Thermodynamic study on phase stability of plutonium under irradiation

Yong LU; Qiaoqiao TANG; Zheng JIANG; Xiang FENG; Cuiping WANG; Xingjun LIU

doi:10.11889/j.0253-3219.2018.hjs.41.060203

您当前的位置：

首页 >

文章列表页 >

Thermodynamic study on phase stability of plutonium under irradiation

LOW ENERGY ACCELERATOR, RAY AND APPLICATIONS | 更新时间：2021-05-19

- Thermodynamic study on phase stability of plutonium under irradiation
- NUCLEAR TECHNIQUES Vol. 41, Issue 6, Article number: 060203(2018)
- 作者机构：
  
  厦门大学材料学院厦门 361005
- 作者简介：
- 基金信息：
  
  Key Research and Development Plan of Ministry of Science and Technology;the Fundamental Research Funds for the Central Universities
- DOI：10.11889/j.0253-3219.2018.hjs.41.060203
  CLC： TL273
- Received：06 February 2018，
  
  Revised：27 March 2018，
  
  Published：10 June 2018
- 稿件说明：
移动端阅览
Yong LU, Qiaoqiao TANG, Zheng JIANG, et al. Thermodynamic study on phase stability of plutonium under irradiation[J]. Nuclear techniques, 2018, 41(6): 060203
DOI：

Yong LU, Qiaoqiao TANG, Zheng JIANG, et al. Thermodynamic study on phase stability of plutonium under irradiation[J]. Nuclear techniques, 2018, 41(6): 060203 DOI： 10.11889/j.0253-3219.2018.hjs.41.060203.

摘要

Pu（钚）是一种十分重要的核工业原料，随温度变化会有不同的结构，并且辐照对其有着重要的影响。为了探究辐照强度、辐照时间对钚的相变化的影响，本研究在纯Pu的吉布斯（Gibbs）自由能计算基础上，通过考虑辐照条件下空位产生的过剩自由能，建立了纯Pu在辐照条件下的热力学模型。计算不同辐照条件下的温度-吉布斯自由能函数，得到了不同辐照强度下纯Pu的相图，分析不同辐照强度、辐照时间对其6个同素异构体相稳定性的影响。研究结果表明：辐照对较低温度下纯Pu的相稳定性影响较大，接近室温时出现了γ-Pu的相区，其稳定存在的温度范围会随着辐照的强度增强、辐照时间加长而扩大，而且辐照使α-Pu趋于稳定。本研究所建立的辐照条件下的纯Pu的相图为Pu基核燃料的设计提供重要的基础理论指导。

Abstract

Background

Pu is an important material for nuclear industry

its structure is sensitive to temperature

and irradiation has an important impact on it.

Purpose

In order to explore the thermodynamic effects of irradiation on plutonium

the phase diagram of pure Pu under the irradiation established in this study provides important theoretical guidance for the design of Pu-based nuclear fuels.

Methods

Based on Gibbs free energy of pure Pu

the thermodynamic model of Pu under irradiation was established by considering the excess free energy of vacancies under irradiation conditions.

Results

The Gibbs free energy function under different irradiation was calculated

and the phase diagrams of pure Pu under different irradiation intensities were obtained. The effects of different irradiation conditions and irradiation time on the stability of six allotropic phases were analyzed.

Conclusion

The results indicated that irradiation has great influence on the phase stability of plutonium at lower temperature and the stable phase region of γ-Pu appears near room temperature. Its stable temperature range increased with the increase of the intensity of irradiation and time.

关键词

Keywords

references

W H Zachariasen , F Ellinger . Crystal structure of alpha-plutonium metal . Journal of Chemical Physics , 1963 . 16 ( 8 ): 777 - 783 . DOI: 10.1063/1.1743837 http://doi.org/10.1063/1.1743837 .

W H Zachariasen , F H Ellinger . The crystal structure of beta plutonium metal . Acta Crystallographica , 1963 . 16 ( 5 ): 369 - 375 . DOI: 10.1107/S0365110X63000992 http://doi.org/10.1107/S0365110X63000992 .

Zachariasen W H. The crystal structure of gamma plutonium[R]. Los Alamos Scientific Laboratory, 1951.

W H Zachariasen , F H Ellinger . Crystal chemical studies of the 5 f -series of elements XXIV:the crystal structure and thermal expansion of γ-plutonium . Acta Crystallographica , 1955 . 8 ( 7 ): 431 - 433 . DOI: 10.1107/S0365110X55001357 http://doi.org/10.1107/S0365110X55001357 .

W B H Lord . Some physical properties of metallic plutonium . Nature , 1954 . 173 ( 4403 ): 534 - 535 . DOI: 10.1038/173534a0 http://doi.org/10.1038/173534a0 .

E R Jette . Some physical properties of plutonium metal . Journal of Chemical Physics , 1955 . 23 ( 2 ): 365 - 368 . DOI: 10.1063/1.1741970 http://doi.org/10.1063/1.1741970 .

