基于海水提铀的多孔芳香框架材料研究进展

doi:10.16085/j.issn.1000-6613.2022-0970

化工进展 ›› 2023, Vol. 42 ›› Issue (3): 1426-1436.DOI: 10.16085/j.issn.1000-6613.2022-0970

基于海水提铀的多孔芳香框架材料研究进展

郭帅帅¹(), 陈锦路², 金梁程龙¹, 陶醉¹, 陈小丽², 彭国文¹^,²^,³()

^1.南华大学资源环境与安全工程学院，湖南衡阳 421001
^2.南华大学化学化工学院，湖南衡阳 421001
^3.南华大学湖南省铀尾矿库退役治理工程技术研究中心，湖南衡阳 421001

收稿日期:2022-05-26 修回日期:2022-07-21 出版日期:2023-03-15 发布日期:2023-04-10
通讯作者: 彭国文
作者简介:郭帅帅（1996—），男，硕士研究生，研究方向为新型功能材料。E-mail：guoss1996@163.com。
基金资助:
中央军委装备发展部预研项目(32101070503)

Research progress of porous aromatic frameworks based on uranium extraction from seawater

GUO Shuaishuai¹(), CHEN Jinlu², JIN Liangchenglong¹, TAO Zui¹, CHEN Xiaoli², PENG Guowen¹^,²^,³()

^1.School of Resource & Environment and Safety Engineering, University of South China, Hengyang 421001, Hunan, China
^2.School of Chemistry and Chemical Engineering, University of South China, Hengyang 421001, Hunan, China
^3.Engineering Technology Research Center for Decommissioning Treatment of Uranium Tailings Pond in Hunan Province, University of South China, Hengyang 421001, Hunan, China

Received:2022-05-26 Revised:2022-07-21 Online:2023-03-15 Published:2023-04-10
Contact: PENG Guowen

摘要/Abstract

摘要：

多孔芳香框架材料是一类新兴的有机多孔纳米材料，具有稳定性高、比表面积大、易于修饰改性等特点，可以满足多种吸附材料设计的需求。近几年众多学者将修饰改性后的多孔芳香框架材料应用于海水提铀，发现其具有较大的铀吸附量、优异的铀选择性、良好的可循环性等特点。本文综述了近年来基于海水提铀的多孔芳香框架材料的研究进展，首先简要介绍了其合成反应与合成技术，然后分类讨论了与铀的相互作用机理，并评估了多种改性多孔芳香框架材料对铀的吸附性能，分析了其对铀的高选择性和高吸附效率的原因。最后，本文针对目前多孔芳香框架材料在海水提铀中的局限性（多孔芳香框架材料的合成、吸附性能的提高、成本的降低及机理的深层次研究等）为未来设计低成本高性能的多孔芳香框架材料吸附剂提供了几点建议。

关键词: 多孔芳香框架材料, 海水提铀, 吸附剂, 合成, 纳米材料

Abstract:

Porous aromatic framework materials are an emerging class of organic porous nanomaterials with high stability, large specific surface area and easy modification, which can meet the needs of various adsorption material designs. In recent years, many scholars have applied the modified porous aromatic framework materials in uranium extraction from seawater and found that they have large uranium adsorption capacity, excellent uranium selectivity and good recyclability. This paper reviews the recent research progress of porous aromatic framework materials based on uranium extraction from seawater. The synthetic reactions and synthesis techniques of porous aromatic framework materials are firstly briefly introduced, and then their interaction mechanisms with uranium are categorically discussed. The adsorption performance of various modified porous aromatic framework materials on uranium are evaluated, and the reasons for the high selectivity and high adsorption efficiency on uranium are analyzed. Finally, the paper provid some suggestions for the future design of low-cost and high-performance porous aromatic framework adsorbents in view of the current limitations of porous aromatic framework materials for uranium extraction from seawater (synthesis of porous aromatic framework materials, improvement of adsorption performance, cost reduction and in-depth study of the mechanism, etc.).

Key words: porous aromatic framework, uranium extraction from seawater, adsorbents, synthesis, nanomaterials

中图分类号:

O6-1

郭帅帅, 陈锦路, 金梁程龙, 陶醉, 陈小丽, 彭国文. 基于海水提铀的多孔芳香框架材料研究进展[J]. 化工进展, 2023, 42(3): 1426-1436.

GUO Shuaishuai, CHEN Jinlu, JIN Liangchenglong, TAO Zui, CHEN Xiaoli, PENG Guowen. Research progress of porous aromatic frameworks based on uranium extraction from seawater[J]. Chemical Industry and Engineering Progress, 2023, 42(3): 1426-1436.

