Effect of <sup>60</sup>Co Irradiation on Boehmite Dissolution in Caustic Solutions

Here, we examine how radiation impacts the dissolution behavior of boehmite by subjecting dry nanoparticles of different sizes to <sup>60</sup>Co γ radiation and subsequently analyzing their dissolution behavior in caustic solutions as a function of temperature. The measured kinetics show that irradiation with an amount 228.24 Mrad significantly slows the dissolution rate, particularly for smaller sizes at lower temperatures. Specifically, the temperature-dependent dissolution rates of irradiated 20 nm boehmite versus pristine material in 3 M NaOH solutions were several times lower (e.g., rate constant of 0.026 vs 0.075 h<sup>-1</sup> at 60 °C), with an apparent activation energy 40 kJ mol<sup>-1</sup> higher. Although various imaging techniques and X-ray diffraction measurements consistently revealed no obvious differences between pristine and irradiated samples, after irradiation significant binding energy shifts were detected in the X-ray photoelectron Spectroscopy peaks of Al 2p and O 1s, and a change in their relative intensities indicated a lower O/Al ratio. This suggests that γ-irradiation may stabilize boehmite particle surfaces by driving their chemistry and structure toward more stable aluminum oxide forms. This finding may help explain slower dissolution rates of boehmite in nuclear waste and may be useful for the development of more robust predictive models and effective strategies for waste processing.

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Publication Details

Journal
Environmental Science & Technology
Published
2024-11-26
DOI
https://doi.org/10.1021/acs.est.4c07544
Citations
1
Primary Topic
Radioactive element chemistry and processing
Type
article
Field-Weighted Citation Impact
0.16

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article

Effect of 60Co Irradiation on Boehmite Dissolution in Caustic Solutions

Jay A. LaVerne, Hanna Hlushko, Carolyn I. Pearce, Lili Liu et al.
1 citations
Environmental Science & Technology
Radioactive element chemistry and processing
0.16
article

Effect of 60Co Irradiation on Boehmite Dissolution in Caustic Solutions

Jay A. LaVerne, Hanna Hlushko, Carolyn I. Pearce, Lili Liu, Kevin M. Rosso, Xin Zhang, Xiang Wang, Ping Chen, Zhe-Ming Wang, Yatong Zhao
article en
1 citations

Abstract

Here, we examine how radiation impacts the dissolution behavior of boehmite by subjecting dry nanoparticles of different sizes to <sup>60</sup>Co γ radiation and subsequently analyzing their dissolution behavior in caustic solutions as a function of temperature. The measured kinetics show that irradiation with an amount 228.24 Mrad significantly slows the dissolution rate, particularly for smaller sizes at lower temperatures. Specifically, the temperature-dependent dissolution rates of irradiated 20 nm boehmite versus pristine material in 3 M NaOH solutions were several times lower (e.g., rate constant of 0.026 vs 0.075 h<sup>-1</sup> at 60 °C), with an apparent activation energy 40 kJ mol<sup>-1</sup> higher. Although various imaging techniques and X-ray diffraction measurements consistently revealed no obvious differences between pristine and irradiated samples, after irradiation significant binding energy shifts were detected in the X-ray photoelectron Spectroscopy peaks of Al 2p and O 1s, and a change in their relative intensities indicated a lower O/Al ratio. This suggests that γ-irradiation may stabilize boehmite particle surfaces by driving their chemistry and structure toward more stable aluminum oxide forms. This finding may help explain slower dissolution rates of boehmite in nuclear waste and may be useful for the development of more robust predictive models and effective strategies for waste processing.

Environmental Science & TechnologyVol. 58(49)
University of Notre Dame (US), Pacific Northwest National Laboratory (US), Washington State University (US)
U.S. Department of Energy
Openalex Percentile: Top 56%
Radioactive element chemistry and processing
0.16
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