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Title: Effect of calcination temperature on neptunium dioxide microstructure and dissolution

Abstract

Comprehensive thermodynamic understanding of nuclear materials is paramount for long-term management of legacy nuclear waste and commercial spent nuclear fuel. Actinide oxides (AnO2(s)) are ubiquitous materials throughout the nuclear fuel cycle, yet existing thermodynamic data has noticeable discrepancies, creating uncertainty in environmental prediction of the fate of nuclear materials. The microstructure of actinide oxides, particularly neptunium (Np) and plutonium (Pu), is rarely investigated using high resolution electron microscopy, but such features may illuminate why differences in solubility measurements persist. The aim of this study was to synthesize NpO2(s) at varying calcination temperatures, characterize the materials using high resolution electron microscopy, and perform batch solubility studies to measure total dissolved Np as a function of calcination temperature. Here, the current work demonstrates the sizable differences in dissolution of NpO2(s) based on process conditions, such as the temperature at which the material is calcined and resultant particle size, and the need for more thorough evaluation of the microstructure of solid phases used to generate thermodynamic data of actinides.

Authors:
ORCiD logo [1]; ORCiD logo [2]
  1. Clemson Univ., Anderson, SC (United States)
  2. Clemson Univ., Anderson, SC (United States); Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)
Publication Date:
Research Org.:
Clemson Univ., SC (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1756008
Alternate Identifier(s):
OSTI ID: 1737655
Grant/Contract Number:  
SC0012530; SC00012530
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Environmental Science: Nano
Additional Journal Information:
Journal Volume: 7; Journal Issue: 12; Related Information: https://doi.org/10.1039/D0EN00689K; Journal ID: ISSN 2051-8153
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; 36 MATERIALS SCIENCE; 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; 54 ENVIRONMENTAL SCIENCES; 77 NANOSCIENCE AND NANOTECHNOLOGY; Neptunium dioxide; solubility; particle size; actinides

Citation Formats

Peruski, Kathryn M., and Powell, Brian A. Effect of calcination temperature on neptunium dioxide microstructure and dissolution. United States: N. p., 2020. Web. doi:10.1039/d0en00689k.
Peruski, Kathryn M., & Powell, Brian A. Effect of calcination temperature on neptunium dioxide microstructure and dissolution. United States. https://doi.org/10.1039/d0en00689k
Peruski, Kathryn M., and Powell, Brian A. 2020. "Effect of calcination temperature on neptunium dioxide microstructure and dissolution". United States. https://doi.org/10.1039/d0en00689k. https://www.osti.gov/servlets/purl/1756008.
@article{osti_1756008,
title = {Effect of calcination temperature on neptunium dioxide microstructure and dissolution},
author = {Peruski, Kathryn M. and Powell, Brian A.},
abstractNote = {Comprehensive thermodynamic understanding of nuclear materials is paramount for long-term management of legacy nuclear waste and commercial spent nuclear fuel. Actinide oxides (AnO2(s)) are ubiquitous materials throughout the nuclear fuel cycle, yet existing thermodynamic data has noticeable discrepancies, creating uncertainty in environmental prediction of the fate of nuclear materials. The microstructure of actinide oxides, particularly neptunium (Np) and plutonium (Pu), is rarely investigated using high resolution electron microscopy, but such features may illuminate why differences in solubility measurements persist. The aim of this study was to synthesize NpO2(s) at varying calcination temperatures, characterize the materials using high resolution electron microscopy, and perform batch solubility studies to measure total dissolved Np as a function of calcination temperature. Here, the current work demonstrates the sizable differences in dissolution of NpO2(s) based on process conditions, such as the temperature at which the material is calcined and resultant particle size, and the need for more thorough evaluation of the microstructure of solid phases used to generate thermodynamic data of actinides.},
doi = {10.1039/d0en00689k},
url = {https://www.osti.gov/biblio/1756008}, journal = {Environmental Science: Nano},
issn = {2051-8153},
number = 12,
volume = 7,
place = {United States},
year = {Mon Oct 19 00:00:00 EDT 2020},
month = {Mon Oct 19 00:00:00 EDT 2020}
}

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