Acta Phys. -Chim. Sin. ›› 2026, Vol. 42 ›› Issue (1): 100127.doi: 10.1016/j.actphy.2025.100127
Special Issue: Electrochemical Separation and Recycling
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Electrochemical lithium extraction by the faradaic materials: advances, challenges and enhancement approaches
Lei Wang1,2,*(
), Panpan Zhang1,2, Zhiyuan Guo1,2, Jing Wang1,2, Jie Ma3,*(), Zhi-yong Ji1,2,*()
- 1 Engineering Research Center of Seawater Utilization of Ministry of Education, School of Chemical Engineering and Technology, Hebei University of Technology, Tianjin 300401, China
2 Hebei Collaborative Innovation Center of Modern Marine Chemical Technology, Tianjin 300401, China
3 Research Center for Environmental Functional Materials, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, China
-
Received:2025-04-29Revised:2025-06-11Accepted:2025-06-30Published:2025-11-01 -
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Cite this article
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
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Fig 1
(A) The operation process of electrochemical lithium extraction with faradaic materials. (B) The schematic image of cation and electron transport during the electrochemical process with the pure electrolyte. (C) The schematic image of cation distribution in the EDL with multi-cation electrolyte."
Fig 1
Fig 2
(A) Crystal structure of LiFePO4. (B) The lithium diffusion path along the [010] direction. Panels (A) and (B) are reproduced with permission [53], Copyright 2008, Springer Nature. (C) Species distributions of Fe2+ and Fe3+ at different pH, reproduced with permission [60], Copyright 2013, American Chemical Society (D) The relationship between the slop of Gibbs free energy (i.e., the chemical potential of interstitial Li and the voltage curve, reproduced with permission [64], Copyright 2024, Elsevier. (E) The CV cure of LiFePO4 measured in various pure electrolytes with the concentration of 1 mol L−1, (F) the calculated migration energy barriers of cations in discharged LiFePO4. Panels (E) and (F) are produced with permission [47], Copyright 2022, National Academy of Sciences."
Fig 2
Fig 3
(A) The crystal structure of LiMn2O4 and lithium diffusion path in LiMn2O4, reproduced with permission [74], copyright 2013, Elsevier; (B) the molecular orbital energy diagram of the octahedral MnO6 and the electronic orbitals of Mn2+/Mn3+/Mn4+ ions, reprinted from Ref. [79] with permission, Copyright 2024, Elsevier; (C) the XRD patterns of LiMn2O4 at different potential vs. Li/Li+, reproduced with permission [84], copyright 2019 Springer Nature. (D) calculated species distribution of Mn3+ and Mn2+ at various pH, reproduced with permission [85], copyright 2024, Elsevier; (E) the CV curve of LiMn2O4 in various electrolytes with different cations, reproduced with permission [33], copyright 2024, American Chemical Society; (F) the calculated intercalation potential of multiple cations in LiMn2O4; (G) Gibbs energy change of the intercalation of different ions in LiMn2O4 structure, Panels (F) and (G) are reproduced with permission [86], copyright 2020, American Chemical Society."
Fig 3
Fig 4
(A) The relationship between the layered, disordered rocksalt and spinel structure of transition metal oxides, reproduced with permission [87], copyright 2017, John Wiley & Sons; (B) the possible lithium diffusion path, tetrahedral-site pathway (the upper) and oxygen dumbbell pathway (the bottom) in NCM, reproduced with permission [43], copyright 2016, John Wiley & Sons; (C) the phase transformation of Li[Ni0.95Co0.025Mn0.025]O2 (Ⅰ), Li[Ni0.9Co0.05Mn0.05]O2 (Ⅱ), Li[Ni0.8Co0.1Mn0.1]O2 (Ⅲ), Li[Ni0.6Co0.2Mn0.2]O2 (Ⅳ) during charging and discharging process, reproduced with permission [92], copyright 2018, American Chemical Society; (D) the cell volume change of NCM with various composition at different voltage, reproduced with permission [93], copyright 2018, American Chemical Society; (E) the CV curve of NCM111 in pure Li+ electrolyte and mixed solution with/without Li+, reproduced with permission [96], copyright 2018, Elsevier."
Fig 4
Fig 5
(A) The schematic image of rhombohedral (left) and monoclinic (right) Li3V2(PO4)3, reproduced with permission [104], copyright 2014, Elsevier; (B) The CV curve of monoclinic Li3V2(PO4)3 in various electrolyte; (C) Energy variations of the migration of Li and Mg in V2PO4, panels (B) and (C) are reproduced with permission [105], copyright 2024, Elsevier; (D) The ion exchange mechanism between H+ and Li+ in Li1.33Mn1.67O4 and Li1.6Mn1.6O4, reproduced with permission [106], copyright 2019, Royal Society of Chemistry."
