MICROCHEMICAL JOURNAL
·
2026
·
IF 5.2
Jiangchuan Tang,Qiaohui Lu,Minghui Luo,Xiao Yang,Huiling Deng,Lijun Wang,Xianggui Chen
A steric-hindrance-mediated “on-off” switchable probe is developed. • Triple-helix aptamer blocks nanozyme sites, inhibiting activity until target binding. • Solution assay detects clothianidin at 5.345 ng/mL with high sensitivity. • The probe is integrated into a portable paper-based device (PAD). • The PAD enables on-site screening with an LOD of 68.221 ng/mL. While the integration of triple-helix aptamer (THA) recognition with nanozyme catalytic activity offers great potential for on-site detection, the commonly used label-free THA-regulated nanozyme strategy suffers from an inherently high background signal, which significantly limits its applicability in environmental and food samples. In this study, a THA-grafted nanozymes was developed based on a steric-hindrance-mediated “on-off” switching mechanism for clothianidin (CLO) detection. THA was immobilized on Fe 3 O 4 @Cu-MOF nanozymes as a steric blocker, which physically masked the active sites via their spatial conformation, effectively suppressing the nanozyme's catalytic activity (“off” state). In the presence of CLO, specific binding induced a conformational change of THA. This conformational change exposes the previously masked active sites, “turning on” the nanozyme's activity and generating a quantitative colorimetric signal. Leveraging this precise switching mechanism, we established a highly sensitive solution-phase assay with a limit of detection (LOD) of 5.35 ng/mL and recoveries ranging from 94.05% to 102.14%, which was comparable to those obtained by liquid chromatography-tandem mass spectrometry (LC-MS/MS). To translate this system into a field-deployable platform, the probe was immobilized on paper to fabricate a paper-based analytical device (PAD). The resulting PAD achieved CLO detection with an LOD of 68.22 ng/mL. Overall, the developed method provides a portable, user-friendly, and practical platform for on-site screening of CLO in food samples. Download: Download high-res image (154KB) Download: Download full-size image
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高影响因子
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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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Pijun Duan,Yuanfeng Qi,Shanshan Feng,Xiaoming Peng,Wei Wang,Yue Yue,Yanan Shang,Yanwei Li,Baoyu Gao,Xing Xu
FeMn bimetallic nanoparticles coated with nitrogen-doped graphene shells (FeMn@N-C) were prepared to decompose clothianidin (CTD) through activation of peroxymonosulfate (PMS). The redox cycles of encapsulated FeMn bimetallic nanoparticles with multiple valence states could accelerate the radical generation and ensure the stability of FeMn@N-C with continuous PMS activation. Coexisting NaH 2 PO 4 could unusually accelerate CTD degradation through facilitating reactive oxygen species (ROS) generation and decreasing bonding dissociation energies of CTD molecule. DFT calculation indicated that the C-Cl bond in CTD molecule was weakened after being surrounded by NaH 2 PO 4 . Two main degradation pathways were proposed in the absence of phosphate and a new dechlorination pathway was first reported after CTD molecule bonding with phosphate, which was confirmed by DFT. This work provides a feasible strategy of PMS activation by graphene coated bimetallic nanoparticles and give a new insight into accelerated degradation of recalcitrant pollutants with phosphate surrounding.
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高影响因子
PEST MANAGEMENT SCIENCE
·
2023
·Vol. 79
·期 7
·2603-2610
·
IF 4.1
Yue Ma,Kefei Zhao,Yi Ding,Shuai Wu,Xun Liao,Xianhui Yin,Zilu Li,Rongyu Li,Youhua Long,Fengpei Du
BACKGROUND Neonicotinoids are among the most essential chemical insecticides worldwide because of their high activity against many important pests and wide application. However, their application is limited by their toxicity to honeybees. Therefore, the development of a facile route to fabricate efficient and eco-friendly pesticide formulations is of great significance. RESULTS In this study, clothianidin-loaded zeolitic imidazolate framework-8 (CLO@ZIF-8) nanoparticles were fabricated by a facile one-pot route using zinc nitrate as a Zn 2+ source and characterized by scanning electron microscopy, transmission electron microscopy, X-ray diffraction, thermogravimetric analysis, energy-dispersive spectrometry and Fourier transform infrared spectroscopy. Based on the pH response of ZIF-8, a ‘burst release effect’ was observed for CLO@ZIF-8 at pH 3 and 5 within 12 h, in contrast to the slow and sustainable release at pH 8. CLO@ZIF-8 improved the retention ability of the pesticide liquid and remained 70% control efficacy on Nilaparvata lugens after water rinsed of sprayed CLO@ZIF-8. The pH response of CLO@ZIF-8 allowed it to maintain 43% control efficacy against N. lugens after 10 days of application, which was twice the efficacy of clothianidin solution (SCA). Moreover, CLO@ZIF-8 reduced the acute toxicity to honeybees ( Apis mellifera ) by ≥120-fold compared with SCA. CONCLUSION This study provides new insights into the application of ZIF-8 to neonicotinoids and suggests the need for the development of a biocompatible and eco-friendly pesticide formulation. © 2023 Society of Chemical Industry.
