کد مقاله | کد نشریه | سال انتشار | مقاله انگلیسی | نسخه تمام متن |
---|---|---|---|---|
1859340 | 1530605 | 2012 | 5 صفحه PDF | دانلود رایگان |
![عکس صفحه اول مقاله: The environmental dependence of redox energetics of PuO2 and α-Pu2O3: A quantitative solution from DFT+UDFT+U The environmental dependence of redox energetics of PuO2 and α-Pu2O3: A quantitative solution from DFT+UDFT+U](/preview/png/1859340.png)
We report a comprehensive density functional theory (DFT)+U(DFT)+U study of the energetics of charged and neutral oxygen defects in both PuO2 and α-Pu2O3, and present a quantitative determination of the equilibrium compositions of reduced PuO2 (PuO2 − x) as functions of environmental temperature and partial pressure of oxygen, which shows fairly agreement with corresponding high-temperature experiments. Under ambient conditions, the endothermic reduction of PuO2 to α-Pu2O3 is found to be facilitated by accompanying volume expansion of PuO2 − x and the possible migration of O-vacancy, whereas further reduction of α-Pu2O3 is predicted to be much more difficult. In contrast to the endothermic oxidation of PuO2, the oxidation of α-Pu2O3 is a stable exothermic process.
► We provide defect physics study.
► A quantitative study of PuO2 − x phase is presented.
► We provide detailed redox property.
Journal: Physics Letters A - Volume 376, Issues 40–41, 20 August 2012, Pages 2672–2676