铀、钍在Nd2Zr2O7烧绿石中的固化研究

O731%TL93; 为研究锕系元素铀、钍在烧绿石中的固化行为,通过喷雾热解-高温烧结成功合成了含铀、钍的系列Nd2Zr2O7烧绿石固化体,并采用XRD、SEM、EDS、Raman光谱和XPS等方法对所得固化体样品进行了表征.结果 表明:铀、钍均能进入Nd2Zr2O7晶格的A位形成稳定的烧绿石结构.Th在固化体中的固溶量(摩尔分数,下同)达到40％,固化体保持较好的烧绿石单相结构;随着Th含量的增加,固化体转变为烧绿石、立方ZrO2和ThO2共存的多相陶瓷结构.U在Nd2-xUxZr2O7烧绿石中的固溶量仅为10％,固化体结构无序化明显增加;随着U含量的增加,固化体快速转变为萤石结构,铀固溶量...

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Published in原子能科学技术 Vol. 55; no. 12; pp. 2309 - 2316
Main Authors 王烈林, 谢华, 陈青云, 李江博, 谢宇骐
Format Journal Article
LanguageChinese
Published 西南科技大学核废物与环境安全国防重点学科实验室,四川绵阳621010 20.12.2021
Subjects
铀;钍;烧绿石;固化
Online AccessGet full text
ISSN1000-6931
DOI10.7538/yzk.2020.youxian.0917

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Abstract O731%TL93; 为研究锕系元素铀、钍在烧绿石中的固化行为,通过喷雾热解-高温烧结成功合成了含铀、钍的系列Nd2Zr2O7烧绿石固化体,并采用XRD、SEM、EDS、Raman光谱和XPS等方法对所得固化体样品进行了表征.结果 表明:铀、钍均能进入Nd2Zr2O7晶格的A位形成稳定的烧绿石结构.Th在固化体中的固溶量(摩尔分数,下同)达到40％,固化体保持较好的烧绿石单相结构;随着Th含量的增加,固化体转变为烧绿石、立方ZrO2和ThO2共存的多相陶瓷结构.U在Nd2-xUxZr2O7烧绿石中的固溶量仅为10％,固化体结构无序化明显增加;随着U含量的增加,固化体快速转变为萤石结构,铀固溶量约为20％.铀、钍在Nd2 Zr2O7烧绿石固化体中固溶量存在较大差异.XPS分析发现,Th在烧绿石固化体中以+4价存在;U在固化体中以+4价和+6价存在,导致固化体A位离子的配位结构发生变化,更多氧离子进入烧绿石体系,导致体系转变为无序化萤石结构,固溶量明显下降.
AbstractList O731%TL93; 为研究锕系元素铀、钍在烧绿石中的固化行为,通过喷雾热解-高温烧结成功合成了含铀、钍的系列Nd2Zr2O7烧绿石固化体,并采用XRD、SEM、EDS、Raman光谱和XPS等方法对所得固化体样品进行了表征.结果 表明:铀、钍均能进入Nd2Zr2O7晶格的A位形成稳定的烧绿石结构.Th在固化体中的固溶量(摩尔分数,下同)达到40％,固化体保持较好的烧绿石单相结构;随着Th含量的增加,固化体转变为烧绿石、立方ZrO2和ThO2共存的多相陶瓷结构.U在Nd2-xUxZr2O7烧绿石中的固溶量仅为10％,固化体结构无序化明显增加;随着U含量的增加,固化体快速转变为萤石结构,铀固溶量约为20％.铀、钍在Nd2 Zr2O7烧绿石固化体中固溶量存在较大差异.XPS分析发现,Th在烧绿石固化体中以+4价存在;U在固化体中以+4价和+6价存在,导致固化体A位离子的配位结构发生变化,更多氧离子进入烧绿石体系,导致体系转变为无序化萤石结构,固溶量明显下降.
Author 李江博
陈青云
谢宇骐
王烈林
谢华
AuthorAffiliation 西南科技大学核废物与环境安全国防重点学科实验室,四川绵阳621010
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XIE Yuqi
XIE Hua
WANG Lielin
LI Jiangbo
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