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高影响因子
MICROCHEMICAL JOURNAL
·
2022
·
IF 5.304
Yanju Wu,Kainan Guo,Junqi Zhao,Qunpeng Duan,Fei Wang,Kui Lu
On the surface of glassy carbon electrode, electrochemically reduced graphene oxide-anionic pillar[6]arene (ErGO-AP6) composite film is directly constructed using a potentiostatic method. This composite film is used as an electrochemical sensing platform for detecting clothianidin (CLO). Studies on the interaction mechanism reveal a higher supramolecular recognition capability between AP6 and CLO, compared to that between β -cyclodextrin ( β -CD) and CLO. Owing to the synergistic effect of ErGO and AP6, the ErGO-AP6 composite film shows an outstanding sensitivity and excellent selectivity towards CLO, superior to that of ErGO- β -CD film. The linear range from 1.0 × 10 −7 to 5.0 × 10 −5 mol L −1 and detection limit of 4.0 × 10 −8 mol L −1 for CLO are achieved. In addition, the presented method is used for fruit and water samples in a recovery test, showing recovery rates between 90.0% and 99.4%. This study provides a promising electrochemical sensing platform for rapid and sensitive analysis of CLO.
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MICROCHIMICA ACTA
·
2024
·Vol. 191
·期 4
·1-10
·
IF 5.3
Cao Hui,Han Yiyi,Chen Zixin,Ding Xiner,Ye Tai,Yuan Min,Yu Jinsong,Wu Xiuxiu,Hao Liling,Yin Fengqin,Xu Fei
A novel molecularly imprinted nanomaterial (Eu (BTC)-MPS@MIP) was synthesized on the surface of silanized europium-based metal–organic frameworks (Eu (BTC)-MPS) using 1, 3, 5-benzotrioic acid (H 3 BTC) as a ligand. The resulting Eu (BTC)-MPS@MIP was applied to constructing a smartphone sensing platform for the sensitive and selective detection of clothianidin (CLT) in vegetables. The synthesized Eu (BTC)-MPS@MIP demonstrated the successful formation of a typical core–shell structure featuring a shell thickness of approximately 70 − 80 nm. The developed sensing platform based on Eu (BTC)-MPS@MIP exhibited sensitivity in CLT detection with a detection limit of 4 µg/L and a linear response in the range 0.01 − 10 mg/L at excitation and emission wavelengths of 365 nm and 617 nm, respectively. The fluorescence sensing platform displayed excellent specificity for CLT detection, as evidenced by a high imprinting factor of 3.1. This specificity is primarily attributed to the recognition sites in the molecularly imprinted polymer (MIP) layer. When applied to spiked vegetable samples, the recovery of CLT ranged from 78.9 to 102.0%, with relative standard deviation (RSD) values falling between 2.2 and 6.2%. The quenching mechanism of Eu (BTC)-MPS@MIP toward CLT can be attributed to the inner filter effect (IFE), resulting from the optimal spectral overlap between the absorption spectrum of CLT and the excitation spectra of Eu (BTC)-MPS@MIP. The proposed method has the potential for extension to the detection of other pesticides by replacing the MIP recognition probes. Graphical abstract
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高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2014
·
IF 3.163
Ming Li,Xiude Hua,Ming Ma,Jisong Liu,Liangliang Zhou,Minghua Wang
