电化学提锂中的法拉第材料：进展、挑战与性能强化方法

doi:10.1016/j.actphy.2025.100127

摘要/Abstract

摘要：

电动汽车行业的快速增长导致锂产品需求激增，推动了先进锂提取技术的发展。其中，电化学提锂技术因其优异锂选择性(相较于竞争性阳离子，如Na⁺和Mg²⁺)、高能效和环境可持续性被认为具有发展前景。关于法拉第材料、操作模式/参数和装置构型的研究已大量发表。尽管已有一些关于电化学提锂技术的综述发表，但仍缺乏系统性总结电化学提锂中法拉第材料研究进展、分析其固有性质如何影响提锂性能并阐明性能增强策略与关键提锂性能指标之间联系的全面综述。在此，我们系统地介绍了电化学提锂技术的原理并汇总了文献中涉及的所有性能指标，包括锂离子嵌入容量、锂离子提取速率、容量保持率、选择性系数(或纯度)、能耗和电流效率。我们全面分析了用于电化学提锂的法拉第材料，其中包括LiFePO₄、LiMn₂O₄、层状镍钴锰氧化物、Li₃V₂(PO₄)₃和Li_1.6Mn_1.6O₄，构建了其性质与性能间的内在关系，并比较了每种材料的优缺点。此外，我们对不同的性能增强策略进行了分类和评估，包括材料设计方法(如3D结构制造、晶体调控、元素掺杂和表面包覆)，以及涉及进水流向、充放电模式和操作参数等方面的条件优化方法，并进一步阐明了每种方法如何影响电化学提锂的某一/某些性能及其内在影响机制。我们同时综述了基于每种法拉第材料的电化学提锂技术的工业化进展及材料成本。本综述旨在通过建立材料设计、操作条件优化和性能结果间的联系，为从事新型电化学提锂法拉第材料研究的学者和工程师提供有价值的见解，并启发法拉第材料开发和工艺优化的创新方法，为实现更可持续和更具成本效益的卤水锂资源开发提供参考。

关键词: 法拉第材料, 提锂, 性能强化, 电化学方法

Abstract:

The rapid growth of the electric vehicle industry has led to a surge in demand for lithium products, driving the development of advanced lithium extraction technologies. Among these, electrochemical lithium extraction has emerged as a promising approach due to its superior lithium selectivity towards competing cations (like Na⁺ and Mg²⁺), high energy efficiency, and environmental sustainability. Many works about the faradaic materials, operation modes/parameters, and cell configurations have been published. Although some reviews about electrochemical lithium extraction technology have been published, there remains a lack of comprehensive reviews that systematically summarize advancements of faradaic materials employed in lithium extraction, analyze how their nature affects the lithium extraction performance, and elucidate the relationship between performance-enhancing strategies and their impact on critical extraction metrics. Here, we systematically introduce the principle of electrochemical lithium extraction technologies and all the performance indices reported in the literature, including the lithium intercalation capacity, lithium extraction rate, capacity retention, selectivity factor (or purity), energy consumption, and current efficiency. We present a comprehensive analysis of the reported faradaic materials used to extract lithium, involving LiFePO₄, LiMn₂O₄, layered nickel cobalt manganese oxides, Li₃V₂(PO₄)₃, and Li_1.6Mn_1.6O₄, establish the interconnection between their attributes and performance, and compare the advantages and disadvantages of each material. Furthermore, we categorize and evaluate different performance-enhancing strategies, including material-design approaches (e.g., 3D structure fabrication, crystal regulation, element doping, and surface coating) and operation-optimized methods in water-flow direction, circuit operation mode, and operation parameters; we further clarify how each method influences specific aspects of electrochemical lithium extraction performance and the underlying mechanisms responsible for these improvements. The industrialization progress of electrochemical lithium extraction technology based on each faradaic material is reviewed, and the cost of these materials is introduced. By establishing a connection between material design, operational optimization, and performance outcomes, this review aims to provide valuable insights for researchers and engineers working on the next generation of faradaic materials employed in electrochemical lithium extraction and to inspire innovative approaches in faradaic material development and process optimization, paving the way for more sustainable and cost-effective lithium recovery from brines.

