层状结构铝系吸附剂在盐湖提锂领域的研究

doi:10.11949/0438-1157.20231035

摘要/Abstract

摘要：

随着动力电池车的快速发展和广泛应用，锂资源的需求量急剧增加。如何实现我国具有国际资源优势的盐湖锂资源高效利用开发是近几十年来盐湖化工产业亟需解决的关键问题。与国外已实现开发利用的盐湖相比，除了西藏部分盐湖以外，我国盐湖锂资源大多是锂浓度低至几十mg/L、镁锂比极高（约500，甚至更高）的低品位资源。截至目前，基于我国盐湖锂资源的特征，已开发了几种盐湖提锂方法，如膜法、吸附法、太阳池法、溶剂萃取法和电化学法等，部分已成功应用于实际盐湖卤水提锂产业化生产中。其中，吸附法因高Li⁺选择性、良好的适用性、工艺简单、绿色高效和可循环利用等特性而备受关注。层状结构铝系吸附剂（Li/Al-LDHs）因具有较高的选择性、绿色环保等优势已成功实现产业化应用。然而，该类吸附剂在规模化应用时仍存在动态吸附容量极低、粉化严重等问题，有待进一步深入研究探讨。从Li/Al-LDHs吸附性能与晶体结构间构效关系出发，梳理总结了Li/Al-LDHs吸附剂循环周期短、应用性能差的原因，并从结构稳定性的角度出发，提出了性能提升的解决方案。

关键词: 锂, 盐湖, 吸附剂, 晶体结构, 结构稳定性

Abstract:

With the rapid development and wide application of power battery vehicles, the demand for lithium resources has increased sharply. How to realize the efficient utilization and development of lithium resources in salt lakes, which has international resource advantages in China, is a key issue that the salt lake chemical industry needs to solve urgently in recent decades. Compared with the salt lakes that have been developed and utilized abroad, except for some salt lakes in Xizang, the lithium resources in China's salt lakes are mostly low-grade resources with lithium concentrations as low as tens of mg/L and extremely high magnesium lithium ratio (about 500 or even higher). Up to now, based on the characteristics of lithium resources in salt lakes, several methods have been developed to extract lithium from salt lakes, such as membrane method, adsorption method, solar pool method, solvent extraction method and electrochemical method, some of which have been successfully applied in the actual industrial production of lithium extraction from salt lake brines. Especially, adsorption method has attracted much attention due to its characteristics of high Li⁺ selectivity, good applicability, simple process, green efficiency and recyclability. Layer-structured aluminum-based adsorbents (Li/Al-LDHs) have been successfully industrialized due to their high selectivity, green environmental protection and other advantages. However, there are still some problems such as extremely low dynamic adsorption capacity and serious pulverization in the large-scale application of this kind of adsorbent, which need further study and discussion. Therefore, based on the structure-activity relationship between the adsorption properties of Li/Al-LDHs and the crystal structure, this paper summarized the reasons for the short cycle period and poor application performance of Li/Al-LDHs adsorbent, and proposed the performance improvement scheme from the perspective of structural stability.

Key words: lithium, salt lake, adsorbents, crystal structure, structure stability

中图分类号:

TQ 028

李彦乐, 刘宜林, 霍俊杰, 孙艳霞, 董生德, 贺欣, 许琪, 马路祥, 周园, 海春喜. 层状结构铝系吸附剂在盐湖提锂领域的研究[J]. 化工学报, 2023, 74(12): 4777-4791.

Yanle LI, Yilin LIU, Junjie HUO, Yanxia SUN, Shengde DONG, Xin HE, Qi XU, Luxiang MA, Yuan ZHOU, Chunxi HAI. Research progress of aluminum adsorbents in lithium extraction from salt lakes[J]. CIESC Journal, 2023, 74(12): 4777-4791.

图/表 16

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名称	国家	Li⁺/% (质量分数)	Mg²⁺/% (质量分数)	Mg²⁺/Li⁺
阿塔卡马盐湖	智利	0.157	0.965	6.147
乌尤尼盐湖	玻利维亚	0.032	0.650	20.313
银峰盐湖	美国	0.030	0.040	1.333
大盐湖	美国	0.006	0.800	133.333
斯马科弗盐湖	美国	0.038	0.750	19.737
克莱顿谷盐湖	美国	0.016	0.019	1.188
东台吉乃尔盐湖	中国	0.085	2.990	35.176
西台吉乃尔盐湖	中国	0.021	1.280	60.952
一里坪盐湖	中国	0.022	2.000	90.909
扎布耶盐湖城	中国	0.970	0.001	0.001
大柴旦盐湖	中国	0.020	1.300	65.000
扎布耶南湖	中国	0.141	0.0004	0.003
扎布耶北湖	中国	0.153	0.002	0.013
察尔汗盐湖	中国	0.0013	2.370	1823.077

名称	国家	Li⁺/% (质量分数)	Mg²⁺/% (质量分数)	Mg²⁺/Li⁺
阿塔卡马盐湖	智利	0.157	0.965	6.147
乌尤尼盐湖	玻利维亚	0.032	0.650	20.313
银峰盐湖	美国	0.030	0.040	1.333
大盐湖	美国	0.006	0.800	133.333
斯马科弗盐湖	美国	0.038	0.750	19.737
克莱顿谷盐湖	美国	0.016	0.019	1.188
东台吉乃尔盐湖	中国	0.085	2.990	35.176
西台吉乃尔盐湖	中国	0.021	1.280	60.952
一里坪盐湖	中国	0.022	2.000	90.909
扎布耶盐湖城	中国	0.970	0.001	0.001
大柴旦盐湖	中国	0.020	1.300	65.000
扎布耶南湖	中国	0.141	0.0004	0.003
扎布耶北湖	中国	0.153	0.002	0.013
察尔汗盐湖	中国	0.0013	2.370	1823.077

