高镁锂比盐湖镁锂分离与锂提取技术研究进展

doi:10.11949/0438-1157.20201715

化工学报 ›› 2021, Vol. 72 ›› Issue (6): 2905-2921.DOI: 10.11949/0438-1157.20201715

• 青海盐湖资源综合利用专栏 • 上一篇下一篇

高镁锂比盐湖镁锂分离与锂提取技术研究进展

王琪¹(),赵有璟^1,²,刘洋¹,王云昊¹,王敏²(),项顼¹()

^1.北京化工大学化工资源有效利用国家重点实验室，北京 100029
^2.中国科学院青海盐湖研究所，中国科学院盐湖资源综合高效利用重点实验室，青海省盐湖资源化学重点实验室，青海西宁 810008

收稿日期:2020-11-30 修回日期:2021-03-12 出版日期:2021-06-05 发布日期:2021-06-05
通讯作者: 王敏,项顼
作者简介:王琪（1995—），女，硕士研究生，913625998@qq.com
基金资助:
国家自然科学基金项目(U20A20138);中央高校基本科研业务费专项资金(XK1803)

Recent advances in magnesium/lithium separation and lithium extraction technologies from salt lake brine with high magnesium/lithium ratio

WANG Qi¹(),ZHAO Youjing^1,²,LIU Yang¹,WANG Yunhao¹,WANG Min²(),XIANG Xu¹()

^1.State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China
^2.Key Laboratory of Comprehensive and Highly Efficient Utilization of Salt Lake Resources, Qinghai Provincial Key Laboratory of Resources and Chemistry of Salt Lakes, Qinghai Institute of Salt Lakes, Chinese Academy of Sciences, Xining 810008, Qinghai, China

Received:2020-11-30 Revised:2021-03-12 Online:2021-06-05 Published:2021-06-05
Contact: WANG Min,XIANG Xu

摘要/Abstract

摘要：

随着锂离子电池在电动汽车、便携式电子设备、电动工具及电网储能中的用量持续增加，锂资源需求量快速增长。我国盐湖集中分布在青藏高原地区，青海盐湖普遍具有高镁锂比、低锂含量的特征。高镁锂比盐湖提锂是世界性难题。本文综述了高镁锂比盐湖卤水镁锂分离与锂提取技术的最新研究进展，包括萃取法、吸附法、反应/分离耦合技术、膜法和电化学法。从各技术原理、特点、性能等方面分析了各方法特征和适用性。在现有技术中，吸附法更适合高镁锂比卤水；萃取法可用于锂浓度较低的卤水；新发展的反应/分离耦合技术能实现高效提锂与镁锂资源综合利用；以纳滤、电渗析、双极膜为代表的膜法具有能耗较低和模块化的优点；电化学法具有装置简单的优势，但仍需进一步优化系统。我国盐湖锂资源提取需提高总收率，提升提锂后资源综合利用程度，发展锂产品高值化、多元化利用途径，加强盐湖提锂的工程化技术研究，突破并掌握核心技术与装备，实现盐湖资源高效、综合、可持续利用的目标。

关键词: 盐湖卤水, 镁锂分离, 锂提取, 吸附剂, 电化学, 膜

Abstract:

As the use of lithium-ion batteries in electric vehicles, portable electronic devices, power tools, and grid energy storage continues to increase, the demand for lithium resources is growing rapidly. In China, over 71% of lithium resources are stored in salt lakes, which are abundant in the Qinghai-Tibet Plateau. Among them, salt lakes in Qinghai province generally have the characteristics of high ratio of magnesium to lithium and low lithium content. Lithium extraction from high Mg/Li ratio salt lakes is a great challenge worldwide. This review focuses on the latest progress of Mg/Li separation and lithium extraction technologies from salt lake brine with high Mg/Li ratio. We comprehensively analyzed the features and applications in terms of principles, characteristics and performance of each method including extraction, adsorption, reaction/separation coupling technology, membrane and electrochemical method. The adsorption method is more suitable for high Mg/Li brine. The extraction method can be used for brine with a lower lithium concentration. The emerging new reaction-coupled separation technology can achieve high-efficiency lithium extraction and comprehensive utilization of magnesium and lithium resources. The membrane methods like nanofiltration, electrodialysis and bipolar membranes have the advantages of lower energy consumption and modularity. The electrochemical method has the simple equipment, but the system needs to be optimized yet. The extraction of lithium from salt lakes requires to increase the total yield, to improve the comprehensive utilization of related resources, to develop high-valued lithium products, and to strengthen the engineering technology. Finally, the goal is to utilize salt lake resources more efficiently, comprehensively and sustainably.

Key words: salt lake brine, Mg/Li separation, lithium extraction, adsorbent, electrochemistry, membrane

中图分类号:

TQ 131.1

王琪, 赵有璟, 刘洋, 王云昊, 王敏, 项顼. 高镁锂比盐湖镁锂分离与锂提取技术研究进展[J]. 化工学报, 2021, 72(6): 2905-2921.

WANG Qi, ZHAO Youjing, LIU Yang, WANG Yunhao, WANG Min, XIANG Xu. Recent advances in magnesium/lithium separation and lithium extraction technologies from salt lake brine with high magnesium/lithium ratio[J]. CIESC Journal, 2021, 72(6): 2905-2921.