Key words: Faradaic materials, Lithium extraction, Performance enhancement, Electrochemical method

王雷, 张盼盼, 郭志远, 汪婧, 马杰, 纪志永. 电化学提锂中的法拉第材料：进展、挑战与性能强化方法[J]. 物理化学学报, 2026, 42(1), 100127. doi: 10.1016/j.actphy.2025.100127

Lei Wang, Panpan Zhang, Zhiyuan Guo, Jing Wang, Jie Ma, Zhi-yong Ji. Electrochemical lithium extraction by the faradaic materials: advances, challenges and enhancement approaches[J]. Acta Phys. -Chim. Sin. 2026, 42(1), 100127. doi: 10.1016/j.actphy.2025.100127

链接本文: https://www.whxb.pku.edu.cn/CN/10.1016/j.actphy.2025.100127

https://www.whxb.pku.edu.cn/CN/Y2026/V42/I1/100127

图/表 15

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表2

Modification method	Material	c (mmol L⁻¹) ^**	V/I	Q_{intercalation} (mg g⁻¹)	r_{Li-extraction} (mg g⁻¹ min⁻¹)	Stability ^***	α ^****	E (Wh mol⁻¹)	Ref.
3D structure fabrication	RGO/LiMn₂O₄	Li 21, Na 330 K 46, Ca 7.7 Mg 4	1.2 V	13.0	0.11	90.7% after 50 cycles***	Li/Na 473.89 Li/K 74.86 Li/Ca 63.07 Li/Mg 38.55	–	[26]
	multiple-crack-porous LiFePO₄	Li 95.7 Na 4226.1 K 392.3 ^**	20 A m⁻²	27.5	–	91.6% 120 cycles	Li/Na 199.9	–	[48]
	LiMn₂O₄/C	Li 39.4 Na 92.8 K 17.7 Mg 3504.4 Ca 2.9 ^**	1.2 V	18.3	0.15	–	Li/Mg 292.2	–	[49]
	LiMn₂O₄/C	Li 28.6 Mg 4166	1.2 V	15.1	0.13	83.4% after 20 cycles	Li/Mg 770.1	–	[49]
	GRO/NCM622	Li 23.5 Na 256.4 K 47.8, Ca 0.6 Mg 120.8	1.11 C	13.8	–	80.8% after 15 cycles	93.4%	1.4	[95]
	H_1.6Mn_1.6O₄@PVA@PANI	Li 38.6 Na 695.3 K 60.3 Ca 0.6 Mg 31.7 ^**	1.0 V	16.7	–	–	Li/Na 109.5 Li/K 14.8 Li/Ca 7.71 Li/Mg 6.9	–	[130]
	H_1.6Mn_1.6O₄@PVA@PANI	Li 53.5 Na 2126.7 K 268.9 Ca 3.5 Mg 306.3 ^**	1.0 V	22.8	–	–	Li/Na 214.2 Li/K 45.0 Li/Ca 25.8 Li/Mg 43.5	–	[130]
3D structure fabrication	LiMn₂O₄/GO	Li 36, Na 4452 K 217, Mg 64 Ca 4.9	15 mA g⁻¹	5.0	–	80% after 150 cycles ^***	Li/Na 557.4 Li/K 219.5 Li/Ca 37.8 Li/Mg 72.8	–	[136]
	pyrazine-linked two-dimensional@ LiMn₂O₄	Li 17.9 Na 187 K 63.3, Ca 4.5 Mg 3.2	59.2 mA g⁻¹	25.1	2.51	92.5% after 20 cycles ^***	~92%	0.39	[137]
	Mesoporous LiMn₂O₄/3D graphite	Li 21.6 Na 43.5 K 25.6 Mg 41.2	3 V	12.5	1.25	90.4% after 20 cycles ^***	Li/Na 330.5 Li/k 296.9 Li/Mg 45.6	23.38	[151]
	LiMn₂O₄/carbon cloth	Li 20, Mg 400		5.9	–	97.4% after 10 cycles ^***	–	–	[152]