方法	商业化利用盐湖	优势	劣势
膜法	青海一里坪盐湖 (五矿盐湖有限公司) 青海西台吉乃尔盐湖 (青海中信国安锂业发展有限公司)	显著降低卤水中的镁锂比，降低了后续提锂难度	易堵塞、重复利用率低、对卤水总盐度控制要求高
吸附法	青海察尔汗盐湖 (青海盐湖蓝科锂业股份有限公司) (西藏藏格锂业科技有限公司)	高选择性、低成本、高效率、无污染	淡水消耗大、吸附容量不稳定、粉体吸附剂的流动性差、循环稳定性差、核心吸附剂关键材料性能提升仍需技术攻关
太阳池法	阿塔卡马盐湖，银峰盐湖(SQM, AL) 西藏扎布耶盐湖(西藏国能矿业发展有限公司)	绿色环保，充分利用盐湖区太阳能、风能等提高盐湖的蒸发率，方便生产钾等副产品	需要大规模建设并维护盐田，初始投资金额大、较适用于低镁锂比盐湖，回收率低
溶剂萃取法	青海大柴旦盐湖(青海柴达木兴华锂盐有限公司) (青海博华锂业有限公司)	操作可连续化，速度快，生产周期短	有机溶剂有毒易燃，易腐蚀设备、成本高、环保压力大
电化学法	西藏捌仟错盐湖 (江苏中南锂业有限公司) (西藏珠峰资源股份有限公司)	高选择性、绿色环保、低成本	循环性有待提高、相关工艺仍需进一步优化、能耗相对较高

方法	商业化利用盐湖	优势	劣势
膜法	青海一里坪盐湖 (五矿盐湖有限公司) 青海西台吉乃尔盐湖 (青海中信国安锂业发展有限公司)	显著降低卤水中的镁锂比，降低了后续提锂难度	易堵塞、重复利用率低、对卤水总盐度控制要求高
吸附法	青海察尔汗盐湖 (青海盐湖蓝科锂业股份有限公司) (西藏藏格锂业科技有限公司)	高选择性、低成本、高效率、无污染	淡水消耗大、吸附容量不稳定、粉体吸附剂的流动性差、循环稳定性差、核心吸附剂关键材料性能提升仍需技术攻关
太阳池法	阿塔卡马盐湖，银峰盐湖(SQM, AL) 西藏扎布耶盐湖(西藏国能矿业发展有限公司)	绿色环保，充分利用盐湖区太阳能、风能等提高盐湖的蒸发率，方便生产钾等副产品	需要大规模建设并维护盐田，初始投资金额大、较适用于低镁锂比盐湖，回收率低
溶剂萃取法	青海大柴旦盐湖(青海柴达木兴华锂盐有限公司) (青海博华锂业有限公司)	操作可连续化，速度快，生产周期短	有机溶剂有毒易燃，易腐蚀设备、成本高、环保压力大
电化学法	西藏捌仟错盐湖 (江苏中南锂业有限公司) (西藏珠峰资源股份有限公司)	高选择性、绿色环保、低成本	循环性有待提高、相关工艺仍需进一步优化、能耗相对较高

吸附剂	原料	条件	吸附性能	文献
Al(OH)₃	AlCl₃·6H₂O，NaOH，brine	T = 30℃ C(Li⁺) ≈ 1145 mg/L	吸附率76.4%	[52]
Al(OH)₃	AlCl₃·6H₂O，KOH，LiCl	T = 80℃ C(Li⁺) ≈ 208~350 mg/L	吸附率95%	[48]
Al(OH)₃	AlCl₃·6H₂O，NaOH，brine	T = 30℃ C(Li⁺) ≈ 5.5~19.5 mg/L	吸附率93%	[50]
Al(OH)₃	Al(OH)₃，LiOH·H₂O，HCl	—	吸附率91%	[53]
Al(OH)₃	铝粉，NaCl，brine	C(Li⁺) ≈ 1000 mg/L Mg²⁺/Li⁺≈ 20	吸附率78.3%	[54]
Li/Al-LDHs	AlCl₃·6H₂O，NaOH，Na₂CO₃	C(Li⁺) ≈ 675 mg/L Mg²⁺/Li⁺≈ 0.08 Na⁺/Li⁺≈ 48.7	吸附率96.07%	[55]
Li/Al-LDHs	LiCl, AlCl₃，NaOH	C(Li⁺) ≈ 399 mg/L Mg²⁺/Li⁺ ≈ 302	吸附容量 ≈ 7.27 mg/g	[57]
Li/Al-LDHs	AlCl₃·6H₂O，NaOH，LiCl	C(Li⁺) ≈ 399 mg/L Mg²⁺/Li⁺≈ 302	吸附容量 ≈ 5.69 mg/g	[58]
Li/Al-LDHs	Fe₃O₄，AlCl₃·6H₂O，NaOH，LiCl	C(Li⁺) ≈ 370 mg/L Mg²⁺/Li⁺≈ 330	吸附容量 ≈ 6 mg/g	[59]
Li/Al-LDHs	Al₂(SO₄)₃·18H₂O，LiOH·H₂O，尿素	C(Li⁺) ≈ 969 mg/L Mg²⁺/Li⁺≈ 35 Na⁺/Li⁺≈ 80	吸附容量 ≈ 9.16 mg/g	[21]
Li/Al-LDHs	LiCl，尿素，铝箔	C(Li⁺) ≈ 527 mg/L	吸附率60%	[60]
Li-Al-O-OH	LiCl，尿素，铝箔，Na₂SO₄	C(Li⁺) ≈ 527 mg/L	吸附率55%	[61]