R D Baker , S S Hecker , D R Harbur . Plutonium a wartime nightmare but a metallurgist's dream , : New Mexico Los Alamos Science , 1983 . 142 - 158 .

N Baclet , B Oudot , R Grynszpan , . Self-irradiation effects in plutoniumalloys . Journal of Alloys & Compounds , 2007 . s444-445 ( 24 ): 305 - 309 . DOI: 10.1016/j.jallcom.2006.10.156 http://doi.org/10.1016/j.jallcom.2006.10.156 .

A V Troshev , A M Lyasota . Effect of self-irradiation on the parameters of the α→β transformation of unalloyed plutonium . Physics of Metals & Metallography , 2010 . 109 ( 6 ): 621 - 625 . DOI: 10.1134/S0031918X10060086 http://doi.org/10.1134/S0031918X10060086 .

A J Schwartz , H Cynn , K J M Blobaum , . Atomic structure and phase transformations in Pu alloys . Progress in Materials Science , 2009 . 54 ( 6 ): 909 - 943 . DOI: 10.1016/j.pmatsci.2009.03.003 http://doi.org/10.1016/j.pmatsci.2009.03.003 .

F J Espinosa , P Villella , J C Lashley , . Local atomic structure of α-Pu . Physical Review B , 2001 . 63 ( 63 ): 174111 DOI: 10.1103/PhysRevB.63.174111 http://doi.org/10.1103/PhysRevB.63.174111 .

J L Sarrao , J D Thompson , N O Moreno , . Discovery of plutonium-based superconductivity . Journal of Physics Condensed Matter , 2003 . 15 ( 28 ): S2275 - S2278 . DOI: 10.1088/0953-8984/15/28/368 http://doi.org/10.1088/0953-8984/15/28/368 .

J L Sarrao , L A Morales , J D Thompson . Superconductivity:a new window on plutonium's complexity . JOM , 2003 . 55 ( 9 ): 38 - 40 . DOI: 10.1007/s11837-003-0028-8 http://doi.org/10.1007/s11837-003-0028-8 .

李萌 , 范红玉 , 崔荷敬 , . 低能氦离子辐照诱导的钨材料结构演化 . 核技术 , 2017 . 40 ( 10 ): 100201 DOI: 10.11889/j.0253-3219.2017.hjs.40.100201 http://doi.org/10.11889/j.0253-3219.2017.hjs.40.100201 http://www.j.sinap.ac.cn/hejishu/CN/abstract/abstract821.shtml .

Meng LI , Hongyu FAN , Hejing CUI , . Low-energy helium-ions irradiation induced morphology and crystalline evolution of tungsten . Nuclear Techniques , 2017 . 40 ( 10 ): 100201 DOI: 10.11889/j.0253-3219.2017.hjs.40.100201 http://doi.org/10.11889/j.0253-3219.2017.hjs.40.100201 http://www.j.sinap.ac.cn/hejishu/CN/abstract/abstract821.shtml .

W G Wolfer . Spectroscopies for environmental studies of actinide species , : New Mexico Los Alamos Science , 2000 . 274 - 285 .

V Natarajan , T K Seshagiri , R Veeraraghavan , . Radiation effects in plutonium and carbonate co-doped calcium hydroxy apatite:an EPR study . Journal of Radioanalytical & Nuclear Chemistry , 2003 . 256 ( 3 ): 445 - 449 . DOI: 10.1023/A:1024591414217 http://doi.org/10.1023/A:1024591414217 .

F Jutier , J C Griveau , E Colineau , . Influence of self-irradiation damages on the superconducting behaviour of Pu-based compounds . Physica B Condensed Matter , 2005 . s359-s361 1078 - 1080 . DOI: 10.1016/j.physb.2005.01.292 http://doi.org/10.1016/j.physb.2005.01.292 .

R O Elliott , C E Olsen . Comparison of self-irradiation effects in alpha plutonium enriched and unenriched in 238 Pu . Journal of Applied Physics , 1964 . 35 ( 6 ): 1925 - 1931 . DOI: 10.1063/1.1713771 http://doi.org/10.1063/1.1713771 .

X J Liu , Y L Zhao , Y Lu , . Steady-state dynamical phase diagram calculation of U-Nb binary system under irradiation:ballistic effect . Journal of Nuclear Materials , 2014 . 451 ( 1-3 ): 366 - 371 . DOI: 10.1016/j.jnucmat.2014.04.028 http://doi.org/10.1016/j.jnucmat.2014.04.028 .

J W Cahn , J E Hilliard . Free energy of a nonuniform system Ⅰ:interfacial free energy . Journal of Chemical Physics , 1959 . 31 ( 3 ): 688 - 699 . DOI: 10.1063/1.1744102 http://doi.org/10.1063/1.1744102 .

K C Russell . Phase stability under irradiation . Progress in Materials Science , 1984 . 28 ( 3 ): 229 - 434 . DOI: 10.1016/0079-6425(84)90001-X http://doi.org/10.1016/0079-6425(84)90001-X .

