CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Tongcai Liu,Danyu Zhang,Kai Yin,Chunping Yang,Shenglian Luo,John C. Crittenden
Unactivated peroxymonosulfate (PMS) degrading organic contaminants has been reported. Previous studies have focused on direct PMS oxidation, while the role of singlet oxygen ( 1 O 2 ) is often overlooked. Here, we studied the oxidation of thiacloprid (THIA) of the neonicotinoid insecticides by PMS without explicit activation. According to electron spin resonance spectroscopy and quenching experiments, the nonradical mechanism (i.e., direct PMS oxidation and 1 O 2 oxidation) was responsible for the THIA degradation. There are two pathways to generate 1 O 2 . The pyridine nitrogen of THIA structure can combine with PMS to produce epoxide , which is beneficial to generation of 1 O 2 . However, the contribution of 1 O 2 from PMS self-decomposition can be ignored. According to kinetic solvent isotropic effect analysis, the overall THIA degradation was attributed to 36.5% 1 O 2 oxidation and 63.5% direct PMS oxidation. A structure-activity assessment and density functional theory suggested that thioether sulfur, amidine nitrogen and the cyanoimino groups were the main reaction sites. Product analysis further confirmed the involvement of 1 O 2 and PMS. Moreover, three major THIA degradation pathways were proposed, including (i) heterolytic cleavage of peroxo bonds and transfer of oxygen atoms, (ii) electron transfer and (iii) oxidation of cyanoimino groups to generate nitroso/nitro-THIA. In addition, identification byproducts (Except for TP141) had lower ecotoxicity toxicity (using ECOSAR) in fish, daphnid and green algae. Effects of pH and natural water matrices on THIA oxidation via PMS were further evaluated. This study investigated the overlooked 1 O 2 oxidation reaction to elucidate the mechanism. The new mechanistic knowledge has important implications for other contaminants for their interactions with PMS.
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Journal of Analysis and Testing
·
2024
·Vol. 8
·期 1
·1-8
·
IF 5.5
Tu Mengling,Zhang Wei,Zhu Yunxiao,Ma Wen,Li Xiao,Zhou Shukun,Li Hongmei,Li Xianjiang
Thiacloprid is the first-generation neonicotinoid insecticide, which is widely used in modern agriculture. Reference materials are essential for sound measurement and traceability of results in chemical analysis. Pure thiacloprid was comprehensively assessed by two orthonormal methods: mass balance (MB) and quantitative nuclear magnetic resonance spectroscopy (qNMR). From MB, its mass fraction value was 998.4 mg/g with the subtraction of structurally related impurities (99.87%), inorganic impurities (0.006 mg/g), water (0.33 mg/g), and volatile organic solvent (0 mg/g). To guarantee sufficient separation of structurally related purity, peak purity of thiacloprid was evaluated by five points of UV spectra. From the qNMR of hydrogen, its mass fraction value was 995.7 mg/g which was traced to the internal standard (methyl sulfone). Finally, the certified value was assigned to 997 mg/g, together with an expanded uncertainty of 3 mg/g ( k = 2). This high-purity thiacloprid can be applied to routine monitoring in agriculture and the food fields.
