ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2017
·Vol. 24
·期 21
·17598-17605
·
IF 2.741
Wang Na,Jia Daqing,Jin Yaoyao,Sun Sheng-Peng,Ke Qiang
The present study investigated the degradation of trichloroethylene (TCE) in sand suspensions by Fenton-like reaction with magnetite (Fe 3 O 4 ) in the presence of various chelators at circumneutral pH. The results showed that ethylenediaminetetraacetic acid (EDTA) and nitrilotriacetic acid (NTA) greatly improved the rate of TCE degradation, while [S,S]-ethylenediaminedisuccinic acid (s,s-EDDS), malonate, citrate, and phytic acid (IP6) have minimal effects on TCE degradation. Quenching tests suggested that TCE was mainly degraded by hydroxyl radical (HO · ) attack, with about 90% inhibition on TCE degradation by the addition of HO · scavenger 2-propanol. The presence of 0.1–0.5% Fe 3 O 4 /sand ( w / w ) contributed to 40% increase in TCE degradation rates. In particular, the use of chelators can avoid high concentrations of H 2 O 2 required for the Fenton-like reaction with Fe 3 O 4 , and moreover improve the stoichiometric efficiencies of TCE degradation to H 2 O 2 consumption. The suitable concentrations of chelators (EDTA and NTA) and H 2 O 2 were suggested to be 0.5 and 20 mM, respectively. Under the given conditions, degradation rate constants of TCE were obtained at 0.360 h −1 with EDTA and 0.526 h −1 with NTA, respectively. Enhanced degradation of TCE and decreased usage of H 2 O 2 in this investigation suggested that Fenton-like reaction of Fe 3 O 4 together with NTA (or EDTA) may be a promising process for remediation of TCE-contaminated groundwater.
研究领域:
环境科学
·
化学工程
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DOI
PubMed
高影响因子
MICROCHEMICAL JOURNAL
·
2023
·
IF 4.8
Shu Wang,Bingliang Zhang
Nitrilotriacetic acid (NTA) and ethylenediaminetetraacetic acid (EDTA), as widely used chelating agents, have created many environmental issues and raised much attention regarding their environmental occurrence. However, the determination of NTA and EDTA in samples of complex solution chemistry remains challenging. Here, we proposed a simple and sensitive method based on liquid chromatography tandem mass spectrometry (LC-MS/MS) to determine NTA and EDTA from aqueous samples without an enrichment step. During the analysis, H + -cation exchange was used to efficiently eliminate interference from metal ions. The intensity of NTA and EDTA with trimethylsilyldiazomethane methylation could be improved hundreds of times that of the virgin samples. To maximize sensitivity, the sample pretreatment methods, the derivatization procedures and the LC-MS/MS conditions were systematically optimized. The validated method showed low limits of quantification (0.4 μg/L for NTA and 1.5 μg/L for EDTA), a wide linear response (up to several mg/L, R 2 > 0.998), and good intra- and inter-day precision (relative standard deviation ≤ 11%). The reliability of this method was successfully validated by analysis of authentic water samples collected from three WWTPs and one river with satisfactory recoveries (80–117%). It can be proposed as a powerful analytical method of NTA and EDTA in authentic water samples and could potentially be adapted to detect other chelates and polydentate compounds.
