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化学进展 2020, Vol. 32 Issue (2/3): 219-229 DOI: 10.7536/PC190824 前一篇   后一篇

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锕系元素分离研究:不对称双酰胺荚醚的萃取化学及应用

刘耀阳1, 刘志斌1, 赵闯1, 周羽1, 高杨1,**(), 何辉1,2   

  1. 1. 哈尔滨工程大学核科学与技术学院 哈尔滨 150001
    2. 中国原子能科学研究院 北京 102413
  • 收稿日期:2019-08-22 出版日期:2020-02-15 发布日期:2019-12-19
  • 通讯作者: 高杨
  • 基金资助:
    哈尔滨工程大学中央高校基本科研业务费(GK2150260176)
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Separation of Actinides: Extraction Chemistry and Application of Unsymmetric Diglycolamides

Yaoyang Liu1, Zhibin Liu1, Chuang Zhao1, Yu Zhou1, Yang Gao1,**(), Hui He1,2   

  1. 1. College of Nuclear Science and Technology, Harbin Engineering University, Harbin 150001, China
    2. China Institute of Atomic Energy, Beijing 102413, China
  • Received:2019-08-22 Online:2020-02-15 Published:2019-12-19
  • Contact: Yang Gao
  • About author:
    ** e-mail:
  • Supported by:
    Special Fund of Central University Basic Scientific Research Fee(GK2150260176)

PUREX乏燃料后处理流程排放出的高放废液,集中了乏燃料中95% 以上的放射性,其中半衰期长、毒性大的次锕系核素是需要在地质处置库中将高放废液与生物圈隔离10万年以上的因素之一。为了更安全可靠地解决高放废液问题,国际上提出了“分离-嬗变”技术,即利用化学方法,将次锕系元素和长寿命裂变产物元素从高放废液中分离出来,根据分离出来元素的性质,对其加以利用或使其嬗变。分离-嬗变技术中的关键是对高放废液中不同类别元素的有效分离。双酰胺荚醚类萃取剂对高放废液中三价锕系、镧系元素展现出了优异的萃取性能,尤其是不对称双酰胺荚醚,在保持相应的对称性双酰胺荚醚良好的萃取性能的同时,在缓解或避免萃取过程中第三相形成方面也有较大优势。本文就不对称酰胺荚醚的历史沿革、合成方法、萃取性能、配位机理、流程工艺以及三相形成等几个方面进行了综述,就多种不对称双酰胺荚醚萃取剂对锕系、镧系及其他主要裂片元素的萃取分配比、分离系数、三相形成临界参数等进行了比较,对该类萃取剂后续的结构设计、配位机理研究及流程应用等方向提供了参考性建议。

关键词： 高放废液, 锕系分离, 萃取, 不对称双酰胺荚醚

The high level liquid waste(HLLW) generated from PUREX reprocessing process contains more than 95% radioactivity of the spent fuel. Among HLLW, minor actinides with long half-life and high toxicity are one of the main factors that need to isolate HLLW from the biosphere for more than 100 000 years in the deep geological repositories. In order to solve the problem of HLLW more safely and reliably, “separation-transmutation” technology has been put forward, that is, the minor actinides and long-lived fission product elements are separated from HLLW by chemical methods, and then the separated elements are utilized or transmuted according to their properties. The effective separation of different kinds of elements from HLLW is the key step in the separation-transmutation technology. The diglycolamide extractants exhibit excellent extractability towards trivalent actinides and lanthanides in HLLW. In particular, the unsymmetric diglycolamides have greater advantage than the corresponding symmetric diglycolamides in relieving or avoiding the formation of the third phase in the extraction process, and at the same time maintain the good extraction performances. In this paper, the development history, synthesis method, extraction performance, coordination mechanism, flow process, and the third phase formation of unsymmetric diglycolamides are reviewed. The extraction ratio, the separation factor and the critical parameters of the third phase formation of lanthanides, actinides and other major fission elements are compared. Some suggestions are provided for the structural design, coordination mechanism research and process application of the unsymmetric diglycolamides.

Key words: high level liquid waste, actinide separation, extraction, unsymmetric diglycolamides
()
图1 对称双酰胺荚醚结构
Fig.1 Symmetric diglycolamides structure
图2 不对称双酰胺荚醚结构
Fig.2 Unsymmetric diglycolamides structure
图式1 (1)仲胺和酸酯反应酰胺化过程合成不对称双酰胺荚醚流程;(2)仲胺和酸酐反应酰胺化过程合成不对称双酰胺荚醚流程;(3)仲胺和酰氯反应酰胺化过程合成不对称双酰胺荚醚流程
Scheme 1 (1) Synthesis of unsymmetric diglycolamides by secondary amines and acid esters;(2) Synthesis of unsymmetric diglycolamides by secondary amines and anhydrides;(3) Synthesis of unsymmetric diglycolamides by secondary amines and acyl chlorides
图3 不对称双酰胺荚醚结构
Fig.3 Unsymmetric diglycolamides structure
表1 Sr(Ⅱ)/Am(Ⅲ)分离系数与水相HNO3浓度的关系[29]
Table 1 Relationship between separation coefficient of Sr(Ⅱ)/Am(Ⅲ) and concentration of HNO3 in aqueous phase[29]
Diluent Extractant
concentration		 HNO3(M) 2 3 4 5 6 8
n-DD 0.1 DHDODGA 347 281 third phase / / /
TODGA 85 74 >157
D2DODGA 183 175 >166 >217
D3DODGA 38 172 >228 >331
0.1 DEHDODGA 144 91 >83 /
0.03 81 324 520 ~1700 >200 >20 000
表2 多种不对称双酰胺荚醚萃取体系Nd(Ⅲ)与HNO3 CAC值与LOC值
Table 2 CAC and LOC of Nd(Ⅲ) and HNO3 in various unsymmetric diglycolamides extraction systems
DGA Diluent HNO3
(M)		 [DGA]
(M)		 Nd(Ⅲ) [DGA]
(M)		 HNO3
[Nd(Ⅲ)]ini
(mM)		 CAC
(mM)		 LOC
(mM)		 [HNO3]ini
(M)		 CAC
(M)		 LOC
(M)
DHDODGA n-dodecane 0.1 third phase 0.1 4 3.2 0.08
1
TODGA / / 14
2
/ 12
3
8 6.4 6 5.1 0.18
4
6 2.8
5
<1 mM <1 mM
3
D2DODGA 15 13.2 7 5.6 0.2
4
5
10 8.1
3
7 3.5
4
D3DODGA >600 32 12 9.3 0.28
5
>600 31
/
105 24
D3DBDGA Extraction of trivalent actinides in HLLW does not form any third phase 15.7 12.4 0.26
3
D3DHDGA 10.9 8.3 0.23
4
D3D2DGA 12 9.4 0.3
5
D3DEHDGA 295 225 24 11.9 9.5 0.3
1
120 41.6 19
2
40 11.5 17
3
DEHDODGA 0.1 7 0.03 9.5
3
5.3
4.1 0.1 5
0.2 11.3 / / /
0.3 / 14.3 0.2 4.9
0.4 28.9
0.5 33.3 0.5 4
DMDODGA 0.64 M
n-octanal/K.O.		 1
2
3		 0.12 / 12.77
11.7
9.98		 /
TEHDGA 1 M
DHOA/n-dodecane		 2
3		 0.2 / 72
62		 0.2 / 7.8 /
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