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化学进展 2020, Vol. 32 Issue (9): 1316-1333 DOI: 10.7536/PC200219 前一篇   后一篇

• 综述 •

固相萃取分离铀

李波1,2(), 马利建3,**, 罗宁1,2, 李首建3, 陈云明1,2, 张劲松1,2,**   

  1. 1. 中国核动力研究设计院 成都 610213
    2. 四川省放射性同位素工程技术研究中心 成都 610213
    3. 四川大学化学学院 成都 610064
  • 收稿日期:2020-02-18 修回日期:2020-03-10 出版日期:2020-09-24 发布日期:2020-03-31
  • 通讯作者: 马利建, 张劲松
  • 作者简介:
    ** Corresponding author e-mail:
  • 基金资助:
    *国家自然科学基金项目(21771128, 21976125); 中国核动力研究院核技术应用项目(16JS1807, 18JS1808)
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Extraction and Separation of Uranium via Solid Phase Extraction

Bo Li1,2(), Lijian Ma3,**, Ning Luo1,2, Shoujian Li3, Yunming Chen1,2, Jinsong Zhang1,2,**   

  1. 1. Nuclear Power Institute of China, Chengdu 610213, China
    2. Radioisotope Engineering Technology Research Center of Sichuan, Chengdu 610213, China
    3. College of Chemistry, Sichuan University, Chengdu 610064, China
  • Received:2020-02-18 Revised:2020-03-10 Online:2020-09-24 Published:2020-03-31
  • Contact: Lijian Ma, Jinsong Zhang
  • Supported by:
    the National Natural Science Foundation of China(21771128, 21976125); the Nuclear Technology Application Foundaion of Nuclear Power Institute of China(16JS1807, 18JS1808)

铀是重要的核工业原料,也是一种有较强化学和生物毒性的重金属。从各类含铀水体系中分离和回收铀对缓解铀资源短缺,保护人类健康和生态环境安全都具有重要的科学和实际意义。本文简要回顾和评述了近15年来具有代表性的新型固相萃取材料及其在铀分离方面的应用研究,并对相关材料在铀分离领域的应用前景进行了分析和展望。

关键词： 铀, 固相萃取, 固相萃取剂, 吸附, 分离

Uranium is an important raw material in the nuclear industry. Besides, uranium is a heavy metal with higher chemical and biological toxicity. Therefore, it is of great scientific and practical significance to efficiently separate and recover uranium from various uranium-containing aqueous systems for alleviating the shortage of uranium resources, and protecting human health and ecological environment safety. In the review, all kinds of representative solid phase extractants developed in the recent 15 years for uranium separation and recovery are briefly summarized, and the prospect and potential research directions of the solid phase extractants are also introduced.

