Issue

Vol. 17 (2025)

Developing High-Energy, Stable All-Solid-State Lithium Batteries Using Aluminum-Based Anodes and High-Nickel Cathodes

https://doi.org/10.1007/s40820-025-01751-y
Xin Wu
Center of Energy Storage Materials & Technology, Department of Energy Science and Engineering, College of Engineering and Applied Sciences, Jiangsu Key Laboratory of Artificial Functional Materials, National Laboratory of Solid‑State Microstructures, and Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing 210093, People’s Republic of China
Meiyu Wang
Department of Materials Science and Engineering, College of Engineering and Applied Sciences, Jiangsu Key Laboratory of Artificial Functional Materials, National Laboratory of Solid‑State Microstructures, and Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing 210093, People’s Republic of China
Hui Pan
Center of Energy Storage Materials & Technology, Department of Energy Science and Engineering, College of Engineering and Applied Sciences, Jiangsu Key Laboratory of Artificial Functional Materials, National Laboratory of Solid‑State Microstructures, and Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing 210093, People’s Republic of China
Xinyi Sun
Center of Energy Storage Materials & Technology, Department of Energy Science and Engineering, College of Engineering and Applied Sciences, Jiangsu Key Laboratory of Artificial Functional Materials, National Laboratory of Solid‑State Microstructures, and Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing 210093, People’s Republic of China
Shaochun Tang
Department of Materials Science and Engineering, College of Engineering and Applied Sciences, Jiangsu Key Laboratory of Artificial Functional Materials, National Laboratory of Solid‑State Microstructures, and Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing 210093, People’s Republic of China
Haoshen Zhou
Center of Energy Storage Materials & Technology, Department of Energy Science and Engineering, College of Engineering and Applied Sciences, Jiangsu Key Laboratory of Artificial Functional Materials, National Laboratory of Solid‑State Microstructures, and Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing 210093, People’s Republic of China
Ping He
Center of Energy Storage Materials & Technology, Department of Energy Science and Engineering, College of Engineering and Applied Sciences, Jiangsu Key Laboratory of Artificial Functional Materials, National Laboratory of Solid‑State Microstructures, and Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing 210093, People’s Republic of China

Corresponding Author: Ping He

pinghe@nju.edu.cn

Nano-Micro Letters, Vol. 17 (2025), Article Number: 239

Abstract

Aluminum (Al) exhibits excellent electrical conductivity, mechanical ductility, and good chemical compatibility with high-ionic-conductivity electrolytes. This makes it more suitable as an anode material for all-solid-state lithium batteries (ASSLBs) compared to the overly reactive metallic lithium anode and the mechanically weak silicon anode. This study finds that the pre-lithiated Al anode demonstrates outstanding interfacial stability with the Li6PS5Cl (LPSCl) electrolyte, maintaining stable cycling for over 1200 h under conditions of deep charge–discharge. This paper combines the pre-lithiated Al anode with a high-nickel cathode, LiNi0.8Co0.1Mn0.1O2, paired with the highly ionic conductive LPSCl electrolyte, to design an ASSLB with high energy density and stability. Using anode pre-lithiation techniques, along with dual-reinforcement technology between the electrolyte and the cathode active material, the ASSLB achieves stable cycling for 1000 cycles at a 0.2C rate, with a capacity retention rate of up to 82.2%. At a critical negative-to-positive ratio of 1.1, the battery’s specific energy reaches up to 375 Wh kg−1, and it maintains over 85.9% of its capacity after 100 charge–discharge cycles. This work provides a new approach and an excellent solution for developing low-cost, high-stability all-solid-state batteries.


Highlights:
1 Anode pre-lithiation technique was employed to promote the reversibility of Al.
2 Dual-reinforcement technology was developed to address the interfacial incompatibility between the Ni-rich cathode active material and sulfide solid-state electrolyte.
3 The fabricated all-solid-state lithium battery comprising the pre-lithiated Al anode and dual-reinforced Ni-rich cathode achieves stable cycling for 1000 cycles with a capacity retention of 82.2%.