Fig 5
Table 1
The comparison of theoretical performance among LiFePO4, LiMn2O4, Li1.6Mn1.6O4, NCM and Li3V2(PO4)3 *."
| LiFePO4 | LiMn2O4 | Li1.6Mn1.6O4 | 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 |
Table 1
Fig 6
The lithium extraction of pure electrode materials in literature: (A) lithium extraction capacity, (B) lithium extraction rate, (C) lithium extraction capacity retention, (D) Energy consumption, (E) selectivity factor between Li and Na, (F) selectivity factor between Li and Mg. The color bars in planes (A)–(D) represent the molar ratio of Li in the feed water, and the color bars in planes (E) and (F) indicate the lithium concentration (mmol L−1). The symbols without fills represent pure Li+ electrolytes. The number in Panel (C) represents the cycle numbers, and the insert image displays the capacity loss per cycle of materials versus cycle numbers. The data is from Ref. [24–26,31,50,72,77,86,96,110,116,126–147]."
Fig 6
Fig 7
(A) The preparation schematic diagram (Ⅰ), 3D Ultra-deep field microscopic images (Ⅱ, Ⅳ) and SEM images (Ⅲ) of multiple-crack-porous LiFePO4 electrode, reproduced with permission [48], copyright 2023, Elsevier; (B) the illustration (Ⅰ) of binder-free 3D LiMn2O4 electrode and its SEM images (Ⅱ, Ⅲ), reproduced with permission [152], copyright 2024, John Wiley & Sons; (C) the preparation process (Ⅰ), SEM images (Ⅱ, Ⅲ) and the comparison of lithium concentration distribution in the electrode with disordered channels (Ⅳ) and vertically aligned channels (Ⅴ), reproduced with permission [153], copyright 2025, American Chemical Society."
Fig 7
Fig 8
(A) schematic diagram of oriented LiFePO4, Wulff shape of LiFePO4 and binding geometries of adsorbed ethylene and diethylene glycol; (B) the SEM image of [010] oriented LiFePO4, Panels A and B are reproduced with permission [157], copyright 2014, American Chemical Society; (C) the lithium diffusion rate of various NCM with different lithium content, reproduced with permission [43], copyright 2015, John Wiley & Sons; (D) the interlayer spacing of various NCM with different lithium content, reproduced with permission [87], copyright 2017, John Wiley & Sons."
Fig 8
Fig 9
(A) The calculated surface oxygen releasing energy of LiMn2O4 with different doping elements, reproduced with permission [165], copyright 2022, American Chemical Society; (B) the effect of different doping elements on the electrochemical performance and crystal structure of NCM, reproduced with permission [166], copyright 2022, Elsevier."
Fig 9
Fig 10
(A) The schematic image of the dry coating method; (B) the schematic illustration of the wet chemical method in which (Ⅰ) and (Ⅱ) refer to the sol-gel method and hydrothermal method respectively; (C) the schematic of general elementary steps of (Ⅰ) CVD and (Ⅱ) ALD process, Panel (Ⅰ) is reprinted with permission [197], copyright 2021, Springer Nature and Panel (Ⅱ) is reproduced with permission [198], copyright 2014, Elsevier."
Fig 10
Table 2
The summary of lithium extraction performance of faradaic materials modified by various methods *."
