Screen-Printed Li Arrays with Reinforced Interphase as Ultrathin Anodes for High-Energy–Density Liquid- and Solid-State Batteries
Corresponding Author: Wei Wu
Nano-Micro Letters,
Vol. 19 (2027), Article Number: 37
Abstract
High-energy–density lithium metal batteries, either liquid or solid state, require ultrathin Li anodes, but their implementation is hindered by poor Li processability in fabrication and inhomogeneous Li plating behaviours upon cycling. This work addresses these challenges through a mask-patterned discrete array using a molten salt-derived Li nanocomposite. The screen-printing strategy circumvents the poor wettability of molten Li on copper that causes high Li|Cu contact angle and non-uniform Li spreading, thus fabricating ultrathin Li foils with equivalent thicknesses below 30 μm. Concurrently, the molten salt-derived inorganic nanoparticles in Li favour homogeneous Li deposition and induce inorganic-rich solid electrolyte interphase to jointly suppress active Li consumption. The resulting Li array (10–28 μm) anodes demonstrate remarkable performance in both liquid- and solid-state systems, achieving high energy densities up to 504 Wh kg−1/1071 Wh L−1 and stable cycling over 260 cycles with high-loading cathodes. This integrated approach resolves both fabrication and cycling challenges of ultrathin Li anodes and offers an alternative solution for high-performance liquid-/solid-state batteries.
Highlights:
1 A screen-printing strategy using mask-patterned discrete arrays overcomes molten Li’s poor wettability on Cu, enabling fabrication of ultrathin Li anodes (< 30 μm).
2 In situ generated inorganic nanoparticles from Mg(TFSI)2 homogenize Li deposition and induce an inorganic-rich solid electrolyte interphases, significantly suppressing active Li consumption.
3 The Li@Mg(TFSI)2 array anode fits both liquid- and solid-state full cells, achieving high energy densities of 504 Wh kg−1/1071 Wh L−1 and stable cycling over 260 cycles.
Keywords
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References
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M.H. Kim, T.U. Wi, J. Seo, A. Choi, S. Ko et al., Design principles for fluorinated interphase evolution via conversion-type alloying processes for anticorrosive lithium metal anodes. Nano Lett. 23(8), 3582–3591 (2023). https://doi.org/10.1021/acs.nanolett.3c00764
Z. Li, L. Wang, X. Huang, X. He, Lithium bis(trifluoromethanesulfonyl)imide (LiTFSI): a prominent lithium salt in lithium-ion battery electrolytes–fundamentals, progress, and future perspectives. Adv. Funct. Mater. 34(48), 2408319 (2024). https://doi.org/10.1002/adfm.202408319
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H. Liu, Y. Ji, Y. Li, S. Zheng, Z. Dong et al., Regulating lithium affinity of hosts for reversible lithium metal batteries. Interdiscip. Mater. 3(2), 297–305 (2024). https://doi.org/10.1002/idm2.12153
Q. Wang, C. Zhao, S. Wang et al., Interphase design for lithium-metal anodes. J. Am. Chem. Soc. 147(11), 9365–9377 (2025). https://doi.org/10.1021/jacs.4c15759
X.-X. Ma, X. Shen, X. Chen, Z.-H. Fu, N. Yao et al., The origin of fast lithium-ion transport in the inorganic solid electrolyte interphase on lithium metal anodes. Small Struct. 3(8), 2200071 (2022). https://doi.org/10.1002/sstr.202200071
J. Oh, S.H. Choi, J.Y. Kim, J. Lee, T. Lee et al., Anode-less all-solid-state batteries operating at room temperature and low pressure. Adv. Energy Mater. 13(38), 2301508 (2023). https://doi.org/10.1002/aenm.202301508