	MXene/LiMn₂O₄	Li 21.6 Na 330.6 K 47.3, Ca 0.8 Mg 39.5	–	–	–	94.3% after 30 cycles ^***	Li/Na 1020 Li/K 293 Li/Ca 151 Li/Mg 271	2.2	[201]
	LiFePO₄/CNT	Li 3.7, Na 29.7 K 3.5, Ca 5.3	0.8 V	14.9	0.1	~100% after 5 cycles	-	–	[202]
	LiFePO₄/biochar	Li 60.4 Mg 1325.5	–	32.1	–	82.3% after 5 cycles	Li/Mg ~180	–	[203]
	LiFePO₄/biochar	Li 203.1 Na 224.3 K 66.5 Mg 3891.4	–	26.2	–	87.9% after 5 cycles	Li/Mg ~920	–	[203]
	LiFePO₄/RGO	Li 95.6 Na 1196.9 K 519.2 Ca 21.7 Mg 2893.7	0.8 V	32.8	3.28	–	Li/Na 586.8 Li/K 573.8 Li/Mg 2240	–	[204]
	LiFePO₄/MF	Li 95.6 Na 1196.9 K 519.2 Ca 21.7 Mg 2893.7 ^**	–	27.9	–	82.1% after 5 cycles		–	[205]
	λ-MnO₂/RGO	Li 23.5 Na 256.4 K 47.8, Ca 0.6 Mg 120.8	15 mA g⁻¹	1.4	–	75% 30 cycles	Li/Na 38 Li/K 57 Li/Ca 8 Li/Mg 41	–	[206]
	λ-MnO₂/ppy/pss	Li 4.3, Na 4.3	0.2 V	35.2	0.29	98.9 after 5 cycles	Li/Na 46	–	[207]
Doping	Li_1−xNi_0.5Mn_1.5O₄	Li 234.8 Na 2566 K 478.3 Ca 5.7 Mg 1208.3	82 mA g⁻¹	10.5	0.35	–	98.0%	3.5	[94]
	Li₃V_1.85Fe_0.15(PO₄Cl_0.15)₃	Li 38.3 Na 1097.0 K 94.3 Ca 5.7 Mg 134.4 ^**	1.2 V	9.4	–	~80% after 100 cycles ***	Li/Na 167.8 Li/K 172.1 Li/Ca 4.1 Li/Mg 56.7	–	[110]
	LiAl_0.05Mn_1.95O₄	Li 42.9 Na 4452.2 K 217.9 Ca 5.0 Mg 669.6	–	–	–	84% after 100 cycles ^***	Li/Na 1653.8 Li/Mg 434.9	2.6	[138]
	LiCr_0.2Mn_1.8O₄	Li 45.7 Na 1923.5 K 66.9, Mg 7.8	1.1 V	15	0.13	86.1% after 500 cycles	–	2.16	[139]
	H_1.6Mn_1.6O₄-B_x	Li 34.5 Na 4384.5 K 399.5 Ca 88.5 Mg 628.5	1.2 V	26.5	0.44	95.6% after 10 cycles	Li/Na 1211.7 Li/K 1291.9 Li/Ca 782.6 Li/Mg 1352.0	–	[147]
	Li_1−xNi_0.025Co_0.025Mn_1.95O₄	Li 23.5 ^** Na 256.4 K 47.8, Ca 0.6 Mg 120.8	0.75 mA	–	–	97.9% after 50 cycles ^***	94.6%	2.12	[162]
	LiNi_0.03Mo_0.01Mn_1.96O₄	Li 23.5 Na 256.4 K 47.8, Ca 0.6 Mg 120.8	0.5 mA cm⁻²	14.4	0.58	97.6% 5 cycles	97.2%	7.91	[208]
	GO/LiLa_0.05Mn_1.95O₄	Li 234.8 Na 2566.4 K 478.3 Ca 5.7 Mg 1208.3	1 V	8.3	–	83.3% after 1000 cycles ^***	Li/Na 365 Li/K 298 Li/Ca 48 Li/Mg 115	–	[209]
	LiCo_0.025V_0.025Mn_1.95O₄	Li 100, Na 100 K 100, Ca 100 Mg 100	–	18.8	0.36	–	–	8.51	[210]
	LiBi_0.3Mn_1.7O₄	Li 55, Na 3424 K 490, Mg 3.1	50	26.2	–	–	Li/Na 111 Li/K 28 Li/Mg 0.7	2.09	[211]
Surface modification	C@LiFePO₄	Li 5, Na 50	30 mA g⁻¹	21	–	82% after 10 cycles	–	3.0	[25]