| Modification method | Material | c (mmol L−1) ** | V/I | Qintercalation (mg g−1) | rLi-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 | – | [ |
| 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 | – | [ | |
| 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 | – | [ | |
| Li 28.6 Mg 4166 | 1.2 V | 15.1 | 0.13 | 83.4% after 20 cycles | Li/Mg 770.1 | – | |||
| 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 | [ | |
| H1.6Mn1.6O4@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 | – | [ | |
| 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 | – | |||
| 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 | – | [ |
| 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 | [ | |
| 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 | [ | |
| LiMn2O4/carbon cloth | Li 20, Mg 400 | 5.9 | – | 97.4% after 10 cycles *** | – | – | [ | ||
| 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 | [ | |
| 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 | - | – | [ | |
| LiFePO4/biochar | Li 60.4 Mg 1325.5 | – | 32.1 | – | 82.3% after 5 cycles | Li/Mg ~180 | – | [ | |
| Li 203.1 Na 224.3 K 66.5 Mg 3891.4 | – | 26.2 | – | 87.9% after 5 cycles | Li/Mg ~920 | – | |||
| 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 | – | [ | |
| LiFePO4/MF | Li 95.6 Na 1196.9 K 519.2 Ca 21.7 Mg 2893.7 ** | – | 27.9 | – | 82.1% after 5 cycles | – | [ | ||
| 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 | – | [ | |
| 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 | – | [ | |
| Doping | Li1−xNi0.5Mn1.5O4 | 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 | [ |
| Li3V1.85Fe0.15(PO4Cl0.15)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 | – | [ | |
| LiAl0.05Mn1.95O4 | 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 | [ | |
| LiCr0.2Mn1.8O4 | 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 | [ | |
| H1.6Mn1.6O4-Bx | 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 | – | [ | |
| Li1−xNi0.025Co0.025Mn1.95O4 | 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 | [ | |
| LiNi0.03Mo0.01Mn1.96O4 | 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 | [ | |
| GO/LiLa0.05Mn1.95O4 | 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 | – | [ | |
| LiCo0.025V0.025Mn1.95O4 | Li 100, Na 100 K 100, Ca 100 Mg 100 | – | 18.8 | 0.36 | – | – | 8.51 | [ | |
| LiBi0.3Mn1.7O4 | Li 55, Na 3424 K 490, Mg 3.1 | 50 | 26.2 | – | – | Li/Na 111 Li/K 28 Li/Mg 0.7 | 2.09 | [ | |
| Surface modification | C@LiFePO4 | Li 5, Na 50 | 30 mA g−1 | 21 | – | 82% after 10 cycles | – | 3.0 | [ |
| 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 | – | [ | |
| 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 | [ | |
| CeO2@LiMn2O4 | Li 30, Na 30 K 30, Ca 30 Mg 30 | – | 12.6 | 0.21 | 60% after 30 cycles *** | 99% | – | [ | |
| 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% | – | [ | |
| 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% | – | [ | ||
| 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 | – | [ | |
| Li1.5Al0.5Ge1.5(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 | [ | |
| AlF3@LiMn2O4 | Li 50, Mg 50 | 1.2 V | 28.1 | – | – | Li/Mg 3.67 | – | [ | |
| ZnO@LiMn2O4 | Li 30, Na 30 K 30, Ca 30 Mg 30 | 1.2 V | 13.3 | 0.17 | – | 99.3% | – | [ | |
| 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 | – | [ | |
| Structure regulation | Truncated octahedral LiNi0.05Mn1.95O4 | 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 | – | [ |
| Li0.3FePO4/C | Li 71.4, Na 4000.0 | – | ~25 | – | > 90% after 100 cycles | Li/Na 138 | – | [ | |
| 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 | [ | |
| Structure regulation | λ-Li1.5MnO2 | 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 | – | [ |
| 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 | – | [ | |
| Layer gradient (NaLi)1−xCoO2 | Li 1.0, Na 1000.0 | 82.8 mA g−1 | – | – | – | Li/Na 13000 | – | [ |
Table 2
Fig 11
(A) The schematic image of flow-by mode and flow-through mode; (B) (Ⅰ) the schematic illustration of the self-driven process and the comparison between the self-driven process and common process regarding lithium extraction capacity (Ⅱ) and energy consumption (Ⅲ), reproduced with permission [129], copyright 2020, Elsevier; (C) (Ⅰ) the schematic illustration of the pulsed current charging/discharging approach, and the capacity (Ⅱ) and lithium purity (Ⅲ) of the constant current method and pulsed method, reproduced with permission [33], copyright 2024, American Chemical Society."
Fig 11
Fig 12
(A) The HR-TEM and selected area electron diffraction of LMO (upper) and LMO-Pyr-2D electrodes (bottom) after 15 cycles, reproduced with permission [137], copyright 2023, Elsevier; (B) The temperature evolution curves of the electrolyte under 1 sun simulated sunlight and the temperature distribution of FP@PPy electrode at saturated temperature (upper) and the lithium extraction capacity and extraction rate on different conditions (bottom), reproduced with permission [229], copyright 2024, Elsevier."
Fig 12
Fig 13
(A) The TRL level of Li3V2(PO4)3, NCM, Li1.6Mn1.6O4, LiFePO4, and LiMn2O4, TRL4 stands for using salt solution or simulated brine with 1 to 2 co-existing ions and systems show good stability, TRL5 is utilizing simulated brine with several co-existing ions and systems show moderate to high stability; TRL6 represents system which is tested with simulated brine comprising of several co-existing ions and show high stability; TRL7 is operated in operational environmental. The evaluation criteria are according to ref. [19]; (B) The optical photo of piloted-scale devices with λ-MnO2 and Ag as electrodes, reproduced with permission [230], copyright 2020, Royal Society of Chemistry; (C) the schematic image of decoupled membrane-free lithium extraction cell; (D) the illustration of piloted-scale decoupled membrane-free lithium extraction system, Panels (C) and (D) are reproduced with permission [144], copyright 2024, American Association for the Advancement of Science."
Fig 13
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