图/表 9

图1 近年来基于海水提铀的PAFs研究进展[20-30]

表1 基于海水提铀的PAFs材料的合成反应和合成技术

合成反应/合成技术	催化剂	特性	制备的PAFs材料	参考文献
Yamamoto-type Ullmann偶联反应	铜、镍	反应条件温和、功能基团适应性强	PAF-1、PPN-6-PAN	[40]
Suzuki偶联反应	钯、镍	操作简便、亲水性较好、副产物无毒	MIGPAF-12/13	[41-42]
Heck偶联反应	钯	催化活性高、官能团耐受性高	MIPAFs	[43-44]
Scholl反应	AlCl₃	可在碱性条件下反应，成本较低	PAF-170/171/172-AO	[28]
傅-克烷基化反应	AlCl₃	可在强酸条件下反应，操作简单	PPAF-3	[25]
原子转移自由基聚合技术	—	增强引发反应的速率，控制反应的程度	PPN-6-PAN	[45-46]
分子印迹技术	—	提高架构稳定性、增强铀选择性	MISS-PAF-1、PPA@MISS-PAF-1、MIPAFs、MIGPAF-12/13	[47]

图2 Yamamoto-type Ullmann偶联反应机理[40]

图3 Ni催化的Suzuki偶联反应机理[50]

图4 分子印迹技术原理[51]

表2 近年来基于海水提铀的PAFs材料一览

材料名称	配体官能团	孔径 /nm	比表面积 /m²·g^-1	K_d/mL·g^-1	吸附机理	参考文献
PPN-6-PAN	偕胺肟	—	19.5	—	通过密度泛函理论（DFT）研究表明吸附剂通过AO（供电子体）与铀酰（受电子体）进行结合的，结合基序为η²型	[21]
PAF-1-CH₂-AO	偕胺肟	0.7	855	1.05×10⁶	通过X射线吸收精细结构谱（XAFS）分析铀与吸附剂的结合基序与η²型相似，且相邻偕胺肟基团之间存在协同结合	[22]
PAF-1-CH₂NHAO	偕胺肟	—	—	—	通过扩展X射线吸收精细结构谱（EXAFS）阐明了两种吸附剂的胺肟与铀酰是以2∶1方式结合的	[24]
PAF-1-NH(CH₂)₂AO			465	1.15×10⁷	通过扩展X射线吸收精细结构谱（EXAFS）阐明了两种吸附剂的胺肟与铀酰是以2∶1方式结合的	[24]
PAF-170-AO	偕胺肟	0.4~4	312	9.37×10⁶	通过X射线能谱（EDS）和X射线光电子能谱（XPS）证明了铀酰离子与偕胺肟基团进行了螯合作用	[28]
PAF-171-AO			425	—
PAF-172-AO			541	—
PPAF-3	含磷配体	—	37	—	通过XPS和傅里叶变换红外光谱（FTIR）表明吸附剂是通过磷酸配体的P $̿$ O来结合铀酰离子的	[25]
P-C4	含磷配体	7.67	110	2.2×10⁷	通过与N-C2对比发现除阴离子与阳离子之间的静电相互作用外，还可能存在UO $2 2 +$ 的轴向O原子与P原子的空心3d轨道相互作用	[26]
MIPAF-11a	水杨醛肟	—	524	—	通过FTIR和XPS表明吸附剂通过水杨醛肟的N、O原子与铀进行配位的	[23]
MIPAF-11b			297	—
MIPAF-11c			182	6.98×10⁵
MIPAF-11d			95	—
MISS-PAF-1	双水杨醛肟	—	412	1.4×10⁷	通过FTIR和XPS表明吸附剂通过—OH和—C $̿$ N与铀形成U—O和U—N配位键进行化学吸附	[27]
PPA@MISS-PAF-1	双水杨醛肟	—	117	2.18×10⁷	除与MISS-PAF-1相同的吸附机理，该吸附剂在非对称交流电化学（AACE）方法下通过PPA产生的扩大电场来提高对铀的吸附性能	[29]
MIGPAF-12	双水杨醛肟	0.8	178	—	通过XPS、FTIR、XAFS表明吸附剂在-1.3V下产生放大的铀酰局域浓度与双水杨醛肟配体结合产生协同电极，提高了铀吸附效率	[30]
MIGPAF-13		1.1	290	2.0×10⁶		[30]

