retained 82.1% after twelve adsorption-desorption cycles. The strategy of fabricating 3D half-embedded adsorbent membrane substantially expands the potential for AHCNs applications in the adsorption and water purification fields.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Chen Wang,Chao Xiong,Yali He,Chen Yang,Xiteng Li,Jianzhong Zheng,Shixing Wang
A novel magnetic Zr-MOF named Ni 0.6 Fe 2.4 O 4 -UiO-66-PEI was synthesized by modifying UiO-66-NH 2 with Ni 0.6 Fe 2.4 O 4 and polyethyleneimine and its sorption characteristics for two representing heavy metals Pb(II) and Cr(VI) in water were examined. This material showed good thermal stability and was sufficiently magnetic to allow effective solid-liquid separation. The material had a maximum adsorption capacity of 273.2 mg/g for Pb(II) at pH 4.0 and 428.6 mg/g for Cr(VI) at pH 3.0, as obtained from the model fitting by the Hill equation. The sorption kinetics for both heavy metals on the material was fast, with adsorption equilibrium established in 60 min and 30 min for Pb(II) and Cr(VI), respectively. Model fitting of the kinetic data showed that Pb(II) and Cr(VI) sorption on Ni 0.6 Fe 2.4 O 4 -UiO-66-PEI followed the pseudo-second-order model. This material had good selectivity for competing ions, and still hold fairly good binding capacities after 5 times of regeneration. Adsorption mechanisms for Pb(II) and Cr(VI) by Ni 0.6 Fe 2.4 O 4 -UiO-66-PEI were proposed by analyzing FTIR, XPS and the electrokinetic property of the material. Specifically, Pb(II) adsorption on Ni 0.6 Fe 2.4 O 4 -UiO-66-PEI could be attributed to chelation of Pb(II) with the imine/amine functional groups in the material’s matrix, while Cr(VI) adsorption might stem from a combination of electrostatic attraction, chelation and redox reaction. It seems that Ni 0.6 Fe 2.4 O 4 -UiO-66-PEI could be used as a green and environmental-friendly material for heavy metals removal, particularly from acidic water streams.
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高影响因子
IONICS
·
2020
·Vol. 26
·期 8
·3901-3909
·
IF 2.394
Li Mei,Sun Zhongxuan,Guo Dan,Han Wei,Sun Yang,Yang Xiaoguang,Zhang Milin
The electrode reaction of Pr(III) and coreduction of Pb(II) and Pr(III) were studied on an inert W electrode in eutectic LiCl-KCl to extract Pr from molten salt. The electrode process kinetic of Pr(III) on W electrode was firstly explored employing cyclic voltammetry (CV) and Tafel technique, such as the diffusion coefficient of Pr(III) in eutectic LiCl-KCl and the exchange current density ( j 0 ) for Pr(III)/Pr(0) couple and the electrode reaction activation energy. Then, various electrochemical techniques were used to investigate the coreduction of Pb(II) and Pr(III). Four cathode current peaks ascribed to the formation of Pr x Pb y intermetallic compounds were detected, which indicated that the Pr could deposit on pre-deposited Pb film, react with Pb, and form Pr x Pb y intermetallic compounds. Furthermore, the electrolytic products formed by galvanostatic electrolysis were characterized by scanning electron microscopy coupled with energy dispersive X-ray diffraction, which illustrated the formation of PrPb 3 intermetallic compound in LiCl-KCl-PbCl 2 -PrCl 3 melt.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2020
·
IF 3.807
Feng Hong,Qiqin Wang,Wenhai Wang,Xixue Chen,Yuting Cao,Youren Dong,Ning Gan,Dazhen Wu,Futao Hu
How to eliminate the background signal of the electrochemical aptasensor and improve its signal amplification efficiency is one of the key factors to build a highly sensitive and selective sensor. Herein, we developed a multi-signal amplified, zero background electrochemical aptasensor for rapid detection of tumor markers, with carcinoembryonic antigen (CEA) as a model analyte . A type of dendritic DNA scaffold labeled with a lead-based metal organic framework (HCR-Pb-MOF) was prepared by hybrid chain reaction as signal tags. After one-step replacement of the signal tags into the supernatant by the target, the inner Pb 2+ ions in the replaced tags were detected by square-wave voltammetry (SWV) for qualification. The assay has some distinct advantages. Firstly, one HCR-Pb-MOF can load many Pb-MOFs, with each Pb-MOF containing large amounts of Pb 2+ ; thus, multi-amplified signals from Pb 2+ can be obtained after one-step replacement of the target. Secondly, Pb-MOF can also completely avoid the leakage of Pb 2+ , which is usually observed in the MOF probes electrostatically adsorbing metal ions , to achieve zero background. Thus, the aptasensor with a one-step replacement detection strategy can greatly improve sensitivity, with the detection limit of CEA being 0.333 pg mL −1 . Finally, the stirring bar was employed after introducing the target into the system. Therefore, the whole sample detection time can be reduced to within 10 min. This aptasensor was successfully applied to rapidly and accurately analyze CEA in human serum, with results consistent to those of ELISA . All of these findings prove that this multi-signal amplified, rapid, zero background electrochemical aptasensor can meet the requirements for rapid and highly sensitive detection of tumor markers in human serum.
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