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Redox-Based Electrochemical Affinity Sensor for Detection of Aqueous Pertechnetate Anion

  • Sayandev Chatterjee*
    Sayandev Chatterjee
    Energy and Environment Directorate, Pacific Northwest National Laboratory, Richland, Washington 99352, United States
    *E-mail: [email protected]
  • Meghan S. Fujimoto
    Meghan S. Fujimoto
    Energy and Environment Directorate, Pacific Northwest National Laboratory, Richland, Washington 99352, United States
  • Yingge Du
    Yingge Du
    Environmental and Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, Washington 99352, United States
    More by Yingge Du
  • Gabriel B. Hall
    Gabriel B. Hall
    Energy and Environment Directorate, Pacific Northwest National Laboratory, Richland, Washington 99352, United States
  • Nabajit Lahiri
    Nabajit Lahiri
    Environmental and Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, Washington 99352, United States
  • Eric D. Walter
    Eric D. Walter
    Environmental and Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, Washington 99352, United States
  • , and 
  • Libor Kovarik
    Libor Kovarik
    Environmental and Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, Washington 99352, United States
Cite this: ACS Sens. 2020, 5, 3, 674–685
Publication Date (Web):February 7, 2020
https://doi.org/10.1021/acssensors.9b01531
Copyright © 2020 American Chemical Society

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    Abstract

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    Rapid, selective, and in situ detection of pertechnetate (TcO4) in multicomponent matrices consisting of interfering anions such as the ubiquitous NO3 and Cl or the isostructural CrO42– is challenging. Present sensors lack the selectivities to exclude these interferences or the sensitivities to meet detection limits that are lower than the drinking water standards across the globe. This work presents an affinity-based electrochemical sensor for TcO4 detection that relies on selective reductive precipitation of aqueous TcO4 induced by a 1,4-benzenedimethanethiol capture probe immobilized on an electrode platform. This results in a direct decrease in the electron transfer current, the magnitude of the decrease being proportional to the amount of TcO4 added. Using this approach, a detection limit of 1 × 10–10 M was achieved, which is lower than the drinking water standard of 5.2 × 10–10 M set by United States Environmental Protection Agency. The proposed approach shows selectivity to the TcO4 anion, allowing detection of TcO4 from a multicomponent groundwater sample obtained from a well at the Hanford site in Washington (well 299-W19-36) that also contained NO3, Cl, and CrO42–, without discernably affecting the detection limits.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acssensors.9b01531.

    • Table for major contaminants present in the well 299-W19-36 at the Hanford site in Washington, voltammogram comparisons of 0.5 mM [Fe(CN)6]4–/3– in 0.1 M KNO3 using uncoated and 1,4-benzenedimethanethiol-coated gold working electrode in the absence of TcO4, voltammetric profile of 1,4-benzenedimethanethiol-coated gold working electrode in 0.1 M KNO3, plot for dependence of peak current intensity ratios with TcO4 exposure time as a function of pH values, DPVs of 0.5 mM [Fe(CN)6]4–/3– in 0.1 M KNO3 using 1,4-benzenedimethanethiol-coated gold working electrode post exposure to 2 mM of different anions, and for TcO4 exposure, 0.2 mM TcO4 was used (PDF)

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    Cited By

    This article is cited by 6 publications.

    1. Amie E. Norton, Malvika Sharma, Christina Cashen, Marie-Anne Dourges, Thierry Toupance, Jeanette A. Krause, Radha Kishan Motkuri, William B. Connick, Sayandev Chatterjee. pH-Mediated Colorimetric and Luminescent Sensing of Aqueous Nitrate Anions by a Platinum(II) Luminophore@Mesoporous Silica Composite. ACS Applied Materials & Interfaces 2021, 13 (14) , 16197-16209. https://doi.org/10.1021/acsami.0c20821
    2. Sayandev Chatterjee, Vanessa E. Holfeltz, Gabriel B. Hall, Isaac E. Johnson, Eric D. Walter, Sungsik Lee, Benjamin Reinhart, Wayne W. Lukens, Nicholas P. Machara, Tatiana G. Levitskaia. Identification and Quantification of Technetium Species in Hanford Waste Tank AN-102. Analytical Chemistry 2020, 92 (20) , 13961-13970. https://doi.org/10.1021/acs.analchem.0c02864
    3. Mun Ryul Choi, Byunghwan Lee. Synthesis of cationic carbon quantum dot-based dual emission fluorescence sensor for detecting perrhenate anions in aqueous solutions. Optical Materials 2022, 134 , 113190. https://doi.org/10.1016/j.optmat.2022.113190
    4. Amie E. Norton, Mahmood Karimi Abdolmaleki, Daoli Zhao, Stephen D. Taylor, Steven R. Kennedy, Trevor D. Ball, Mark O. Bovee, William B. Connick, Sayandev Chatterjee. Vapoluminescence hysteresis in a platinum(II) salt-based humidity sensor: Mapping the vapochromic response to water vapor. Sensors and Actuators B: Chemical 2022, 359 , 131502. https://doi.org/10.1016/j.snb.2022.131502
    5. Fengqin Wang, Fengxiao Zhang, Zhongrui Zhao, Zhenyu Sun, Yanyan Pu, Yanjun Wang, Xiaoqing Wang. Multifunctional MOF-based probes for efficient detection and discrimination of Pb 2+ , Fe 3+ and Cr 2 O 7 2− /CrO 4 2−. Dalton Transactions 2021, 50 (35) , 12197-12207. https://doi.org/10.1039/D1DT01446C
    6. Amie E. Norton, Mahmood Karimi Abdolmaleki, Jessica M. Ringo, Vikas M. Shingade, Christina Cashen, Malvika Sharma, William B. Connick, Sayandev Chatterjee. A colorimetric/luminescence sensor for detecting MeCN in water: Towards direct detection of dissolved organic contaminants. Sensors and Actuators B: Chemical 2021, 329 , 129207. https://doi.org/10.1016/j.snb.2020.129207