Two rapid, sensitive immunoassays based on monoclonal antibody for detecting clothianidin were developed and applied in agricultural samples: a quantitative enzyme-linked immunosorbent assay (ELISA) and a semiquantitative gold immunochromatographic assay (GICA). Under optimal conditions, the half-maximal inhibition concentration (IC 50 ) and the limit of detection (LOD, IC 10 ) of clothianidin were 25.6 and 3.8 ng mL − 1 for ELISA. GICA using colloidal gold-MAb probe had a visual detection limit of 8 ng mL − 1 , and the results can be judged by the naked eye within 10 min. The cross-reactivities of the immunoassays with its analogues were negligible except for that with dinotefuran. For the spiked agricultural samples, recoveries of 78.0 to 114.5% with relative standard deviations (RSDs) of 3.2 to 12.8% were achieved for ELISA and further evaluated by GICA. Furthermore, the results of ELISA and GICA for the authentic samples correlated well with those obtained by HPLC . Overall, the proposed ELISA and GICA are satisfactory for rapid, sensitive, and quantitative/semiquantitative detection of clothianidin residues in agricultural samples.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2025
·
IF 6.2
Yulun Chen,Linquan Wang,Aying Wen,Hang Yu,Yahui Guo,Yuliang Cheng,Weirong Yao,Shaofeng Yuan
Matrix binding poses a challenge to accurate pesticide residue detection in fruits and vegetables. This study investigated the distribution, binding status, and detection accuracy of neonicotinoid insecticides thiamethoxam (TMX) and clothianidin (CLO) in eggplant. To address the limitations posed by matrix binding, a pectinase-assisted extraction method was developed, which significantly enhanced the detectable levels of pesticides compared to the standard method and cellulase-assisted extraction. In situ Raman mapping and scanning electron microscopy revealed a strong correlation between the pectin distribution and the pesticide residues observed near the epidermal surface. Spectroscopic, nuclear magnetic resonance, and computational chemistry analyses demonstrated that TMX formed covalent bonds with pectin, while CLO interacted through hydrogen bonding. Notably, thermal processing promoted the formation of amide bonds, reducing detectable TMX levels. In summary, the optimized pectinase-assisted extraction method increased detectable TMX and CLO levels in positive samples by 25–40%, providing an effective approach for overcoming matrix binding effects.
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高影响因子
PESTICIDE BIOCHEMISTRY AND PHYSIOLOGY
·
2024
·
IF 4.2
Zhiyuan Meng,Zixin Yan,Ruixian Yang,Xinyi Wu,Xiuli Zhang,Hui Pan,Xin Bao,Li Liu,Xiaojun Chen
The widespread application of neonicotinoid insecticides (NNIs) has attracted widespread attention to their potential ecotoxicological effects. In this study, we systematically evaluated the toxic effects of thiamethoxam (TMX) and its metabolite clothianidin (CLO) on earthworms ( Eisenia fetida ). Specifically, the antioxidant system responses and endogenous metabolite metabolism responses in earthworms were analyzed in the temporal dimension after 7, 14, 21 and 28 days of exposure to TMX and CLO. The results found that TMX and CLO could inhibit the growth phenotype of earthworms and cause significant changes in antioxidant system related indicators. More importantly, we found that TMX and CLO could cause significant changes in the metabolic profiles of earthworms through NMR-based metabolomics. From the changes in endogenous metabolites, the toxicity effects of TMX on earthworms gradually increases with prolonged exposure time. Differently, the toxicity effects of CLO on earthworms is significantly higher than that of TMX in the early stages of exposure. Meanwhile, these impacts will not weaken with prolonged exposure time. Furthermore, the results of KEGG enrichment pathway analysis indicated that TMX and CLO could significantly interfere with energy homeostasis, redox homeostasis, osmotic regulation, amino acid metabolism and protein synthesis in earthworms. These findings further deepen our understanding of the ecotoxicological effects of NNIs on soil organism.