Contents

1 Introduction

2 Solid phase extractants for uranium separation

2.1 Inorganic materials

2.2 Polymer materials

2.3 Carbonaceous materials

2.4 Metal-organic frameworks materials

2.5 Other solid phase extractants

2.6 Evaluation of the separation performance of various materials toward uranium

3 Conclusion and outlook

Key words: uranium, solid phase extraction, solid phase extractant, adsorption, separation
()
图1 近15年来每年发表的关于铀固相萃取方面的文章数量(资料来源:web of science,检索时间: 2020年1月)
Fig.1 Numbers of annually published articles on the solid phase extraction of uranium in the recent 15 years(source:web of science, 2020-01 )
图2 铀与赤铁矿(Fe2O3)和nZVI反应过程中不同时间的STEM-XEDS映射图[5]
Fig.2 STEM-XEDS mappings of uranium reactions with hematite(Fe2O3) and nZVI at different times[5]
图3 (a)POMN竞争吸附模拟海水中的铀,(b)POMN分散在水中及其磁分离[16]
Fig.3 (a) Competitive adsorption of uranium on POMN in simulated seawater,(b)Water dispersion of POMN and magnetic separation[16]
表1 各磁性纳米材料对铀的吸附容量对比
Table 1 Comparison of adsorption capacity of uranium on various inorganic materials(T = 298 K)
Adsorbents pH Co(mg/L) qe(mg/g) m/v(g/L) ref
DTiOxNTs 6.0 150 366 0.2 32
CoFe2O4 6.0 300 160 1 33
IONPs 5.5 130 500 1000 39
O-Fe3O4 7.0 50 125 / 41
Fe3O4@SiO2-AO 5.0 140 105 0.4 42
QASM 3.7 60 12.5 0.77 43
EDTA-mGO 5.5 25 277 0.1 44
Fe3O4@C@Ni-Al LDH 6.0 220 174 1 45
Fe3O4@TiO2 6.0 150 90 1 46
Fe3O4/GO 5.5 50 69 0.3 48
g-C3N4/TiO2 6.9 20 64 0.25 49
图4 (a) KMS-1吸附铀前(左)后(右)的形貌,(b) KMS-1通过交换层间K+来捕获UO22+离子[7]
Fig.4 (a) SEM images of KMS-1(left) and UO22+-exchanged KMS-1(right),(b) Mechanism of capture of UO22+ ions by KMS-1 through exchange of its interlayer potassium cations[7]
图5 (a) MoS2-g-PDMA的合成机理,(b) MoS2-g-PDMA吸附铀可能的机理[53]
Fig.5 (a) The schematic for synthesis of MoS2-g-PDMA,(b) Possible sorption mechanism of MoS2-g-PDMA towards uranium[53]
表2 对比各种双层氢氧化物对铀的吸附容量
Table 2 Comparison of adsorption capacity of uranium on various double hydroxides
Adsorbents pH Co(mg/L) qe(mg/g) m/v(g/L) ref
Cys-LDH 5.0 60 211 0.1 56
Ca/Al LDH-Gl 5.0 35 266 0.1 57
γ-Fe2O3/LDO 5.0 66 526 0.1 58
Fe3O4@C@Ni-Al LDH 6.0 220 174 1 45
LDH@nZVI 5.0 40 176 0.1 59
LDO-C 5.0 145 354 0.1 60
rGO-LDH 4.0 130 277 0.5 61
Ca-Mg-Al-LDO 5.0 70 487 0.1 62
图6 水合插层策略制备Ti3C2Tx及其对铀的分离[65]
Fig.6 Hydrated intercalation strategy synthesis of Ti3C2Tx MXene for efficient uranium separation[65]
图7 聚丙烯无纺布表面离子印迹聚合过程[87]
Fig.7 Preparation of surface ion-imprinted polypropylene nonwoven fabric[87]
图8 CPT-T吸附铀可能的机理[99]
Fig.8 Possible sorption mechanism of CPT-T towards uranium[99]
图9 (a)CPT-IHEP1的合成过程,(b)实验和模拟的CPT-IHEP1的PXRD结构[102]
Fig.9 (a)Synthetic procedures for COF-IHEP1,(b)experiment(black)and predicted(red)PXRD patterns of CPT-IHEP1[102]