研究领域:
环境科学
·
分析化学
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DOI
高影响因子
WATER RESEARCH
·
2024
·
IF 11.4
Yihua Chen,Jiaxin Zhu,Hang Ma,Yurong Gu,Tongzhou Liu
Perfluorooctane sulfonate (PFOS) is a persistent organic pollutant posing a risk in environmental persistence, bioaccumulation and biotoxicity. This study was to reach a comprehensive and deeper understanding of PFOS elimination in a UV 254 photolytic treatment with the co-presence of Fe 2+ and nitrilotriacetic acid trisodium salt (NTA). PFOS defluorination was noticeably enhanced in the UV/Fe 2+ -NTA treatment compared with UV/NTA, UV/Fe 2+ and our previously studied UV/Fe 3+ treatments. UV–vis, FTIR, and UPLC/MS-MS results indicated the formation of PFOS-Fe 2+ -NTA complex in PFOS, Fe 2+ and NTA mixture. The transition energy gap of PFOS-Fe 2+ -NTA decreased below the excitation energy supplied by UV 254 irradiation, corresponding with red shift appearing in UV–vis scanning spectrum. This favored intramolecular electron transfer from Fe 2+ -NTA to PFOS under UV 254 irradiation to form electron-accepting PFOS. Molecular electrostatic potential and atom charge distribution analyses suggested electron density rearrangement and perturbation in the perfluorinated carbon chain of electron-accepting PFOS, leading to the decrease in bond dissociation energies. Intermediate products detection suggested the parallel defluorination pathways of PFOS desulfonation, middle carbon chain scission and direct C-F cleavage. NTA exhibited crucial functions in the UV/Fe 2+ -NTA treatment by holding Fe 2+ /Fe 3+ in soluble form as a chelant and favoring water activation to generate hydrated electrons (e aq − ) under UV irradiation as a photosensitizer. Fe 2+ acting as the conduit for electron transfer and the bridge of PFOS anion and NTA was thought functioning best at 200 µM in this study. The degree of UV/Fe 2+ -NTA -synergized PFOS defluorination also depended on e aq − yield and UV 254 photon flux. The structure dependence on the electron transfer process of PFOS and PFOA was explored incorporating molecular structure descriptors. Because of possessing greater potential to acquire electrons or less likeliness to donate its electrons than PFOA, PFOS exhibited faster defluorination kinetics in the published “reduction treatments” than “oxidation” ones. Whereas, PFOA defluorination kinetics were at similar level in both “reduction” and “oxidation” treatments.
研究领域:
环境科学
·
化学
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DOI
PubMed
高影响因子
JOURNAL OF ENVIRONMENTAL ENGINEERING
·
2021
·Vol. 148
·期 1
·04021072
·
IF 1.86
Ting Su,Xiaoning Wang,Xinan Chen,Yan Cheng,Zhenkai Wang,Zhangxiong Wu,Winston Duo Wu,Sheng-Peng Sun
The ferric-nitrilotriacetate (Fe3+-NTA)-catalyzed homogenous Fenton-like reaction (i.e., Fe3+-NTA/H2O2) has received increasing interest for environmental applications, but its potential in degrading trichloroethylene (TCE) in groundwater still is not well known. The results of this study showed that Fe3+-NTA/H2O2 was more effective than other Fe3+-chelate/H2O2 processes (e.g., including ethylenediaminetetraacetate, ethylenediamine-N,N′-disuccinate, citrate, malonate, and tartrate) in degrading TCE in groundwater at natural pH (∼8.0). The effects of important parameters including the ratio of NTA∶Fe3+, and the dosages of Fe3+-NTA and H2O2 were investigated. Greater than 98% degradation efficiency of TCE in actual groundwater was obtained after 60 min of reaction time under the given conditions of NTA∶Fe3+=1.5∶1, 0.1 mM Fe3+-NTA, 5 mM H2O2, and pH 8.0. Hydroxyl radical (HO•) was responsible for the degradation of TCE, and the by-products were identified as formic acid and chloride ion (Cl−). Greater than 90% degradation efficiency of TCE in a sand column was achieved under dynamic conditions [0.5 mM Fe3+-NTA (1∶1.5), 4 mM H2O2, and hydraulic retention time of 4 h], resulting in stoichiometric ratios of ΔCl−∶ΔTCE and ΔTCE∶ΔH2O2 of ∼3∶1 and 4%, respectively. Compared with iron mineral (e.g., magnetite)-catalyzed Fenton-like processes, Fe3+-NTA/H2O2 led to much smaller consumption of H2O2 (at least 1 order of magnitude smaller). In addition, the buffering capacity of bicarbonate anions (HCO3−) in groundwater had a positive effect on the degradation of TCE by Fe3+-NTA/H2O2.
