膜技术分离稀土金属元素的研究进展

doi:10.16085/j.issn.1000-6613.2021-2597

摘要/Abstract

摘要：

稀土金属元素是我国重要的战略资源，因其在高精尖产品中的独特作用，稀土金属元素的分离纯化显得格外重要。膜分离技术是一种高效率、低能耗、环境友好的分离手段，在众多领域应用广泛，将其用于稀土金属分离可明显提升分离效率，降低稀土工业对环境的破坏，但目前的研究尚处于起步阶段，将面临较多挑战。本文介绍了膜技术分离稀土金属的三种策略，包括离子印迹膜、聚合物包合膜和液膜，总结了膜材料的制备方法和分离性能，分析比较了膜技术细分类型的特点和利弊。本文还指出离子印迹膜的选择分离性优势巨大，但在吸附容量上仍有提升空间，也是未来几年膜分离技术的研究重点；聚合物包合膜和液膜分离技术，可根据萃取剂类型和用量灵活调整活性位点种类和数量，在膜技术分离稀土金属的工业化应用方面具有较大潜力。

关键词: 稀土金属, 膜分离, 离子印迹, 包合膜, 液膜

Abstract:

Rare earth metals are regards as the essential strategic resources in China due to the unique roles in high-precision products. The separation and purification of rare earth elements is particularly important in order to satisfy the high purity criterion of products. Membrane separation technology is a highly efficient, low power consuming and environmental-friendly separation method, which can be widely used in extensive fields. In addition, their application in rare earth metal separation can efficiently improve the separation properties and greatly decrease the serious environment pollutions caused by the rare earth separation and its related industries. Hence, the scientific researches on these issues are highly crucial but still facing challenges. In this review, three kinds of membrane separation strategies, including ion imprinted membrane, polymer inclusion membrane and liquid membrane, were systematically introduced. Moreover, the preparation methods and separation properties of membrane materials were summarized, and the characteristics, advantages and disadvantages of subdivision types of membrane technology were discussed and compared. Furthermore, Ion imprinted membrane exhibited the great advantages in separation selectivity, but further improvement of adsorption capacity was highly needed, which was also the research focus of membrane separation technology in the next few years. Polymer inclusion membrane and liquid membrane separation technology showed the great potentials in the rare earth separation using membrane technology in the industrial application because it can flexibly adjust the type and quantity of active sites targeting at rare earth separation according to the type and amount of extractant.

Key words: rare earth, membrane separation, ion imprinted, polymer inclusion membrane, liquid membrane

中图分类号:

TQ028

张逸, 刘东昊, 丁一刚. 膜技术分离稀土金属元素的研究进展[J]. 化工进展, 2022, 41(10): 5567-5577.

ZHANG Yi, LIU Donghao, DING Yigang. Research progress of membrane technology for the separation of rare earth elements[J]. Chemical Industry and Engineering Progress, 2022, 41(10): 5567-5577.

图/表 6

参考文献 69

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膜骨架	载体	稀土金属	主要研究结果	文献
PVDF	P227	Lu	载体质量分数40%、稀土浓度1mmol·L^-1时，萃取率91%	［27］
PVDF	P227	Lu/Sm/La	pH=1.5时，对Lu、Sm、La回收率为82%、40%、4%	［28］
EVOH	Cyanex272	Lu	处理能力较大，但载体质量分数25%时分离选择性3.78	［29］
PAN	Calix8	La	静电纺丝法制备，吸附容量达155.10mg·g^-1	［30］
PVC	P204	La/Gd/Y	载体质量分数45%、pH=1.5时，萃取率接近100%	［31］
CTA	D2EHAF	Sc	可选择性分离混合液中Sc，重复用5次萃取率基本不变	［32］
CA	CMPO	Ce	稀土浓度200mg·L^-1时，萃取率大于90%	［33］
CA	TODGA	Ce	稀土浓度200mg·L^-1时，扩散系数为6.65×10^-12m²·s^-1	［34］
PVDF	［A336］［P507］	Lu/Yb	载体质量分数37.5%时，对Yb的选择性高于Lu	［35］
PVDF	［A336］［P227］	Y	载体质量分数37.5%、稀土浓度1.1mmol·L^-1时，可重复用8次	［36］
PVDF	Cyphos 104	Lu/Yb	载体质量分数25%、稀土浓度20mmol·L^-1时，分离选择性1.37	［37］