表2 近年来基于海水提铀的PAFs材料一览

材料名称	配体官能团	孔径 /nm	比表面积 /m²·g^-1	K_d/mL·g^-1	吸附机理	参考文献
PPN-6-PAN	偕胺肟	—	19.5	—	通过密度泛函理论（DFT）研究表明吸附剂通过AO（供电子体）与铀酰（受电子体）进行结合的，结合基序为η²型	[21]
PAF-1-CH₂-AO	偕胺肟	0.7	855	1.05×10⁶	通过X射线吸收精细结构谱（XAFS）分析铀与吸附剂的结合基序与η²型相似，且相邻偕胺肟基团之间存在协同结合	[22]
PAF-1-CH₂NHAO	偕胺肟	—	—	—	通过扩展X射线吸收精细结构谱（EXAFS）阐明了两种吸附剂的胺肟与铀酰是以2∶1方式结合的	[24]
PAF-1-NH(CH₂)₂AO			465	1.15×10⁷	通过扩展X射线吸收精细结构谱（EXAFS）阐明了两种吸附剂的胺肟与铀酰是以2∶1方式结合的	[24]
PAF-170-AO	偕胺肟	0.4~4	312	9.37×10⁶	通过X射线能谱（EDS）和X射线光电子能谱（XPS）证明了铀酰离子与偕胺肟基团进行了螯合作用	[28]
PAF-171-AO			425	—
PAF-172-AO			541	—
PPAF-3	含磷配体	—	37	—	通过XPS和傅里叶变换红外光谱（FTIR）表明吸附剂是通过磷酸配体的P $̿$ O来结合铀酰离子的	[25]
P-C4	含磷配体	7.67	110	2.2×10⁷	通过与N-C2对比发现除阴离子与阳离子之间的静电相互作用外，还可能存在UO $2 2 +$ 的轴向O原子与P原子的空心3d轨道相互作用	[26]
MIPAF-11a	水杨醛肟	—	524	—	通过FTIR和XPS表明吸附剂通过水杨醛肟的N、O原子与铀进行配位的	[23]
MIPAF-11b			297	—
MIPAF-11c			182	6.98×10⁵
MIPAF-11d			95	—
MISS-PAF-1	双水杨醛肟	—	412	1.4×10⁷	通过FTIR和XPS表明吸附剂通过—OH和—C $̿$ N与铀形成U—O和U—N配位键进行化学吸附	[27]
PPA@MISS-PAF-1	双水杨醛肟	—	117	2.18×10⁷	除与MISS-PAF-1相同的吸附机理，该吸附剂在非对称交流电化学（AACE）方法下通过PPA产生的扩大电场来提高对铀的吸附性能	[29]
MIGPAF-12	双水杨醛肟	0.8	178	—	通过XPS、FTIR、XAFS表明吸附剂在-1.3V下产生放大的铀酰局域浓度与双水杨醛肟配体结合产生协同电极，提高了铀吸附效率	[30]
MIGPAF-13		1.1	290	2.0×10⁶		[30]

表3 基于偕胺肟配体的PAFs吸附性能

材料名称	循环性能 /次	铀水溶液		模拟海水		实际海水		参考文献
材料名称	循环性能 /次	铀吸附量/mg·g^-1	吸附条件	铀吸附量/mg·g^-1	吸附条件	铀吸附量/mg·g^-1	吸附条件	参考文献
PPN-6-PAN	—	—	—	65.2	24h, 60mg/L	4.81	42d, 80mg/L	[21]
PAF-1-CH₂-AO	2	304	12h, 7.36mg/L	40	7.05mg/L	—	—	[22]
PAF-1-CH₂NHAO	—	102	24h, 1~400mg/L	—	—	—	—	[24]
PAF-1-NH(CH₂)₂AO	3	385	24h, 1~400mg/L	—	—	36.5	7d, 8mg/L
PAF-170-AO	10	—	—	702	24h, 7mg/L	6	21d, 3.3μg/L	[28]
						8.92	60d, 3.3μg/L
PAF-171-AO	—	—	—	608	24h, 7mg/L	—	—
PAF-172-AO	—	—	—	569	24h, 7mg/L	—	—

表4 基于含磷配体的PAFs吸附性能

吸附剂

名称

循环性能

/次

铀水溶液

参考

文献

表5 基于水杨醛肟配体的PAFs吸附性能

吸附剂名称	循环性能 /次	铀水溶液		模拟海水		实际海水		参考文献
吸附剂名称	循环性能 /次	铀吸附量/mg·g^-1	吸附条件	铀吸附量/mg·g^-1	吸附条件	铀吸附量/mg·g^-1	吸附条件	参考文献
MIPAF-11a	—	0.02	40min, 20mg/L	—	—	—	—	[23]
MIPAF-11b	—	21.4	40min, 20mg/L	—	—	—	—
MIPAF-11c	10	37.28	40min, 20mg/L	35.44	1h, 7.05mg/L	—	—
MIPAF-11d		35.48	40min, 20mg/L	—	—	—	—
MISS-PAF-1	4	253	50~200mg/L	73.26	7.05mg/L	5.79	56d, 4.4μg/L	[27]
PPA@MISS-PAF-1	10	—	—	—	—	307.3	60min, 8mg/L	[29]
						16.5	90d, 3.3μg/L
MIGPAF-12	—	—	—	—	—	367.4	60min, 8mg/L	[30]
MIGPAF-13	6	—	—	—	—	419.2	60min, 8mg/L

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基于海水提铀的多孔芳香框架材料研究进展

Research progress of porous aromatic frameworks based on uranium extraction from seawater

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