	C@Li₃V₂(PO₄)₃	Li 42.1 Na 912.9 K 75.8, Ca 5.4 Mg 109.7 ^**	1.2 V	11.7	–	78% after 50 cycles ^***	Li/Na 116.88 Li/K 136.1 Li/Ca 4.92 Li/Mg 187.5	–	[105]
	AlPO₄@LiMn₂O₄	Li 30.7 Na 31.0 K 31.2 Ca 32.0 Mg 33.0	50 mA g⁻¹	30.2	0.50	93.6% after 20 cycles ^***	91%	5.19	[140]
	CeO₂@LiMn₂O₄	Li 30, Na 30 K 30, Ca 30 Mg 30	–	12.6	0.21	60% after 30 cycles ^***	99%	–	[141]
	PAA-CePO₄@LiMn₂O₄	Li 55 Na 3424.1 K 489.7 Mg 3.1 ^**	50 mA g⁻¹	24.7	0.41	78.5% after 15 cycles	64.8%	–	[142]
	CePO₄@LiMn₂O₄	Li 27.6 Na 27.8 K 29.3 Ca 26.1 Mg 30.9		32.72	0.55	66.7% after 5 cycles	95.02%	–	[142]
	NiFe₂O₄@LiMn₂O₄	Li 87.9, Na 2608.7 K 461.5, Ca 0.04 Mg 2.3	~50 mA g⁻¹	18.8	–	–	Li/Na 8.9	–	[143]
	Li_1.5Al_0.5Ge_1.5(PO₄)₃@ LiMn₂O₄	Li 30.1, Na 30.3 K 31.15, Ca 30.7 Mg 30.7	50 mA g⁻¹	17.1	–	–	Li/Mg 95 Li/Na 119	1.47	[212]
	AlF₃@LiMn₂O₄	Li 50, Mg 50	1.2 V	28.1	–	–	Li/Mg 3.67	–	[213]
	ZnO@LiMn₂O₄	Li 30, Na 30 K 30, Ca 30 Mg 30	1.2 V	13.3	0.17	–	99.3%	–	[214]
	In₂O₃@LiMn₂O₄	Li 76.3, Na 1101 K 0.06, Ca 1.11 Mg 0.18	–	21.3	0.36	–	75.46% Li/Na 21.1	–	[215]
Structure regulation	Truncated octahedral LiNi_0.05Mn_1.95O₄	Li 18, Na 5817.5 K 90.7, Ca 14 Mg 253.7 ^**	50 mA g⁻¹	21	–	~100% after 5 cycles	Li/Na 1166 Li/K 20.4 Li/Ca 37.7 Li/Mg 214.1	–	[27]
	Li_0.3FePO₄/C	Li 71.4, Na 4000.0	–	~25	–	> 90% after 100 cycles	Li/Na 138	–	[132]
	Truncated octahedral LiMn₂O₄	Li 30, Na 30 K 30, Ca 30 Mg 30	50 mA g⁻¹	20.25	0.17	~100% after 50 cycles	–	12.28	[155]
Structure regulation	λ-Li_1.5MnO₂	Li 6.0 Na 4146.4 K 259.0 Ca 1.4 Mg 1225.1 Cu 5.1 10⁻⁴ Fe 1.2 10⁻² Ni 1.1 10⁻³ ^**	1.2 V	30.1	–	80% after 100 cycles ^***	Li/Na 6.8 Li/K 4.2 Li/Ca 2.5 Li/Mg 2.0 Li/Cu 5.5 Li/Fe 8.3 Li/Ni 2.2	–	[216]
	LFP (010)	Li 35.4, Na 671.5 K 60.6, Mg 27.9 ^**	1.0 V	5.88	0.01	–	Li/Na 12.01 Li/K 10.05 Li/Mg 2.37	–	[217]
	Layer gradient (NaLi)_1−xCoO₂	Li 1.0, Na 1000.0	82.8 mA g⁻¹	–	–	–	Li/Na 13000	–	[218]

表2

图11

图12

图13

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	LiFePO₄	LiMn₂O₄	Li_1.6Mn_1.6O₄	NCM	Li₃V₂(PO₄)₃
Electrical conductivity	Low	High	High	High	Medium
Ionic conductivity	Low	High	High	High	High
Capacity	Medium	Medium	High	High	Low
Stability	High	Medium	Medium	Low	Low
Cost	Low	Low	Low	High	Medium
Commercialization **	Industrial	Industrial	Lab	Industrial	Lab

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