Effect of 60Co Irradiation on Boehmite Dissolution in Caustic Solutions

Environ Sci Technol. 2024 Dec 10;58(49):21760-21769. doi: 10.1021/acs.est.4c07544. Epub 2024 Nov 26.

Abstract

Here, we examine how radiation impacts the dissolution behavior of boehmite by subjecting dry nanoparticles of different sizes to 60Co 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-1 at 60 °C), with an apparent activation energy 40 kJ mol-1 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.

Keywords: 60Co irradiation; boehmite; dissolution; kinetics; nuclear waste; γ-irradiation.

MeSH terms

  • Aluminum Hydroxide* / chemistry
  • Aluminum Oxide* / chemistry
  • Cobalt Radioisotopes / chemistry
  • Gamma Rays
  • Kinetics
  • Solubility
  • Solutions
  • Temperature
  • X-Ray Diffraction

Substances

  • Aluminum Oxide
  • Aluminum Hydroxide
  • aluminum oxide hydroxide
  • Cobalt Radioisotopes
  • Solutions