膜骨架	载体	稀土金属	主要研究结果	文献
PVDF	P227	Lu	载体质量分数40%、稀土浓度1mmol·L^-1时，萃取率91%	［27］
PVDF	P227	Lu/Sm/La	pH=1.5时，对Lu、Sm、La回收率为82%、40%、4%	［28］
EVOH	Cyanex272	Lu	处理能力较大，但载体质量分数25%时分离选择性3.78	［29］
PAN	Calix8	La	静电纺丝法制备，吸附容量达155.10mg·g^-1	［30］
PVC	P204	La/Gd/Y	载体质量分数45%、pH=1.5时，萃取率接近100%	［31］
CTA	D2EHAF	Sc	可选择性分离混合液中Sc，重复用5次萃取率基本不变	［32］
CA	CMPO	Ce	稀土浓度200mg·L^-1时，萃取率大于90%	［33］
CA	TODGA	Ce	稀土浓度200mg·L^-1时，扩散系数为6.65×10^-12m²·s^-1	［34］
PVDF	［A336］［P507］	Lu/Yb	载体质量分数37.5%时，对Yb的选择性高于Lu	［35］
PVDF	［A336］［P227］	Y	载体质量分数37.5%、稀土浓度1.1mmol·L^-1时，可重复用8次	［36］
PVDF	Cyphos 104	Lu/Yb	载体质量分数25%、稀土浓度20mmol·L^-1时，分离选择性1.37	［37］

类型	载体	稀土金属	主要研究结果	文献
ELM	苯胺	RE	表面活性剂T154、有机相磺化煤油时，可从磷矿浸取液中萃取出93%的混合RE	［38］
ELM	Cyanex272	Dy	表面活性剂Span80/85、有机相煤油时，萃取率99.6%	［39］
EPLM	P507	Y/La/Sm/Al	金属总浓度1.22g·L^-1、电压4.5~5kV时，回收率分别为97.7%、90.3%、19.7、95.1%	［40］
EPLM	PMBP	Sc	稀土浓度10mg·L^-1、电压5kV时，萃取率96.9%	［41］
BOLM	N1923	RE/Al	稀土浓度116.68mg·L^-1、Al浓度27.7mg·L^-1时，RE/Al选择性为44.89，稀土回收率为84.4%	［42］
BOLM	P507	RE	稀土浓度116.68mg·L^-1时，稀土回收率为90%以上	［43］
FSLM	D2EHPA	Eu	PVDF为膜骨架、稀土浓度0.1mmol·L^-1时，萃取率94.2%	［44］
FSLM	TODGA	RE	PVDF为膜骨架、稀土浓度72.4mg·L^-1时，可从含有Ca/Mg/Fe/RE的磷矿模拟废液中萃取出96.3%的RE	［45］
HFSLM	PC-88A	Nd	4mol·L^-1硝酸时，萃取率95%，反萃率87%	［46］
HFSLM	D2EHPA	Nd/Pr/Dy	2mol·L^-1硝酸时，萃取率分别58.62%、85.59%、98.46%	［47］
HFLM	TODGA	Nd	稀土浓度1g·L^-1、3.5mol·L^-1硝酸时，萃取率接近100%	［48］
HFLM	PC-88A	Dy	0.3mol·L^-1硝酸时，通过二级萃取可从含有20%Dy的FeNdB磁铁中回收高纯度Dy（>97%）	［49］

类型	载体	稀土金属	主要研究结果	文献
ELM	苯胺	RE	表面活性剂T154、有机相磺化煤油时，可从磷矿浸取液中萃取出93%的混合RE	［38］
ELM	Cyanex272	Dy	表面活性剂Span80/85、有机相煤油时，萃取率99.6%	［39］
EPLM	P507	Y/La/Sm/Al	金属总浓度1.22g·L^-1、电压4.5~5kV时，回收率分别为97.7%、90.3%、19.7、95.1%	［40］
EPLM	PMBP	Sc	稀土浓度10mg·L^-1、电压5kV时，萃取率96.9%	［41］
BOLM	N1923	RE/Al	稀土浓度116.68mg·L^-1、Al浓度27.7mg·L^-1时，RE/Al选择性为44.89，稀土回收率为84.4%	［42］
BOLM	P507	RE	稀土浓度116.68mg·L^-1时，稀土回收率为90%以上	［43］
FSLM	D2EHPA	Eu	PVDF为膜骨架、稀土浓度0.1mmol·L^-1时，萃取率94.2%	［44］
FSLM	TODGA	RE	PVDF为膜骨架、稀土浓度72.4mg·L^-1时，可从含有Ca/Mg/Fe/RE的磷矿模拟废液中萃取出96.3%的RE	［45］
HFSLM	PC-88A	Nd	4mol·L^-1硝酸时，萃取率95%，反萃率87%	［46］
HFSLM	D2EHPA	Nd/Pr/Dy	2mol·L^-1硝酸时，萃取率分别58.62%、85.59%、98.46%	［47］
HFLM	TODGA	Nd	稀土浓度1g·L^-1、3.5mol·L^-1硝酸时，萃取率接近100%	［48］
HFLM	PC-88A	Dy	0.3mol·L^-1硝酸时，通过二级萃取可从含有20%Dy的FeNdB磁铁中回收高纯度Dy（>97%）	［49］

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