表3 对比各种聚合物对铀的吸附容量
Table 3 Comparison of adsorption capacity of uranium on various polymer materials (T = 298 K)
Adsorbents pH Co(mg/L) qe(mg/g) m/v(g/L) ref
CCTS-DHBA resin 3.0 100 330 0.2 82
PS-PAMAM-PPA 5.0 500 99.9 1 83
HSDC 4.5 250 373 0.4 84
U(Ⅵ)-ⅡP 7.0 200 134 0.5 85
ⅡP3 4.0 700 133 4 88
ⅡP 4.5 528 120 0.68
CCU 4.5 275 240 0.4 96
TCD 4.5 275 158 0.4 97
MOCOF 1 M HNO3 100 57 0.4 98
COF-IHEP1 3 120 112 0.4 102
MCPs 5.5 100 165 0.2 103
CMP-EP 6 M HNO3 100 67 1 104
PPAFs 1 250 147 0.4 105
表4 对比各种炭质材料对铀的吸附容量
Table 4 Comparison of adsorption capacity of uranium on various carbon materials (T = 298 K)
Adsorbents pH Co(mg/L) qe(mg/g) m/v(g/L) ref
HTC-Sal 4.3 300 261 0.5 2
HTC-Acy 4.5 300 339 0.5 114
AO-HTC-DAMN 4.3 300 466 0.4 115
HTC-btg 4.5 300 307 0.4 116
HCSs-PO4 5.0 200 286 0.2 118
AO-HTC 5.0 200 724 0.1 119
HCSs-300 7.0 50 180 0.2 120
HCC 7.0 90 273 0.2 121
AOMGO 5.0 150 286 0.2 6
AGH 6.0 250 398 0.5 130
AMGO 5.9 35 141 0.2 131
RGO-PDA/oxime 5.0 100 1049 0.001 132
CB[6]/GO/Fe3O4 5.0 75 122 0.2 133
rGO-LDH 4.0 130 277 0.5 61
FGs 5.0 250 455 0.2 134
CMK-3 6.0 120 178 0.2 137
PANI-CMK-3 6.0 120 118 0.2 138
CMK-3-SO3H 6.0 110 168 0.2 139
CMK-3-PO4 6.0 110 485 0.2 140
AO/CMK-3 6.0 110 238 0.2 141
MC-O-PO(OH)2 4.0 130 85 1 143
Oxime-CMK-5 4.5 200 65 0.4 144
P-Fe-CMK-3 4.0 300 150 0.2 145
AO-g-MWCNTs 4.5 300 145 1 149
MWNTs-C 6.0 400 89 2 150
MWNTs-F 5.0 120 72 1 131
PAMAM/WMCNT 5.0 180 80 1.5 152
MWCNTs 5.0 50 39 1 153
DGA-MWCNT / / 133 / 154
GO-CNTs 5.0 200 92 0.6 155
CoFe2O4/MWCNTs 6.0 100 213 0.4 156
PVA/MWCNTs 3.0 1000 160 0.6 157
图10 偕胺肟接枝水热炭(AO-HTC-DAMN)的制备过程[115]
Fig.10 Preparation of amidoxime-anchored AO-HTC-DAMN[115]
图11 DFT计算提出的Urea-GO与铀酰离子的配位机理[135]
Fig.11 Proposed ligand exchange mechanism of uranyl extraction based on DFT calculation[135]
图12 ND-AO的制备及其可能的吸附机理[159]
Fig.12 Preparation of ND-AO and the possible adsorption mechanism[159]
图13 UiO-66-AO的合成[165]
Fig.13 Synthetic route of UiO-66-AO[165]
表5 对比各种COFs对铀的吸附容量
Table 5 Comparison of adsorption capacity of uranium on various COFs (T = 298 K)
Adsorbents pH Co(mg/L) qe(mg/g) m/v(g/L) ref
MIL-101-DETA 5.5 200 350 0.4 166
ED-MIL-101(Cr) 4.5 100 200 0.5 167
MOF-AC 2 100 118 0.5 168
MOF-3 7.0 500 304 1 169
C-Zn-MOF-74 4 400 360 1 170
Zn(ADC)(4,40-BPE)0.5 6.0 200 312 0.5 171
GO-COOH/UiO-66 8.0 500 998 0.5 172
Fe3O4@ZIF-8 3.0 250 523 0.4 173
图14 MA-TMA吸附铀前后颜色变化(a)和(b)及配位机理(c)和(d)[180]
Fig.14 (a)and(b)Color change after MA-TMA adsorption of uranium , (c)and(d)possible coordination mechanism[180]
图15 氢键超分子吸附铀后结构形貌变化及配位机理[181]
Fig.15 Morphology and coordination mechanism of HSOF adsorbed uranium[181]
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