Keywords

All-solid-state lithium battery Ni-rich cathode Pre-lithiated Al anode High energy density Interface modification
Wu, Xin, Meiyu Wang, Hui Pan, Xinyi Sun, Shaochun Tang, Haoshen Zhou, and Ping He. 2025. “Developing High-Energy, Stable All-Solid-State Lithium Batteries Using Aluminum-Based Anodes and High-Nickel Cathodes”. Nano-Micro Letters 17 (April):239. https://doi.org/10.1007/s40820-025-01751-y.
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References
  1. X. Lu, Y. Wang, X. Xu, B. Yan, T. Wu et al., Polymer-based solid-state electrolytes for high-energy-density lithium-ion batteries–review. Adv. Energy Mater. 13(38), 2301746 (2023). https://doi.org/10.1002/aenm.202301746
  2. S. Jeong, Y. Li, W.H. Sim, J. Mun, J.K. Kim et al., Advances of sulfide-type solid-state batteries with negative electrodes: progress and perspectives. EcoMat 5(6), e12338 (2023). https://doi.org/10.1002/eom2.12338
  3. X. Xu, Y. Wang, Q. Yi, X. Wang, R.A.P. Camacho et al., Ion conduction in composite polymer electrolytes: potential electrolytes for sodium-ion batteries. ChemSusChem 16(8), e202202152 (2023). https://doi.org/10.1002/cssc.202202152
  4. H.H. Jia, C.J. Hu, Y.X. Zhang, L.W. Chen, A review on solid-state Li-S battery: from the conversion mechanism of sulfur to engineering design. J. Electrochem. 29, 2217008 (2023). https://doi.org/10.13208/j.electrochem.2217008
  5. B. Du, H. Zhou, P. He, Halide lithium conductors: from design and synthesis to application for all-solid-state batteries. ACS Appl. Energy Mater. 8(2), 723–745 (2025). https://doi.org/10.1021/acsaem.4c02948
  6. J.A. Lewis, F.J.Q. Cortes, Y. Liu, J.C. Miers, A. Verma et al., Linking void and interphase evolution to electrochemistry in solid-state batteries using operando X-ray tomography. Nat. Mater. 20(4), 503–510 (2021). https://doi.org/10.1038/s41563-020-00903-2
  7. J. Li, J. Luo, X. Li, Y. Fu, J. Zhu et al., Li metal anode interface in sulfide-based all-solid-state Li batteries. EcoMat 5(8), e12383 (2023). https://doi.org/10.1002/eom2.12383
  8. S. Liu, L. Zhou, J. Han, K. Wen, S. Guan et al., Super long-cycling all-solid-state battery with thin Li6PS5Cl-based electrolyte. Adv. Energy Mater. 12(25), 2200660 (2022). https://doi.org/10.1002/aenm.202200660
  9. X.L. Wang, R.J. Xiao, Y. Xiang, H. Li, L.Q. Chen, Density functional investigation on cathode/electrolyte interface in solid-state lithium batteries. J. Electrochem. 23, 381–390 (2017). https://doi.org/10.13208/j.electrochem.170142
  10. X. Li, F.E. Kersey-Bronec, J. Ke, J.E. Cloud, Y. Wang et al., Study of lithium silicide nanops as anode materials for advanced lithium ion batteries. ACS Appl. Mater. Interfaces 9(19), 16071–16080 (2017). https://doi.org/10.1021/acsami.6b16773
  11. D.H.S. Tan, Y.-T. Chen, H. Yang, W. Bao, B. Sreenarayanan et al., Carbon-free high-loading silicon anodes enabled by sulfide solid electrolytes. Science 373(6562), 1494–1499 (2021). https://doi.org/10.1126/science.abg7217
  12. Y. Liu, C. Wang, S.G. Yoon, S.Y. Han, J.A. Lewis et al., Aluminum foil negative electrodes with multiphase microstructure for all-solid-state Li-ion batteries. Nat. Commun. 14(1), 3975 (2023). https://doi.org/10.1038/s41467-023-39685-x
  13. H. Pan, M. Zhang, Z. Cheng, H. Jiang, J. Yang et al., Carbon-free and binder-free Li-Al alloy anode enabling an all-solid-state Li-S battery with high energy and stability. Sci. Adv. 8(15), eabn4372 (2022). https://doi.org/10.1126/sciadv.abn4372
  14. Y. Zhu, X. He, Y. Mo, Origin of outstanding stability in the lithium solid electrolyte materials: insights from thermodynamic analyses based on first-principles calculations. ACS Appl. Mater. Interfaces 7(42), 23685–23693 (2015). https://doi.org/10.1021/acsami.5b07517
  15. Y. Lu, C.-Z. Zhao, J.-Q. Huang, Q. Zhang, The timescale identification decoupling complicated kinetic processes in lithium batteries. Joule 6(6), 1172–1198 (2022). https://doi.org/10.1016/j.joule.2022.05.005
  16. Y. Jung, Y.Y. Song, Y.S. Kim, Y. Chung, D.H. Lee et al., Impact of conducting agents on sulfide and halide electrolytes in disordered rocksalt cathode-based all-solid-state batteries. EcoMat 6, e12502 (2024). https://doi.org/10.1002/eom2.12502
