Impact Factor:

12.2

DOI number:

10.1021/acs.est.4c07

Journal:

Environmental Science & Technology

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.

Co-author:

Ping Chen, Xiang Wang, Hanna Hlushko, Jay A LaVerne, Lili Liu, Carolyn I Pearce, Zheming Wang

First Author:

Yatong Zhao

Indexed by:

Journal paper

Correspondence Author:

Kevin M Rosso, Xin Zhang

Discipline:

Engineering

Document Type:

J

Volume:

58

Issue:

49

Page Number:

21760-21769

Translation or Not:

no

Date of Publication:

2024-11-26

Included Journals:

SCI

Links to published journals:

https://pubs.acs.org/doi/full/10.1021/acs.est.4c07544