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B. Li, W. Zhang, K. Yang, L. Li, J. Luo et al., Bridging atomic and macroscopic perspectives on heteroepitaxial growth in lithium metal anodes. ACS Energy Lett. 9(10), 5215–5224 (2024). https://doi.org/10.1021/acsenergylett.4c02403
P. Zou, Y. Sui, H. Zhan, C. Wang, H.L. Xin et al., Polymorph evolution mechanisms and regulation strategies of lithium metal anode under multiphysical fields. Chem. Rev. 121(10), 5986–6056 (2021). https://doi.org/10.1021/acs.chemrev.0c01100
J. Gu, Y. Shi, Z. Du, M. Li, S. Yang, Stress relief in metal anodes: mechanisms and applications. Adv. Energy Mater. 13(40), 2302091 (2023). https://doi.org/10.1002/aenm.202302091
X. Hu, Z. Zhang, X. Zhang, Y. Wang, X. Yang et al., External-pressure–electrochemistry coupling in solid-state lithium metal batteries. Nat. Rev. Mater. 9(5), 305–320 (2024). https://doi.org/10.1038/s41578-024-00669-y
Y. Hu, H. Li, Z. Chen, W. Cen, Q. Wang et al., Li-alloy texture creates in-built Li(110) epitaxy in a thin Li-metal anode allowing high depth-of-discharge cycling in carbonate electrolyte. Chem. Eng. J. 466, 143084 (2023). https://doi.org/10.1016/j.cej.2023.143084
G. Zhang, T. Zhang, Y. Liu, Q. Wang, R. He et al., Molecular design of asymmetric difluorinated ether electrolytes for stable operation of high-voltage lithium metal batteries. Angew. Chem. Int. Ed. 64(38), e202506056 (2025). https://doi.org/10.1002/anie.202506056
J. Xing, T. Chen, L. Yi, Z. Wang, Z. Song et al., Endowing Cu foil self-wettable in molten lithium: a roll-to-roll wet coating strategy to fabricate high-performance ultrathin lithium metal anodes. Energy Storage Mater. 63, 103067 (2023). https://doi.org/10.1016/j.ensm.2023.103067
Y. Zhao, T. Zhou, L.P.H. Jeurgens, X. Kong, J.W. Choi et al., Electrolyte engineering for highly inorganic solid electrolyte interphase in high-performance lithium metal batteries. Chem 9(3), 682–697 (2023). https://doi.org/10.1016/j.chempr.2022.12.005
L. Deng, Y. Liu, H. Qi, Y. Yang, Z. Wang et al., A nanoengineered lithium-hosting carbon/zinc oxide composite electrode material for efficient non-aqueous lithium metal batteries. Nat. Nanotechnol. 20(10), 1439–1448 (2025). https://doi.org/10.1038/s41565-025-01983-4
J. Gao, C. Chen, Q. Dong, J. Dai, Y. Yao et al., Stamping flexible Li alloy anodes. Adv. Mater. 33(11), 2005305 (2021). https://doi.org/10.1002/adma.202005305
L. Fu, X. Wang, B. Zhang, Z. Chen, Y. Li et al., A Li3P nanop dispersion strengthened ultrathin Li metal electrode for high energy density rechargeable batteries. Nano Res. 17(5), 4031–4038 (2024). https://doi.org/10.1007/s12274-023-6275-9
S. Huang, Z. Wu, B. Johannessen, K. Long, P. Qing et al., Interfacial friction enabling ≤ 20 μm thin free-standing lithium strips for lithium metal batteries. Nat. Commun. 14(1), 5678 (2023). https://doi.org/10.1038/s41467-023-41514-0
H. Kwon, H.J. Choi, J.K. Jang, J. Lee, J. Jung et al., Weakly coordinated Li ion in single-ion-conductor-based composite enabling low electrolyte content Li-metal batteries. Nat. Commun. 14(1), 4047 (2023). https://doi.org/10.1038/s41467-023-39673-1
Y. Meng, D. Zhou, R. Liu, Y. Tian, Y. Gao et al., Designing phosphazene-derivative electrolyte matrices to enable high-voltage lithium metal batteries for extreme working conditions. Nat. Energy 8(9), 1023–1033 (2023). https://doi.org/10.1038/s41560-023-01339-z
G. Zhang, J. Chang, L. Wang, J. Li, C. Wang et al., A monofluoride ether-based electrolyte solution for fast-charging and low-temperature non-aqueous lithium metal batteries. Nat. Commun. 14(1), 1081 (2023). https://doi.org/10.1038/s41467-023-36793-6
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