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2022
·
IF 7.926
Zhikang Deng,Yongtao Cheng,Jinyao Zhu,Lie Yang,Zulin Zhang,Li Wu
Thiacloprid (THI), as a commonly used neonicotinoid, is frequently detected in environmental media, posing a potential threat to the environment and organisms. In this study, microalgae fuel cells (MFCs) with Chlorella sp. as cathode and wastewater (with sludge) as anode were constructed to remove THI (10, 20 and 50 mg/L) while generating bioelectricity . The results showed that, comparing with the open-circuit condition, the generation of bioelectricity (closed-circuit) significant enhanced the removal of THI by 13.14–32.47%. The presence of low concentration of THI (10–20 mg/L) did not significantly affect the accumulation of Chlorella sp. biomass, while high concentration THI (50 mg/L) strongly depressed its biomass. It was also found that high concentration THI caused obvious oxidative damages (MDA) to Chlorella sp., although SOD activity was upregulated. Both the highest THI removal efficiency (%) and stable bioelectricity voltage (202 mV) occurred at the low THI concentration (10 mg/L). Seven degradation products of THI were identified and the oxidation of the thiazole ring was the main detoxification way of THI. Additionally, toxicity evaluation also showed that the toxicity of degradation products were lower than THI. This study implies that MFCs could be a promising application, coupling pollutants removal , bioenergy generation and biomass production.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2019
·Vol. 26
·期 23
·23471-23479
·
IF 2.914
Tao Zhexuan,Deng Jiaqi,Wang Yan,Chen He,Ding Yuan,Hua Xiude,Wang Minghua
A rapid and sensitive immunoassay for the simultaneous detection of imidacloprid and thiacloprid was developed by using magnetic nanoparticles (MNPs) and upconversion nanoparticles (UCNPs). The UCNPs of NaYF 4 :Yb, Er and NaYF 4 :Yb, Tm were synthesized and conjugated with anti-imidacloprid monoclonal antibody (mAb) and anti-thiacloprid mAb as signal labels, while the MNPs were conjugated with antigens of thiacloprid and imidacloprid as separation elements. The fluorescence intensities of Yb/Er- and Yb/Tm-doped UCNPs were detected simultaneously in 544 nm and 477 nm under the excitation of NIR light (980 nm). The amounts of mAb-conjugated UCNPs that were separated by antigen-conjugated MNPs were determined based on competitive immunoassays. Under the optimal conditions, the 50% inhibiting concentration (IC 50 ) and limit of detection (LOD, IC 10 ) were 5.80 and 0.32 ng/mL for imidacloprid and 6.45 and 0.61 ng/mL for thiacloprid, respectively. The immunoassay exhibited negligible cross-reactivity with analogs of imidacloprid and thiacloprid except imidaclothiz (86.2%). The average recoveries of imidacloprid and thiacloprid in environmental and agricultural samples, including paddy water, soil, pears, oranges, cucumbers, and wheat, ranged from 78.4 to 105.9% with relative standard deviations (RSDs) of 2.1–11.9% for imidacloprid and ranged from 82.5 to 102.3% with RSDs of 1.0–16.5% for thiacloprid. In addition, the results of the immunoassay correlated well with high-performance liquid chromatography for the detection of the authentic samples.
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CHEMOSPHERE
·
2024
·
IF 8.1
Xiaohui Yan,Yongpan Shan,Yajie Ma,Yanqin Wang,Changcai Wu,Xiangliang Ren,Xianpeng Song,Dan Wang,Hongyan Hu,Xiaoyan Ma,Yan Ma
Nanotechnology aligns with the requirements of sustainable development of agriculture, and nano-pesticides offer a promising approach to controlling agricultural pests and increasing productivity. Non-target predators also play a crucial role in pest controls and enhancing the efficacy of pesticide on target organisms. Reducing the toxicity of pesticides to non-target organisms is key to of coordinating chemical control and biological control methods. Therefore, it is essential to assess the toxicity of nano-pesticides on non-target predators. In this study, a carbon dots-doped mesoporous silica nano-delivery system (Thi@CD-MSN) was successfully developed using CD-MSN as carrier material and thiacloprid (Thi) as a model pesticide. The results demonstrated that the synthesized Thi@CD-MSN exhibited a relatively high loading efficiency (33.58%). Laboratory bioassay experiments revealed that Thi@CD-MSN demonstrated effective insecticidal activity (LC 50 = 21.67 mg/L) in controlling Aphis gossypii Glover. Besides, the acute toxicity of Thi@CD-MSN on Chrysoperla pallens larvae was significantly lower than that of Thi, as was its toxicity to 4T1 cells. These findings suggest that CD-MSN can serve as an ecological safety carrier for pesticide delivery, improving the effective utilization of Thi while reducing the risks to non-target predators. These results are essential for comprehending the effects of nano-pesticides on non-target predators, providing informative data for implementing biological and chemical control strategies. It strengthens the safety evaluation of nano-pesticides.