  17. X. Li, Z. Ren, M. Norouzi Banis, S. Deng, Y. Zhao et al., Unravelling the chemistry and microstructure evolution of a cathodic interface in sulfide-based all-solid-state Li-ion batteries. ACS Energy Lett. 4(10), 2480–24 (2019). https://doi.org/10.1021/acsenergylett.9b01676
  18. X. Li, L. Jin, D. Song, H. Zhang, X. Shi et al., LiNbO3-coated LiNi0.8Co0.1Mn0.1O2 cathode with high discharge capacity and rate performance for all-solid-state lithium battery. J. Energy Chem. 40, 39–45 (2020). https://doi.org/10.1016/j.jechem.2019.02.006
  19. J.Y. Lee, S. Noh, J.Y. Seong, S. Lee, Y.J. Park, Suppressing unfavorable interfacial reactions using polyanionic oxides as efficient buffer layers: low-cost Li3PO4 coatings for sulfide-electrolyte-based all-solid-state batteries. ACS Appl. Mater. Interfaces 15(10), 12998–13011 (2023). https://doi.org/10.1021/acsami.2c21511
  20. Q. Zhang, A.M. Bruck, A.M. Stavola, W. Liang, P. Aurora et al., Enhanced electrochemical stability of sulfide-based LiNi0.8Mn0.1Co0.1O2 all-solid-state batteries by Ti surface doping. Batter. Supercaps 4(3), 529–535 (2021). https://doi.org/10.1002/batt.202000213
  21. T.-T. Zuo, F. Walther, S. Ahmed, R. Rueß, J. Hertle et al., Formation of an artificial cathode–electrolyte interphase to suppress interfacial degradation of Ni-rich cathode active material with sulfide electrolytes for solid-state batteries. ACS Energy Lett. 8(3), 1322–1329 (2023). https://doi.org/10.1021/acsenergylett.2c02835
  22. S. Deng, X. Li, Z. Ren, W. Li, J. Luo et al., Dual-functional interfaces for highly stable Ni-rich layered cathodes in sulfide all-solid-state batteries. Energy Storage Mater. 27, 117–123 (2020). https://doi.org/10.1016/j.ensm.2020.01.009
  23. X. Li, Q. Sun, Z. Wang, D. Song, H. Zhang et al., Outstanding electrochemical performances of the all-solid-state lithium battery using Ni-rich layered oxide cathode and sulfide electrolyte. J. Power Sources 456, 227997 (2020). https://doi.org/10.1016/j.jpowsour.2020.227997
  24. X. Liu, J. Shi, B. Zheng, Z. Chen, Y. Su et al., Constructing a high-energy and durable single-crystal NCM811 cathode for all-solid-state batteries by a surface engineering strategy. ACS Appl. Mater. Interfaces 13(35), 41669–41679 (2021). https://doi.org/10.1021/acsami.1c11419
  25. Y. Wang, Z. Wang, D. Wu, Q. Niu, P. Lu et al., Stable Ni-rich layered oxide cathode for sulfide-based all-solid-state lithium battery. eScience 2(5), 537–545 (2022). https://doi.org/10.1016/j.esci.2022.06.001
  26. J. Wang, S. Zhao, A. Zhang, H. Zhuo, G. Zhang et al., High lithium-ion conductivity, halide-coated, Ni-rich NCM improves cycling stability in sulfide all-solid-state batteries. ACS Appl. Energy Mater. 6, 3671–3681 (2023). https://doi.org/10.1021/acsaem.2c02774
  27. Y. Huang, L. Zhou, C. Li, Z. Yu, L.F. Nazar, Waxing bare high-voltage cathode surfaces to enable sulfide solid-state batteries. ACS Energy Lett. 8(11), 4949–4956 (2023). https://doi.org/10.1021/acsenergylett.3c01717
  28. J. Liang, Y. Zhu, X. Li, J. Luo, S. Deng et al., A gradient oxy-thiophosphate-coated Ni-rich layered oxide cathode for stable all-solid-state Li-ion batteries. Nat. Commun. 14(1), 146 (2023). https://doi.org/10.1038/s41467-022-35667-7
  29. J. Kim, M.J. Kim, J. Kim, J.W. Lee, J. Park et al., High-performance all-solid-state batteries enabled by intimate interfacial contact between the cathode and sulfide-based solid electrolytes. Adv. Funct. Mater. 33(12), 2211355 (2023). https://doi.org/10.1002/adfm.202211355
  30. Y. Su, X. Liu, H. Yan, J. Zhao, Y. Cheng et al., Assembly of an elastic & sticky interfacial layer for sulfide-based all-solid-state batteries. Nano Energy 113, 108572 (2023). https://doi.org/10.1016/j.nanoen.2023.108572
  31. H. Kim, J.Y. Jung, K. Kim, C. Hwang, J. Yu et al., Functionalized electrode additive for simultaneously reinforcing chemo-mechanical properties of millimeter-thick dry-electrode for high-energy all-solid-state batteries. Adv. Energy Mater. 14(14), 2303965 (2024). https://doi.org/10.1002/aenm.202303965
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