研究领域:
环境科学
·
化学工程
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DOI
高影响因子
RSC Advances
·
2019
·Vol. 9
·期 1
·397-407
·
IF 3.049
Yulian Li,Junyong He,Kaisheng Zhang,Tao Liu,Yi Hu,Xifan Chen,Chengming Wang,Xingjiu Huang,Lingtao Kong,Jinhuai Liu
Copper (Cu2+), cadmium (Cd2+) and lead ions (Pb2+) are toxic to human beings and other organisms. In this study, a silica gel material modified with nitrilotriacetic acid (NTA-silica gel) was sensibly designed and prepared via a simple amidation procedure for the removal of Cu2+, Cd2+ and Pb2+ from water. The NTA-silica gels showed rapid removal performances for the three metal ions (Pb2+ (<2 min), Cu2+ and Cd2+ (<20 min)) with relatively high adsorption capacities (63.5, 53.14 and 76.22 mg g−1 for Cu2+, Cd2+ and Pb2+, respectively). At the same concentration of 20 mg L−1, the removal efficiencies of the three metals by the adsorbent ranged from 96% to 99%. The Freundlich and Langmuir models were utilized to fit the adsorption isotherms. The adsorption kinetics for the three metal ions was pseudo-second-order kinetics. The removal performance of the NTA-silica gels increased in a wide pH range (2–9) and maintained in the presence of competitive metal ions (Na+, Mg2+, Ca2+ and Al3+) with different concentrations. In addition, the NTA-silica gels were easily regenerated (washed with 1% HNO3) and reused for 5 cycles with high adsorption capacity. This study indicates that the NTA-silica gel is a reusable adsorbent for the rapid, convenient, and efficient removal of Cu2+, Cd2+, and Pb2+ from contaminated aquatic environments.
研究领域:
环境科学
·
环境化学
·
水污染控制
·
吸附材料
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环境功能材料
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DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 29
·期 30
·45623-45634
·
IF 5.19
Liang Linqing,Wang Jiahong,Tong Xinhao,Zhang Shutong
The Fe 3 O 4 @nSiO 2 @mSiO 2 /NTA (FNMs-NTA) was prepared by grafting magnetic mesoporous microspheres with nitrilotriacetic acid (NTA) and applied as an adsorbent for the removal of Cr(III) from complex solutions. Some characterization techniques including Brunauer–Emmett–Teller (BET), Fourier transform infrared spectrometer (FT-IR), X-ray diffraction (XRD), small-angle X-ray diffraction (SAXS), vibrating sample magnetometer (VSM), and thermal gravimetric analysis (TGA) were used to characterize functional groups and pore structure of FNMs-NTA, which proved that NTA was successfully decorated onto the magnetic Fe 3 O 4 @nSiO 2 @mSiO 2 (FNMs) and FNMs-NTA featured a regular mesoporous structure. The batch adsorption of Cr(III) by FNMs-NTA exhibited high adsorption capacity (16.0 mg·g −1 at pH 3.0, and 25 °C). Adsorption data followed Freundlich isotherm and adsorption process was a spontaneous adsorption process. Moreover, the kinetics of adsorption were well explained by pseudo-second-order kinetic model. FNMs-NTA showed resistance to interfering inorganic cations (Na + , Ca 2+ ) and complexing agents (EDTA). Furthermore, FNMs-NTA exhibited remarkable regeneration performance and easy separation under external magnetic field. X-ray photoelectron spectroscopy (XPS) analysis showed the FNMs-NTA had excellent adsorption ability for Cr(III) because of the ion exchange and surface complexation.
研究领域:
环境科学
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材料科学
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DOI
PubMed
高影响因子
IET Nanobiotechnology
·
2019
·Vol. 14
·期 1
·67-72
·
IF 1.925
Wenjing Wang,Fengzhen Zhou,Xiyao Cheng,Zhengding Su,Huiling Guo
To effective capture and universal enrichment of His-tagged protein, polyacrylic acid (PAA) brushes were used to encapsulate Fe 3 O 4 nanoparticles, connect NTA, and Ni 2+ to prepare magnetic beads. These materials provide many advantages, such as excellent stability, tuneable particle size, and a surface for further functionalisation with biomolecules. His-tagged green fluorescence protein (GFP) was separated efficiently, and the binding capacity of Fe 3 O 4 /MPS@PAA/NTA-Ni 2+ was 93.4 mg/g. Compared with High-Affinity Ni-NTA Resin and Ni-NTA Magnetic Agarose Beads, Fe 3 O 4 /MPS@PAA/NTA-Ni 2+ nanocomposites exhibited higher separation efficiency and binding capacity towards His-tagged GFP. Moreover, the selectivity and recyclability of them for the target proteins were maintained well after six cycles. This study would widen the application of PAA in constructing multifunctional nanocomposites for biomedical fields.