图/表 19

图1 全球锂最终用途市场分布情况[1]

Fig.1 Distribution of global end-use markets of lithium[1]

表1 中国主要高镁锂比盐湖卤水资源组成

Table 1 The compositions of high Mg/Li ratio salt lake brines in China

盐湖地区	镁/锂质量比	锂离子浓度/(g/L)	镁离子浓度/(g/L)	文献
察尔汗	1437.5	0.08	115.0	[4]
一里坪	63.7	0.379	24.15	[4]
龙木错	74.0	1.21	89.5	[5]
西台吉乃尔	59.1	0.26	15.36	[6]
东台吉乃尔	40.3	0.14	5.64	[6]
大柴旦	133.8	0.016	2.14	[7]

图2 七级逆流萃取流程图[10]

Fig.2 Flow chart of seven-stage countercurrent extraction[10]

图3 TBP/FeCl3/P507用于萃取提锂机理[14]

Fig.3 Mechanism of TBP/FeCl3/P507 for extraction of lithium[14]

图4 三阶段SCT的过程图 [15]

Fig.4 Process diagram of three-stage SCT[15]

图5 尖晶石LiMn2O4的晶体结构（锰离子驻留在氧离子形成的八面体中。虚线箭头表示锂的扩散路径）(a)；锂扩散通道从四面体8a位置通过由六个空位包围的八面体16c空位到相邻的8a位置的示意图(b)[23]

Fig.5 Crystal structure of spinel LiMn2O4(Manganese ions reside in the octahedra formed by oxygen ions. The dotted arrow denotes a lithium diffusion path) (a); Schematic illustration of the lithium diffusion channel from a tetrahedral 8a site to an adjacent 8a site through an octahedral 16c vacancy surrounded by six manganese ions in the octahedral 16d gate sites (b)[23]

图6 用EGDE交联球形CTS/LMO示意图[31]

Fig.6 Schematic diagram of cross-linking spherical CTS/LMO with EGDE[31]

图7 锂钛酸盐的晶体结构[33]

Fig.7 Crystal structure of lithium titanate[33]

图8 P-HTO-NF锂回收示意图[35]

Fig.8 Schematic diagram of P-HTO-NF lithium recovery[35]

图9 Al(OH)3吸附Li+转化为LiAl-LDH示意图[41]

Fig.9 Schematic diagram of Al(OH)3 adsorption of Li+ into LiAl-LDH[41]

图10 反应/分离耦合技术从盐湖卤水中分离镁、锂并制备LDHs产品流程[58]

Fig.10 Scheme of Mg/Li separation and LDHs preparation by reaction-coupled separation technology [58]

图11 反应/分离耦合技术分离盐湖卤水中镁、锂的理论判据边界条件[59]

Fig.11 Theoretical criterion and boundary conditions for separation of magnesium and lithium in salt lake brine by reaction-coupled separation technology[59]

图12 合成LiAl-LDHs并制备有序空位型锂吸附剂高选择性捕获锂离子[60]

Fig.12 Scheme of selective capture of lithium ions by ordered vacancy adsorbent prepared by LiAl-LDHs[60]

图13 电渗析过程示意[73]

Fig.13 Schematic diagram of the electrodialysis process[73]

图14 液膜萃取和电渗析夹心式液膜电渗析系统回收Li+[77]

Fig.14 Liquid membrane extraction and electrodialysis sandwich liquid membrane electrodialysis recovery Li+ system[77]

图15 BMED与NF、RO、CED一体化膜从盐湖卤水中制取LiOH[79]

Fig.15 Schematic diagram of the production of LiOH from salt lake brine with integrated membranes of BMED, NF, RO and CED[79]

图16 采用LiFePO4-Ag体系进行电化学锂回收[87]

Fig.16 LiFePO4-Ag system for electrochemical lithium recovery process[87]

图17 利用LiFePO4/FePO4结构电化学提取锂[90]

Fig.17 Structure of the LiFePO4/FePO4 for electrochemical lithium extraction[90]

表2 现有盐湖卤水锂提取技术比较

Table 2 Summary of existing lithium extraction techniques

方法		优势	尚存问题
萃取法	有机溶剂萃取	选择性高	成本高，腐蚀，严重环境污染
萃取法	离子液体萃取	污染较有机萃取剂少，绿色环保	萃取剂制取复杂、造价高
吸附法	锰系离子筛	吸附容量高，选择性高	酸处理腐蚀污染，吸附剂溶损严重
	钛系离子筛	吸附容量高，稳定	酸处理吸附剂溶损严重，易团聚
	铝系吸附剂	选择性高，不需酸处理	吸附容量低，造粒后容量衰减
反应/分离耦合法		反应条件温和，镁锂同时回收，资源综合利用率高	引入钠盐
膜法	纳滤	流程简单、尺寸筛选效应高	镁离子透过率较高，膜易污染、前处理要求较高
	电渗析	能耗低，有效分离二价离子	无法分离单价金属离子
	双极膜	能耗低，直接合成LiOH	无法处理高镁锂比卤水
电化学法	离子捕获系统	无酸洗脱，稳定性强	能耗高，电解液要求高，耗电量大
电化学法	摇椅电池系统	可逆性，环境友好性	能耗高，电解液要求高，耗电量大

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高镁锂比盐湖镁锂分离与锂提取技术研究进展

Recent advances in magnesium/lithium separation and lithium extraction technologies from salt lake brine with high magnesium/lithium ratio

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