2018
DOI: 10.1021/acs.jpcc.8b03546
|View full text |Cite
|
Sign up to set email alerts
|

Thermodynamical Stability of Plutonium Monoxide with Carbon Substitution

Abstract: The existence of condensed plutonium monoxide (PuO) has long been controversial, in which carbon element plays a vital role. In this work, we modeled PuO with carbon substitution of oxygen as the special quasirandom structures of NaCl-type plutonium monoxycarbide (PuO x C 1−x ) and performed first-principles calculations on these models. It is found that PuO could indeed be stabilized by carbon substitution. The amount of carbon element to stabilize PuO is very small if the source of carbon is CO or CO 2 . If … Show more

Help me understand this report

Search citation statements

Order By: Relevance

Paper Sections

Select...
4
1

Citation Types

3
13
0

Year Published

2019
2019
2025
2025

Publication Types

Select...
7

Relationship

2
5

Authors

Journals

citations
Cited by 11 publications
(16 citation statements)
references
References 50 publications
3
13
0
Order By: Relevance
“…Because PuN has quite a narrow composition range, the SQS is only constructed with nine points, from PuN 0.75À1.0 (Pu 32 N 24 to Pu 32 N 32 ), 31,32,36,41 using a supercell of 64 sites, which is evolved from a NaCl-type structure. 14 The local pair and multisite correlation function of the fully disordered system are regulated by Monte Carlo algorithm to generate the SQS conguration.…”
Section: Computational Detailsmentioning
confidence: 99%
See 2 more Smart Citations
“…Because PuN has quite a narrow composition range, the SQS is only constructed with nine points, from PuN 0.75À1.0 (Pu 32 N 24 to Pu 32 N 32 ), 31,32,36,41 using a supercell of 64 sites, which is evolved from a NaCl-type structure. 14 The local pair and multisite correlation function of the fully disordered system are regulated by Monte Carlo algorithm to generate the SQS conguration.…”
Section: Computational Detailsmentioning
confidence: 99%
“…Besides, the recent report of PuC 1Àx and PuO x C 1Àx gives us great condence in using theoretical methods to explore thermodynamic stability. 31,32 In this paper, the special quasirandom structure (SQS) will be applied to describe the solid solution sub-stoichiometric PuN. [31][32][33][34][35][36][37][38] All SQS's are calculated by performing rst principles calculations within the framework of density functional theory (DFT).…”
Section: Introductionmentioning
confidence: 99%
See 1 more Smart Citation
“…This is because not only are impurities ubiquitous through the lifetime of PuO 2 such as in its production, purification, fabrication, storage, application, and recovery but also the inherent radioactivity (decay and fission) of Pu results in the continuous accumulation of a large variety of transmuted products . On the whole, impurities in PuO 2 exhibit negative effects; particularly, the incompatible rare gases (RGs) have been confirmed to deteriorate the macroscopic properties of PuO 2 or other Pu-based materials despite the fact that the underlying microscopic mechanisms remain unclear. However, a few impurities are found to be beneficial; for instances, Zr can stabilize oxide-type nuclear fuels under radiation conditions and enhance their thermal conductivity, and carbon can retard or restrain Pu corrosion. Naturally, the positive effects provide guidance for tailoring the functionalities of PuO 2 , similar to the cases of its analogues such as UO 2 and CeO 2 ; in fact, U-Zr-O and Ce-Zr-O ternary compounds have been technologically and industrially used, and more ternary compounds are under validation for potential applications. Unfortunately, to our knowledge, there is still an extraordinary scarcity of relevant comprehensive studies in the literature regarding impurities in PuO 2 . In experiments, on one hand the scarcity is attributed to the difficulties in handling and preparing high-quality radioactive PuO 2 samples; on the other hand, a detailed microscopic characterization of solid-state materials doped by low-concentration impurities is quite a challenging task.…”
Section: Introductionmentioning
confidence: 99%
“…For instance, H tends to form [O 2– H + ] − in PuO 2 by binding with lattice O whereas interstitial H + is involved in UO 2 . This difference results from the dual nature of 5f electrons: Pu 5f electrons in PuO 2 are more localized and less favorable to participate in further chemical bonding or vice versa for UO 2 . , In contrast, the substitutional metal site in fluorite-type oxides such as UO 2 , ThO 2 , and CeO 2 is determined to be the exclusive site for low-concentration transition-metal (TM) impurities. , This conclusion is proposed to hold for PuO 2 despite the fact that a comprehensive study on TM behaviors in PuO 2 is lacking; the only exception is the DFT energetics and structures of Fe in PuO 2 , which partially supports the conclusion …”
Section: Introductionmentioning
confidence: 99%