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Effect of Cr(III) Adsorption on the Dissolution of Boehmite Nanoparticles in Caustic Solution
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    Effect of Cr(III) Adsorption on the Dissolution of Boehmite Nanoparticles in Caustic Solution
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    • Wenwen Cui
      Wenwen Cui
      Physical & Computational Science Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United States
      National Engineering Laboratory for Hydrometallurgical Cleaner Production Technology, Key Laboratory of Green Process and Engineering, Institute of Process Engineering, Chinese Academy of Sciences, Beijing, 100190, China
      University of Chinese Academy of Sciences, Beijing, 100049, China
      More by Wenwen Cui
    • Xin Zhang*
      Xin Zhang
      Physical & Computational Science Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United States
      *Email: [email protected]
      More by Xin Zhang
    • Carolyn I. Pearce
      Carolyn I. Pearce
      Energy & Environment Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United States
    • Mark H. Engelhard
      Mark H. Engelhard
      Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, Washington 99354, United States
    • Hailin Zhang
      Hailin Zhang
      Physical & Computational Science Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United States
      National Engineering Laboratory for Hydrometallurgical Cleaner Production Technology, Key Laboratory of Green Process and Engineering, Institute of Process Engineering, Chinese Academy of Sciences, Beijing, 100190, China
      University of Chinese Academy of Sciences, Beijing, 100049, China
      More by Hailin Zhang
    • Yining Wang
      Yining Wang
      Physical & Computational Science Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United States
      More by Yining Wang
    • Steve M. Heald
      Steve M. Heald
      Advanced Photon Source, Argonne National Laboratory, Lemont, Illinois 60439, United States
    • Shili Zheng
      Shili Zheng
      National Engineering Laboratory for Hydrometallurgical Cleaner Production Technology, Key Laboratory of Green Process and Engineering, Institute of Process Engineering, Chinese Academy of Sciences, Beijing, 100190, China
      More by Shili Zheng
    • Yi Zhang
      Yi Zhang
      National Engineering Laboratory for Hydrometallurgical Cleaner Production Technology, Key Laboratory of Green Process and Engineering, Institute of Process Engineering, Chinese Academy of Sciences, Beijing, 100190, China
      More by Yi Zhang
    • Sue B. Clark
      Sue B. Clark
      Energy & Environment Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United States
      Department of Chemistry, Washington State University, Pullman, Washington 99164, United States
      More by Sue B. Clark
    • Ping Li*
      Ping Li
      National Engineering Laboratory for Hydrometallurgical Cleaner Production Technology, Key Laboratory of Green Process and Engineering, Institute of Process Engineering, Chinese Academy of Sciences, Beijing, 100190, China
      *Email: [email protected]
      More by Ping Li
    • Zheming Wang*
      Zheming Wang
      Physical & Computational Science Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United States
      *Email: [email protected]
      More by Zheming Wang
    • Kevin M. Rosso*
      Kevin M. Rosso
      Physical & Computational Science Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United States
      *Email: [email protected]
    Other Access OptionsSupporting Information (1)

    Environmental Science & Technology

    Cite this: Environ. Sci. Technol. 2020, 54, 10, 6375–6384
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.est.9b07881
    Published April 16, 2020
    Copyright © 2020 American Chemical Society

    Abstract

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    The incorporation of relatively minor impurity metals onto metal (oxy)hydroxides can strongly impact solubility. In complex highly alkaline multicomponent radioactive tank wastes such as those at the Hanford Nuclear Reservation, tests indicate that the surface area-normalized dissolution rate of boehmite (γ-AlOOH) nanomaterials is at least an order of magnitude lower than that predicted for the pure phase. Here, we examine the dissolution kinetics of boehmite coated by adsorbed Cr(III), which adheres at saturation coverages as sparse chemisorbed monolayer clusters. Using 40 nm boehmite nanoplates as a model system, temperature-dependent dissolution rates of pure versus Cr(III)-adsorbed boehmite showed that the initial rate for the latter is consistently several times lower, with an apparent activation energy 16 kJ·mol–1 higher. Although the surface coverage is only around 50%, solution analysis coupled to multimethod solids characterization reveal a phyicochemical armoring effect by adsorbed Cr(III) that substantially reduces the number of dissolution-active sites on particle surfaces. Such findings could help improve kinetics models of boehmite and/or metal ion adsorbed boehmite nanomaterials, ultimately providing a stronger foundation for the development of more robust complex radioactive liquid waste processing strategies.

    Copyright © 2020 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.est.9b07881.

    • SEM images for boehmite and Cr(III)-adsorbed boehmite in various stages of dissolution process with increasing time; Arrhenius curve for boehmite and Cr(III)-adsorbed boehmite via using total Al and Cr concentration in solutions; kinetic parameters of boehmite and Cr(III)-adsorbed boehmite via using total Al and Cr concentration in solutions (PDF)

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    Cited By

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    This article is cited by 13 publications.

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    Environmental Science & Technology

    Cite this: Environ. Sci. Technol. 2020, 54, 10, 6375–6384
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.est.9b07881
    Published April 16, 2020
    Copyright © 2020 American Chemical Society

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