Direct glyphosate soil monitoring at the triazine-based covalent organic framework with the theoretical study of sensing principle
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2023
Authors
Knežević, Sara
Terzić Jovanović, Nataša
Vlahović, Filip

Ajdačić, Vladimir
Costache, Vlad
Vidić, Jasmina
Opsenica, Igor
Stanković, Dalibor

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Covalent organic frameworks (COFs) are emerging as promising sensing materials due to their controllable structure and function properties, as well as excellent physicochemical characteristics. Here, specific interactions between a triazine-based COF and a mass-used herbicide – glyphosate (GLY) have been utilized to design a disposable sensing platform for GLY detection. This herbicide has been extensively used for decades, however, its harmful environmental impact and toxicity to humans have been recently proven, conditioning the necessity for the strict control and monitoring of its use and its presence in soil, water, and food. Glyphosate is an organophosphorus compound, and its detection in complex matrices usually requires laborious pretreatment. Here, we developed a direct, miniaturized, robust, and green approach for disposable electrochemical sensing of glyphosate, utilizing COF’s ability to selectively capture and concentrate negatively charged glyphosate molecules inside its ...nanopores. This process generates the concentration gradient of GLY, accelerating its diffusion towards the electrode surface. Simultaneously, specific COF-glyphosate binding catalyses the oxidative cleavage of the C–P bond and, together with pore nanoconfinement, enables sensitive glyphosate detection. Detailed sensing principles and selectiveness were scrutinized using DFT-based modelling. The proposed electrochemical method has a linear working range from 0.1 μM to 10 μM, a low limit of detection of 96 nM, and a limit of quantification of 320 nM. The elaborated sensing approach is viable for use in real sample matrices and tested for GLY determination in soil and water samples, without pretreatment, preparation, or purification. The results showed the practical usefulness of the sensor in the real sample analysis and suggested its suitability for possible out-oflaboratory sensing.
Keywords:
Environmental monitoring / Disposable sensing / Emerging pollutant / Electrochemical sensor / Density functional theorySource:
Chemosphere, 2023, 341, 139930-Funding / projects:
DOI: 10.1016/j.chemosphere.2023.139930
ISSN: 0045-6535
PubMed: 37659506
Scopus: 2-s2.0-85169541358
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VinčaTY - JOUR AU - Knežević, Sara AU - Terzić Jovanović, Nataša AU - Vlahović, Filip AU - Ajdačić, Vladimir AU - Costache, Vlad AU - Vidić, Jasmina AU - Opsenica, Igor AU - Stanković, Dalibor PY - 2023 UR - https://vinar.vin.bg.ac.rs/handle/123456789/11546 AB - Covalent organic frameworks (COFs) are emerging as promising sensing materials due to their controllable structure and function properties, as well as excellent physicochemical characteristics. Here, specific interactions between a triazine-based COF and a mass-used herbicide – glyphosate (GLY) have been utilized to design a disposable sensing platform for GLY detection. This herbicide has been extensively used for decades, however, its harmful environmental impact and toxicity to humans have been recently proven, conditioning the necessity for the strict control and monitoring of its use and its presence in soil, water, and food. Glyphosate is an organophosphorus compound, and its detection in complex matrices usually requires laborious pretreatment. Here, we developed a direct, miniaturized, robust, and green approach for disposable electrochemical sensing of glyphosate, utilizing COF’s ability to selectively capture and concentrate negatively charged glyphosate molecules inside its nanopores. This process generates the concentration gradient of GLY, accelerating its diffusion towards the electrode surface. Simultaneously, specific COF-glyphosate binding catalyses the oxidative cleavage of the C–P bond and, together with pore nanoconfinement, enables sensitive glyphosate detection. Detailed sensing principles and selectiveness were scrutinized using DFT-based modelling. The proposed electrochemical method has a linear working range from 0.1 μM to 10 μM, a low limit of detection of 96 nM, and a limit of quantification of 320 nM. The elaborated sensing approach is viable for use in real sample matrices and tested for GLY determination in soil and water samples, without pretreatment, preparation, or purification. The results showed the practical usefulness of the sensor in the real sample analysis and suggested its suitability for possible out-oflaboratory sensing. T2 - Chemosphere T1 - Direct glyphosate soil monitoring at the triazine-based covalent organic framework with the theoretical study of sensing principle VL - 341 SP - 139930 DO - 10.1016/j.chemosphere.2023.139930 ER -
@article{ author = "Knežević, Sara and Terzić Jovanović, Nataša and Vlahović, Filip and Ajdačić, Vladimir and Costache, Vlad and Vidić, Jasmina and Opsenica, Igor and Stanković, Dalibor", year = "2023", abstract = "Covalent organic frameworks (COFs) are emerging as promising sensing materials due to their controllable structure and function properties, as well as excellent physicochemical characteristics. Here, specific interactions between a triazine-based COF and a mass-used herbicide – glyphosate (GLY) have been utilized to design a disposable sensing platform for GLY detection. This herbicide has been extensively used for decades, however, its harmful environmental impact and toxicity to humans have been recently proven, conditioning the necessity for the strict control and monitoring of its use and its presence in soil, water, and food. Glyphosate is an organophosphorus compound, and its detection in complex matrices usually requires laborious pretreatment. Here, we developed a direct, miniaturized, robust, and green approach for disposable electrochemical sensing of glyphosate, utilizing COF’s ability to selectively capture and concentrate negatively charged glyphosate molecules inside its nanopores. This process generates the concentration gradient of GLY, accelerating its diffusion towards the electrode surface. Simultaneously, specific COF-glyphosate binding catalyses the oxidative cleavage of the C–P bond and, together with pore nanoconfinement, enables sensitive glyphosate detection. Detailed sensing principles and selectiveness were scrutinized using DFT-based modelling. The proposed electrochemical method has a linear working range from 0.1 μM to 10 μM, a low limit of detection of 96 nM, and a limit of quantification of 320 nM. The elaborated sensing approach is viable for use in real sample matrices and tested for GLY determination in soil and water samples, without pretreatment, preparation, or purification. The results showed the practical usefulness of the sensor in the real sample analysis and suggested its suitability for possible out-oflaboratory sensing.", journal = "Chemosphere", title = "Direct glyphosate soil monitoring at the triazine-based covalent organic framework with the theoretical study of sensing principle", volume = "341", pages = "139930", doi = "10.1016/j.chemosphere.2023.139930" }
Knežević, S., Terzić Jovanović, N., Vlahović, F., Ajdačić, V., Costache, V., Vidić, J., Opsenica, I.,& Stanković, D.. (2023). Direct glyphosate soil monitoring at the triazine-based covalent organic framework with the theoretical study of sensing principle. in Chemosphere, 341, 139930. https://doi.org/10.1016/j.chemosphere.2023.139930
Knežević S, Terzić Jovanović N, Vlahović F, Ajdačić V, Costache V, Vidić J, Opsenica I, Stanković D. Direct glyphosate soil monitoring at the triazine-based covalent organic framework with the theoretical study of sensing principle. in Chemosphere. 2023;341:139930. doi:10.1016/j.chemosphere.2023.139930 .
Knežević, Sara, Terzić Jovanović, Nataša, Vlahović, Filip, Ajdačić, Vladimir, Costache, Vlad, Vidić, Jasmina, Opsenica, Igor, Stanković, Dalibor, "Direct glyphosate soil monitoring at the triazine-based covalent organic framework with the theoretical study of sensing principle" in Chemosphere, 341 (2023):139930, https://doi.org/10.1016/j.chemosphere.2023.139930 . .