研究领域:
生物技术
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蛋白质工程
·
纳米材料
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2017
·
IF 6.216
Yaoyao Jin,Sheng-Peng Sun,Xueying Yang,Xiao Dong Chen
The activation of potassium persulfate (KPS) by Fe II -NTA complex has been investigated to degrade ibuprofen in aqueous solutions under neutral pH conditions. The results showed that ibuprofen degradation by Fe II -NTA/KPS process was not successful due to the rapid oxidation of Fe II -NTA complex by dissolved oxygen. However, an efficient degradation of ibuprofen was achieved by Fe II -NTA/KPS process in the presence of hydroxylamine (HA). It was evident that the steady-state Fe II concentration in Fe II -NTA/HA/KPS process was much higher than that in Fe II -NTA/KPS process because of the quick regeneration of Fe II -NTA complex by HA. The suitable conditions for Fe II -NTA/HA/KPS process were obtained at [Fe II ] = 0.1 mM, [NTA/Fe] = 1:1, [HA/Fe] = 20:1 and [KPS/Fe] = 30:1. The generation of sulfate radical (SO 4 − ) and hydroxyl radical ( OH) contributed to ∼80% of ibuprofen degradation, and ∼20% of ibuprofen degradation was resulted from other reactive species such as persulfate radical (S 2 O 8 − ). Fe II -NTA complex was more effective than Fe II -EDDS and Fe II -EDTA complexes in the activation of KPS, and moreover which was also capable of activating Oxone at neutral pH. A successful degradation of ibuprofen in lake water was achieved by Fe II -NTA/HA/KPS process, while the rate of ibuprofen degradation in simulated groundwater was relatively slower because of the scavenging effects of HCO 3 − on SO 4 − / OH. The major intermediates in ibuprofen degradation were identified by LC-QTOF-MS analysis and the degradation pathways were proposed.
研究领域:
环境科学
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化学工程
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DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2023
·
IF 8.4
Yiyu Chen,Huiting Lian,Bin Liu,Guangming Liu,Xiaofeng Wei
Food allergy diagnosis requires a highly sensitive detection of allergen-specific immunoglobulin E (sIgE) in the serum. Enzyme-linked immunosorbent assay (ELISA) is a classical method widely used for sIgE detection but had to rely on costly and time-consuming assay procedures, skilled technicians, and bulky equipment. Here, a multiplexed origami paper analytical device (moPAD) that is hexahistidine-tagged and integrated with a nitrilotriacetic acid-functionalized surface with nickel (Ni-NTA) was developed to achieve low-cost and high-efficiency immunosensing of multiple allergen-specific IgEs in serum. The major oyster allergens, Cra a 1, Cra a 2, and Cra a 4, were used to detect sIgE in human serum. The feasibility of the moPAD-based immunosensing strategy was successfully demonstrated by desirable sensitivities for multiple targets. The detection results of moPAD for 72 serum samples were 100% consistent with clinical test results, while 69 of these results showed no significant differences from ELISA results, demonstrating the accuracy and stability of this method. A fully integrated moPAD reduces detection time and achieves highly sensitive quantification using a simple smartphone-based readout. Efficient allergen modification of paper devices has great applicability in allergen component-resolved diagnostics. The implementation of moPAD can make the process of allergy diagnosis simpler for patients, physicians, and healthcare systems alike.
