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Radiolysis and Radiation-Driven Dynamics of Boehmite Dissolution Observed by In Situ Liquid-Phase TEM

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    Contaminants in Aquatic and Terrestrial Environments

    Radiolysis and Radiation-Driven Dynamics of Boehmite Dissolution Observed by In Situ Liquid-Phase TEM
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    Environmental Science & Technology

    Cite this: Environ. Sci. Technol. 2022, 56, 8, 5029–5036
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    https://doi.org/10.1021/acs.est.1c08415
    Published April 7, 2022
    Copyright © 2022 American Chemical Society
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    Abstract

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    Over the last several decades, there have been several studies examining the radiation stability of boehmite and other aluminum oxyhydroxides, yet less is known about the impact of radiation on boehmite dissolution. Here, we investigate radiation effects on the dissolution behavior of boehmite by employing liquid-phase transmission electron microscopy (LPTEM) and varying the electron flux on the samples consisting of either single nanoplatelets or aggregated stacks. We show that boehmite nanoplatelets projected along the [010] direction exhibit uniform dissolution with a strong dependence on the electron dose rate. For nanoplatelets that have undergone oriented aggregation, we show that the dissolution occurs preferentially at the particles at the ends of the stacks that are more accessible to bulk solution than at the others inside the aggregate. In addition, at higher dose rates, electrostatic repulsion and knock-on damage from the electron beam causes delamination of the stacks and dissolution at the interfaces between particles in the aggregate, indicating that there is a threshold dose rate for electron-beam enhancement of dissolution of boehmite aggregates.

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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.1c08415.

    • The supporting information is available free of charge on the ACS publication websites. Additional figures and movies are presented (PDF)

    • Boehmite nanoplatelets remained largely unchanged even after a 150 s exposure to the electron beam at a dose rate of 2.5 e/(Å2s) (Movie S1) (AVI)

    • The electron beam dose was incresed to 4.5 e/(Å2s), the nanoplatelets continuously dissolved along both directions and eventually disappeared (Movie S2) (AVI)

    • The electron beam dose was incresed to 6.0 e/(Å2s), the nanoplatelets continuously dissolved along both directions and eventually disappeared (Movie S3) (AVI)

    • Figure 4A shows images of an aggregate of five NPs at several times during irradiation, with a dose rate of 3.8 e/(Å2s) (Movie S4) (AVI)

    • For the aggregate shown in Figure 4 A, increasing the dose rate to 5 e/(Å2s) led to its breakup and dissolution (Movie S5) (AVI)

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    Cited By

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    This article is cited by 7 publications.

    1. Yatong Zhao, Ping Chen, Xiang Wang, Hanna Hlushko, Jay A. LaVerne, Lili Liu, Carolyn I. Pearce, Zheming Wang, Kevin M. Rosso, Xin Zhang. Effect of 60Co Irradiation on Boehmite Dissolution in Caustic Solutions. Environmental Science & Technology 2024, Article ASAP.
    2. Yuhang Wang, Dewansh Rastogi, Kotiba A. Malek, Jiayue Sun, Martin Changman Ahn, Akua A. Asa-Awuku, Taylor J. Woehl. Imaging Dissolution Dynamics of Individual NaCl Nanoparticles during Deliquescence with In Situ Transmission Electron Microscopy. Environmental Science & Technology 2024, 58 (35) , 15551-15561. https://doi.org/10.1021/acs.est.4c02356
    3. Ping Chen, Yifeng Zhu, Rachael Bergman, Sichuang Xue, Yatong Zhao, Jay A. LaVerne, Xiaofeng Guo, Carolyn I. Pearce, Zheming Wang, Tianhu Chen, Kevin M. Rosso, Xin Zhang. Effects of Ionizing Radiation on the Thermodynamic Stability of Boehmite and Gibbsite. The Journal of Physical Chemistry C 2024, 128 (8) , 3578-3587. https://doi.org/10.1021/acs.jpcc.3c08456
    4. Yatong Zhao, Qing Guo, Sichuang Xue, Ping Chen, Qian Zhao, Lili Liu, Hanna Hlushko, Jay LaVerne, Carolyn I. Pearce, Aijun Miao, Zheming Wang, Kevin M. Rosso, Xin Zhang. Effect of Adsorbed Carboxylates on the Dissolution of Boehmite Nanoplates in Highly Alkaline Solutions. Environmental Science & Technology 2024, 58 (4) , 2017-2026. https://doi.org/10.1021/acs.est.3c06595
    5. Yanfu Wei, Peng Yuan, Junming Zhou, Jing Liu, Dusan Losic, Honghai Wu, Hongling Bu, Xinjie Tan, Zheng Li. Direct Atomic-Scale Insight into the Precipitation Formation at the Lanthanum Hydroxide Nanoparticle/Solution Interface. The Journal of Physical Chemistry Letters 2023, 14 (17) , 3995-4003. https://doi.org/10.1021/acs.jpclett.3c00336
    6. Lili Liu, Karen Kruska, Gabriel B. Hall, Richard A. Clark, David E. Meier, Edgar C. Buck. Formation and growth of cerium (III) oxalate nanocrystals by liquid-cell transmission electron microscopy. Scripta Materialia 2022, 219 , 114856. https://doi.org/10.1016/j.scriptamat.2022.114856
    7. Junyu Zhang, Zhefei Sun, Zewen Kang, Haichen Lin, Haodong Liu, Yang He, Zhiyuan Zeng, Qiaobao Zhang. Unveiling the Dynamic Oxidative Etching Mechanisms of Nanostructured Metals/Metallic Oxides in Liquid Media Through In Situ Transmission Electron Microscopy. Advanced Functional Materials 2022, 32 (36) , 2204976. https://doi.org/10.1002/adfm.202204976
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    Environmental Science & Technology

    Cite this: Environ. Sci. Technol. 2022, 56, 8, 5029–5036
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.est.1c08415
    Published April 7, 2022
    Copyright © 2022 American Chemical Society
    Request reuse permissions

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