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高影响因子
Environmental Technology & Innovation
·
2024
·
IF 6.7
Rui Zhao,Zheng Zhang,Meng Yu,Rui Gao,Zhe Sun,Shou-he Pan,Ying-jian Ma,Yong Xu,Xue-min Wu
Pine wilt disease (PWD) is one of the most destructive diseases affecting global forest ecosystems, and Monochamus alternatus (MA) is the main insect vector of pine wood nematodes. Effective control methods that cover the entire emergence period of vector insects are urgently required. Improving the rainfastness of agrochemicals on leaves can extend the holding period. Thus, a new environmentally friendly castor oil-based polyurethane nanoemulsion (CWPU-NE) was developed to enhance the rainfastness of clothianidin. CWPU adsorbs on the surface of clothianidin particles through electrostatic and intermolecular hydrogen bonding and attaches to the surface of leaves through hydrogen bonding and film formation. The results showed that clothianidin was still effective against MA 60 d after application. The developed CWPU-NE functioned as an efficient rainfastness adjuvant that enhanced the rainfastness, retention, protection, and sustained release behavior of clothianidin. Thus, it has great potential for PWD control and wider agricultural applications.
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FOOD CONTROL
·
2025
·
IF 6.3
Lijun Wang,Zhenni Yu,Yi Li,Jing Cao,Xiao Yang,Xianggui Chen
Thiamethoxam (TMX) and its metabolite clothianidin (CLO) represent significant risks to both ecological systems and human health. Consequently, it is vital to establish straightforward, specific, and sensitive techniques for detecting them to protect public health. This research introduced a dual-mode strategy that employed colorimetric and fluorescent methods for homogeneous detection of TMX and CLO, utilizing the inhibition of single-atom nanozyme activity mediated by carbon dots (CDs) along with the internal filter effect (IFE). Fe/Co single atoms anchored on N-doped carbon material (Fe/Co-N-C), which exhibited peroxidase-like activity, was functionalized with an aptamer (Apt), and orange-emitting CDs (O-CDs, fluorescence peak at 574 nm) were conjugated with complementary strands (CS), to obtain the Fe/Co-N-C/Apt-CS/O-CDs complex. In the absence of targets, CS/O-CDs suppressed the peroxidase-like activity of the Fe/Co-N-C/Apt by inhibiting the Fe/Co-N-C/Apt probe-substrates interaction and scavenging existing •OH, while retaining their own strong fluorescence. Upon introduction of TMX/CLO, the CS/O-CDs dissociated from the Fe/Co-N-C/Apt, which restored the significant peroxidase-like activity of the Fe/Co-N-C/Apt, enabling it to catalyze H 2 O 2 -mediated 3,3′,5,5′-tetramethylbenzidine (TMB) oxidation to blue oxidized TMB (oxTMB). Consequently, oxTMB quenched the O-CDs fluorescence via the IFE. Under optimized conditions, the proposed method achieved detection limits of 8.30 μg/L (TMX) and 7.52 μg/L (CLO) by fluorescence, and 11.05 μg/L (TMX) and 11.33 μg/L (CLO) by colorimetry. Recoveries in spiked food samples ranged from 87.36 % to 98.80 %, comparable to those obtained by liquid chromatography-tandem mass spectrometry. These results demonstrate the significant promise of this strategy for sensitive and reliable on-site detection of TMX and CLO residues.
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TALANTA
·
2023
·
IF 6.1
Hongqin Yang,Lian Xia,Jia Zheng,Zhengmin Xie,Jianli Zhou,Yuangen Wu
Clothianidin pesticide not only pollutes the ecological environment, but also poses a potential threat to human health. Thus, it is of great importance to develop efficient and accurate methods to recognize and detect clothianidin residues in agricultural products. Aptamer has the advantages of easy modification, high affinity and good stability, which is particularly suitable as a recognition biomolecule for pesticide detection. However, the aptamer against clothianidin has not been reported. Herein, the aptamer (named CLO-1) had good selectivity and strong affinity ( K d = 40.66 ± 3.47 nM) to clothianidin pesticide, which was screened for the first time by Capture-SELEX strategy. The binding effect of CLO-1 aptamer to clothianidin was further studied by circular dichroism (CD) spectroscopy and molecular docking technique. Finally, the CLO-1 aptamer was used as the recognition molecule to construct a label-free fluorescent aptasensor using GeneGreen dye as sensing signal for the highly sensitive detection of clothianidin pesticide. The constructed fluorescent aptasensor had the limit of detection (LOD) as low as 5.527 μg L −1 for clothianidin, and displayed good selectivity against other competitive pesticides. The aptasensor was applied to detect the clothianidin spiked in tomatoes, pears and cabbages, and the recovery rate was good in the range of 81.99%–106.64%. This study provides a good application prospect for the recognition and detection of clothianidin.
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高影响因子
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