研究领域:
免疫学
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生物医学工程
·
诊断技术
·
过敏研究
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高影响因子
BIOPROCESS AND BIOSYSTEMS ENGINEERING
·
2021
·Vol. 44
·期 10
·2193-2204
·
IF 3.21
He Song,Wu Xiaomei,Ma Baodi,Xu Yi
The novel Ni-NTA-functionalized magnetic chitosan microspheres (MCS-NTA-Ni) were prepared via amino functionalization of MCS with epichlorohydrin and ethylenediamine, followed by the introduction of the aldehyde groups and NTA in turn, and nickel (II) ions were chelated in the end. MCS-NTA-Ni contained numerous long-armed NTA-Ni surface groups, ensuring high enzyme loading and providing more space and flexibility to attach enzymes and maintain their activity. This microsphere can have highly selective adsorption of his-tagged recombinant protein. The his-tagged recombinant Microbacterium esterase of E. coli BL21 (DE3)/pET21a-EstSIT01 was first immobilized on MCS-NTA-Ni by affinity fixation, giving high immobilization yield (90.1%) and enzyme loading (120 mg/g). Compared with free esterase, the immobilized esterase was found to exhibit higher pH stability and thermal stability. In addition, the immobilized esterase had excellent reusability for the synthesis of key chiral intermediate of d -biotin and the substrate conversion could still keep 100% after 8 cycles continuously.
研究领域:
生物化学
·
酶工程
·
合成生物学
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DOI
PubMed
高影响因子
ENVIRONMENTAL RESEARCH
·
2023
·
IF 8.3
Wen Qin,Jianshan Peng,Jingru Yang,Yang Song,Jun Ma
In this study, the relative residual UV absorbance (UV 254 ) and/or electron donating capacity (EDC) was investigated as a surrogate parameter to evaluate the abatement of micropollutants during the Fe(II)/PMS and Mn(II)/NTA/PMS processes. In the Fe(II)/PMS process, due to the generation of SO 4 •- and •OH at acidic pH, UV 254 and EDC abatement was greater at pH 5. In the Mn(II)/NTA/PMS process, UV 254 abatement was greater at pH 7 and 9, while EDC abatement was greater at pH 5 and 7. This was attributed to the fact that MnO 2 was formed at alkaline pH to remove UV 254 by coagulation, and manganese intermediates (Mn(V)) were formed at acidic pH to remove EDC via electron transfer . Due to the strong oxidation capacity of SO 4 •- , •OH and Mn(V), the abatement of micropollutants increased with increasing dosages of oxidant in different waters in both processes. In the Fe(II)/PMS and Mn(II)/NTA/PMS processes, except for nitrobenzene (∼23% and 40%, respectively), the removal of other micropollutants was greater than 70% when the oxidant dosages were greater in different waters. The linear relationship between the relative residual UV 254 , EDC and the removal of micropollutants was established in different waters, showing a one-phase or two-phase linear relationship. The differences of the slopes for one-phase linear correlation in the Fe(II)/PMS process (micropollutant-UV 254 : 0.36–2.89, micropollutant-EDC: 0.26–1.75) were less than that in the Mn(II)/NTA/PMS process (micropollutant-UV 254 : 0.40–13.16, micropollutant-EDC: 0.51–8.39). Overall, these results suggest that the relative residual UV 254 and EDC could truly reflect the removal of micropollutants during the Fe(II)/PMS and Mn(II)/NTA/PMS processes.
研究领域:
环境科学
·
化学工程
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DOI
PubMed
高影响因子
JOURNAL OF WUHAN UNIVERSITY OF TECHNOLOGY-MATERIALS SCIENCE EDITION
·
2018
·Vol. 33
·期 3
·559-565
·
IF 0.524
Guo Huiling,Sun Honghao,Su Zhengding,Hu Shuchao,Wang Xiaotao
A facile approach has been developed to synthesize Fe 3 O 4 @PAM (polyacrylamide) nanoparticles (NPs) with carboxyl groups on the surfaces by copolymerization with acrylamide and acrylic acid in Fe 3 O 4 NPs aqueous suspension. Nitrilotriacetic acid (NTA) was conjugated to the magnetic NPs via well-known carboniimide chemistry using EDC and NHS. The Ni 2+ ions loaded on the surface of NPs provide abundant docking sites for immobilization of His-tagged green fluorescent proteins (His-tagged GFP). The high magnetic property of Fe 3 O 4 @PAM@NTA-Ni 2+ allows an easy separation of the NPs from solution under an external magnetic field, with high His-tagged protein binding capacity (42 μg protein/mg of NPs). The NPs can be recycled for at least four times without significant loss of binding capacity to proteins. These materials show great potential to separate His-tagged protein with low-cost purification at industrial scale.
研究领域:
材料科学
·
生物化学
·
生物技术
·
纳米技术
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产品关联
DOI
高影响因子