G S Was . Fundamentals of radiation materials science , : New York Springer , 2007 . 155 - 184 .

胡赓祥 , 蔡珣 , 戎咏华 . 材料科学基础 , : 上海上海交通大学出版社 , 2006 . 108 - 222 .

Gengxiang HU , Xun CAI , Yonghua RONG . Fundamentals of materials science , : Shanghai Shanghai Jiao Tong University Press , 2006 . 108 - 222 .

N Ravishankar , T A Abinandanan , K Chattopadhyay . Application of effective potential formalism to mechanical alloying in Ag-Cu and Cu-Fe systems . Materials Science & Engineering A , 2001 . s304-306 ( 00 ): 413 - 417 . DOI: 10.1016/S0921-5093(00)01484-2 http://doi.org/10.1016/S0921-5093(00)01484-2 .

B P Uberuaga , S M Valone , M I Baskes . Accelerated dynamics study of vacancy mobility in δ-plutonium . Journal of Alloys & Compounds , 2006 . 444-445 ( 2007 ): 314 - 319 . DOI: 10.1016/j.jallcom.2006.10.083 http://doi.org/10.1016/j.jallcom.2006.10.083 .

L Berlu , G Jomard , G Rosa , . Computer simulation of point defects in plutonium using MEAM potentials . Journal of Nuclear Materials , 2008 . 372 ( 2-3 ): 171 - 176 . DOI: 10.1016/j.jnucmat.2006.11.016 http://doi.org/10.1016/j.jnucmat.2006.11.016 .

S M Valone , M I Baskes , M Stan , . Simulations of low energy cascades in fcc Pu metal at 300 K and constant volume . Journal of Nuclear Materials , 2004 . 324 ( 1 ): 41 - 51 . DOI: 10.1016/j.jnucmat.2003.09.006 http://doi.org/10.1016/j.jnucmat.2003.09.006 .

A Kubota , W G Wolfer , S M Valone , . Modeling of aging in plutonium by molecular dynamics . Nuclear Instruments & Methods in Physics Research , 2003 . 202 ( 202 ): 82 - 87 . DOI: 10.1007/s10820-007-9057-x http://doi.org/10.1007/s10820-007-9057-x .

B Y Ao , X L Wang , P H Chen , . Energy calculation of point defects in plutonium by embedded atom method . Acta Physica Sinica , 2010 . 59 ( 7 ): 4818 - 4825 . DOI: 10.7498/aps.59.4818 http://doi.org/10.7498/aps.59.4818 .

X H Yu , Z L Zhan , J Rong , . Vacancy formation energy and size effects . Chemical Physics Letters , 2014 . 600 ( 600 ): 43 - 45 . DOI: 10.1016/j.cplett.2014.03.046 http://doi.org/10.1016/j.cplett.2014.03.046 .

R Sizmann . The effect of radiation upon diffusion in metals . Journal of Nuclear Materials , 1978 . s69-70 ( 1-2 ): 386 - 412 . DOI: 10.1016/0022-3115(78)90256-8 http://doi.org/10.1016/0022-3115(78)90256-8 .

E M Foltyn , Jr F W Clinard , J Rankin , . Self-irradiation effects in 238 Pu-substituted zirconolite Ⅱ:effect of damage microstructure on recovery . Journal of Nuclear Materials , 1985 . 136 ( 1 ): 97 - 103 . DOI: 10.1016/0022-3115(85)90035-2 http://doi.org/10.1016/0022-3115(85)90035-2 .

Views

下载量

CSCD

Alert me when the article has been cited

提交

Tools

Publicity Resources

Slow positron beam study on defects induced by Xe ions irridiation in matrix graphite of fuel elements

Study of adsorption characteristic of uranium(VI) on clay colloid

Investigation of helium irradiation induced hardening in nickel-based alloy

High-temperature thermodynamics for fluorinating uranium compounds

Radiation effects on physicochemical characteristics of pork

Related Author

XU Hongxia

LIN Jun

ZHU Zhiyong

LIU Jiandang

GU Bingchuan

YE Bangjiao

SONG Yiting

LENG Yangchun

Related Institution

State Key Laboratory of Particle Detection and Electronics, University of Science and Technology of China

Shanghai Institute of Applied Physics, Chinese Academy of Sciences

Key Subject Laboratory of National Defense for Radioactive Waste and Environmental Security, Southwest University

University of Chinese Academy of Sciences

Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Jiading Campus

AI问答

Address：2019 Jialuo Road, Jiading, Shanghai, China Postal code：201800
Tel：021-39194977 Email：LHB@sinap.ac.cn
Technical support is provided by Beijing Founder electronics co., LTD 沪ICP备05005479号-1 京公网安备11010802024621
It is recommended to read the content of this site in Chrome&IE9+. Please switch to extreme mode in browser 360.
Cookies We use cookies to help provide and enhance our service and tailor content. By continuing, you agree to the use of cookies.
Total Visits：880473

⁰