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JOURNAL OF FOOD COMPOSITION AND ANALYSIS
·
2024
·
IF 4
Dongjian Li,Mulinde Timothy Ezra,Haoran Li,Yifei Chen,Chengyun Si,Xuefang Luo
Neonicotinoids (NEOs) are widely used in agricultural cultivation, and the presence of residual NEOs poses a serious threat to consumer health. Therefore, trace detection of NEOs is particularly important. In this study, a response surface experimental design was employed to develop AgNP with high enhancement factor and surface height anisotropy, effectively enhancing the Raman signals of acetamiprid (ACE) and thiacloprid (THI) through densely populated hotspots on the surface. Gaussian simulation calculations were used to assign peaks in the ACE and THI spectra. Subsequently, convolutional neural network, backpropagation neural network, and AlexNet neural network were employed to identify the ACE, THI, and mixed component spectra, successfully distinguishing the spectra of the three compounds and achieving qualitative analysis of unknown spectra. Furthermore, genetic algorithm-partial least squares was used to model the spectral data, achieving a correlation coefficient of 0.97. The method was applied for the detection of spiked tea samples, achieving a precision RSD of 4.84 %. Therefore, this sensor combined with intelligent algorithms can be used for spectral identification and trace detection of mixed pesticide samples with structurally similar compounds.
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ENVIRONMENTAL RESEARCH
·
2020
·
IF 5.715
Zhenlan Xu,Xiaoting Qian,Chao Wang,Chunrong Zhang,Tao Tang,Xueping Zhao,Lingxiangyu Li
Microplastics (MPs) as a type of emerging contaminant in the environment have attracted extensive attentions in recent years, and understanding the impacts of MPs on soil biodiversity and functioning are thus increasingly urgent. Nevertheless, few studies were performed to investigate potential effects of MPs on decay of soil organic pollutants in particular pesticides and enzyme activities . Herein, three types of MPs including polystyrene fragments (PS-50) and polyvinyl chloride beads (PVC-42000 and PVC-10) were added to soil at environmentally relevant concentrations (0.2 and 1.0%) to study their impacts on dissipation of thiacloprid and activities of urease, acid phosphatase , invertase and catalase . MPs exhibited negligible impacts on thiacloprid dissipation regardless of MPs type and content, being probably attributed to the unaltered bioavailability of thiacloprid in soil even after an addition of MPs, which was documented by using the hydroxypropyl-β- cyclodextrin (HPCD) extraction method. Batch sorption experiments also exhibited the comparable adsorption capacity of thiacloprid to soil with and without MPs, along with K f valuses of 3.44–3.77. Besides, MPs exerted negligible effects on enzyme activities of soil. Taken together, this study showed negligible impacts of MPs at environmentally relevant concentrations on thiacloprid dissipation and enzyme activity, expanding our knowledge on impacts of MPs at the environmentally relevant concentrations on pesticide dissipation in soil.
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高影响因子
Journal of Cleaner Production
·
2025
·
IF 10
Miao Wang,Donghui Xu,Ying Zhang,Jie Zhou,Zhihao Lin,Yiming Zhao,Xin Ding,Bin Sheng,Xiaobin Wen,Xiao Song,Ge Chen,Xiaomin Xu,Xin Yang,Guangyang Liu
The application of ZIF nanomaterials as controlled release agents for pesticides holds significant promise in enhancing pesticide utilization efficiency, prolonging their effectiveness, and minimizing pesticide residues. However, the loading efficiency of single ZIF is limited and susceptible to external stimuli. Therefore, in order to improve the loading rate of the material and enhance the bioavailability of the pesticide, a novel porous nanocarrier (MPN (Fe) @ZIF-8) was prepared for loading the neonicotinoid pesticide thiacloprid (THIA) by combining the biocompatible material metal polyphenol network (MPN) with ZIF-8 using the co-precipitation method and layer-by-layer self-assembly strategy. Through the selection of carrier materials and optimization of loading conditions, MPN (Fe) @ZIF-8 with irregular coral-like structure was obtained, which had high specific surface area (82.15 m 2 /g) and excellent load ratio (18.93 %). In addition, with the aim of preventing pesticide leakage, polyethyleneimine (PEI) was added to the nanocarrier system as a sealing agent, and porous ZIF nanopesticides with pH-responsive properties (MPN (Fe) @ZIF-8@THIA@PEI) were prepared. In vitro release experiments showed that MPN (Fe) @ZIF-8@THIA@PEI favoured the release of THIA (72.33 % cumulative release) under alkaline conditions (pH = 8.6), whereas it was delayed (42.24 % cumulative release) under acidic conditions (pH = 3.6). It was noteworthy that MPN (Fe) @ZIF-8@THIA@PEI has a higher lethality rate (89.04 %) against B. tabaci than commercial THIA reagents (66.67 %). Furthermore, after 8 h of UV irradiation, the residual pesticide in the commercial THIA reagent was only 11.27 %, while that in MPN (Fe) @ZIF-8@THIA@PEI remained at 73.98 %. Hence, this work provides new ideas for the development of green and environmentally friendly stimuli-responsive porous controlled release agents.
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Journal of Food Measurement and Characterization
·
2020
·Vol. 14
·期 4
·2021-2029
·
IF 1.648
Hussain Abid,Pu Hongbin,Sun Da-Wen
Surface-enhanced Raman spectroscopy (SERS) with cysteamine modified silver-coated gold nanoparticles (Au@Ag-CysNPs) was presented for fast screening of oxamyl and thiacloprid in liquid samples of milk. Concentrations at different levels were detected ranging from 0.5 to 10 ppm by choosing 500–1600 cm −1 spectral range. A strongest Raman peak at 679 cm −1 was ascribed to oxamyl, whereas a band at 1095 cm −1 was associated with thiacloprid in milk samples. The morphology and average size of core-shell nanoparticles (Au@AgNPs) and Au@Ag-CysNPs were acquired by High-resolution transition electron microscopy images and dynamic light scattering. Images showed that Au@AgNPs which had a core size of 28 nm and a shell of 6 nm thickness was modified with 6 nm cysteamine hydrochloride successfully. High coefficient of determination (R 2 ) values of 0.9968 and 0.9875 was calculated for oxamyl and thiacloprid with the limits of detection of 0.031 ppm and 0.023 ppm, respectively. The current novel nanoparticle was easy to prepare and was suitable to serve as a sensitive substrate for SERS detection applications, which could be employed for assessing other accidental contaminants in other food matrices in future studies.
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RSC Advances
·
2014
·Vol. 5
·期 4
·3039-3044
·
IF 3.708
Ming Li,Ming Ma,Xiude Hua,Haiyan Shi,Qiuxia Wang,Minghua Wang
Quantum dots (QDs), luminescent semiconductor nanocrystals, have the potential to simplify the performance of multi-analyte analysis. In this work, a novel indirect competitive fluorescence-linked immunosorbent assay (FLISA) based on QDs for the detection of clothianidin and thiacloprid simultaneously in environmental and agricultural samples were performed in a single well of the microtiter plate. The QDs-labeled antibody conjugates, which consists of CdSe/ZnS core–shell QDs and polyclonal antibodies, were prepared through the 1-ethyl-3-(3-dimethylaminopropyl) carbodiimide hydrochloride (EDC) coupling method. Under optimal conditions, the half-maximal inhibition concentration (IC50) and the limit of detection (LOD, IC10) of the FLISA were 12.5 and 0.3 ng mL−1 for clothianidin, and 9.27 and 0.4 ng mL−1 for thiacloprid, respectively. The cross-reactivities of the FLISA with the analogues of clothianidin and thiacloprid were negligible except for dinotefuran (10.4% for clothianidin). The spiked recoveries were 73.3% to 113.1% with relative standard deviations (RSDs) of 2.7 to 13.3% for the detection of clothianidin and thiacloprid in river water, soil, cabbage, rice and tomato. Furthermore, the results of FLISA for the authentic samples correlated well with those obtained by HPLC. The proposed FLISA is a satisfactory tool for rapid, sensitive, and quantitative detection of two pesticides simultaneously in agricultural and environmental samples. This study provides a strategy for the development of QDs-based fluoroimmunoassay for the quantitative analysis of two pesticides.
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TALANTA
·
2024
·
IF 5.6
Bin Yang,Jia Liu,Xin Liu,Shiyue Niu,Fengming Zhang,Yuting Wang,Daqian Song,Shuyun Bi
The high efficient surface-enhanced Raman scatterring (SERS) methods to detect thiacloprid and imidacloprid were established using ZIF-8-wrapped Ag nanoparticles (AgNPs) modified with β -cyclodextrin ( β -CD). The substrate of ZIF-8/ β -CD@AgNPs was characterized by ultraviolet visible spectra (UV–vis), thermogravimetric analysis (TGA), X-ray diffraction (XRD), transmission electron microscopy (TEM) and scanning transmission electron microscopy (STEM). The interaction between the substrate and thiacloprid/imidacloprid was also explored. The optimum measurement conditions were obtained by response surface model based on single-factor experiments. Enhancement factors (EFs) of thiacloprid and imidacloprid were respectively 2.29 × 10 6 and 2.60 × 10 6 . A good linearity between the scattering intensity and the concentration of thiacloprid/imidacloprid within 3–1000 nmol L −1 /6–400 nmol L −1 was established. The interference experiments indicated that the methods had good selectivity . The SERS methods were successfully applied to detect thiacloprid and imidacloprid in several vegetables samples. The recoveries ranged from 95.5 % to 105 % (n = 5). The detection limits (LODs) (S/N = 3) for thiacloprid and imidacloprid were 1.50 and 0.83 nmol L −1 , respectively.
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RSC Advances
·
2025
·Vol. 15
·期 37
·30817-30828
·
IF 4.6
Hui Fui,Xinran Ma,Yiping Huang,Shiyao Xi,Zhandong Ren,Yuchan Zhu
AS a low-cost and high-performance catalyst, spinel cobalt oxide (Co3O4) has two different catalytic active sites (tetrahedral Co2+ and octahedral Co3+) to drive the activation of peroxymonosulfate (PMS) through Co2+/Co3+ redox cycle. Tuning Co2+/Co3+ atomic ratio on the surface of Co3O4 for the construction of a synergy in the Co2+/Co3+ redox cycle might be an effective way to further boost PMS activation performance of Co3O4 catalyst. Herein, we suggested a metal-doping strategy to regulate Co2+/Co3+ atomic ratio of Co3O4 by partially substituting Co2+ with inert Mg2+ and formed a series of Mg doped Co3O4 (MCO) catalysts. Structural characterizations and experimental investigations demonstrated that Mg doping did not change Co3O4 host lattice and particle morphology, but could manipulate surface Co2+/Co3+ atomic ratio of Co3O4 for an improved PMS activation. The optimal MCO catalysts (MCO-0.2) with the suitable Co2+/Co3+ atomic ratios (1.13) exhibited the excellent thiacloprid (THIA) degradation performance through PMS activation, and the apparent degradation rate constant (0.2835 min−1) was highly outperformed that of pure Co3O4 (0.09555 min−1) and other similar cobalt-based catalysts. The optimal THIA degradation conditions might be: catalyst dose 100 mg L−1, PMS concentration 0.8 mM, pH 7 and THIA concentration 20 mg L−1. Quenching experiments and electron paramagnetic resonance (EPR) characterizations suggested SO4˙−, HO˙ and 1O2 were all involved in THIA degradation during the MCO-0.2/PMS process. Furthermore, the steady-state concentrations of these reactive species and their relative contributions to THIA degradation were also calculated by combining a kinetic model and a series of probe compound-based experiments. The results indicated that SO4˙− and HO˙ were generated at lower steady-state concentrations than that of 1O2, but they dominated THIA abatement during the MCO-0.2/PMS process. This study presented new insights into the construction of efficient PMS activator and a mechanistic understanding for PMS-mediated reaction.
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