, Volume 24, Issue 10, pp 2935–2943 | Cite as

Improving Li-ion battery charge rate acceptance through highly ordered hierarchical electrode design

  • Yunsung Kim
  • Andy Drews
  • Rajeswari Chandrasekaran
  • Ted Miller
  • Jeff SakamotoEmail author
Original Paper


In Li-ion technology, increasing electrode loading (thickness) is one approach to improve performance; however, this approach typically compromises power density and safety. To achieve the goal of decoupling energy and power density, a novel electrode architecture is proposed. The electrode design enhances uniform ionic current, especially in thick electrodes. A highly ordered and hierarchical (HOH) graphite anode concept was designed, fabricated, and tested for efficacy. The HOH electrodes consisted of ordered arrays of macro-scale line-of-sight linear channels made through laser ablation. SEM and Raman spectroscopy demonstrated that laser ablation is a feasible approach to fabricate HOH electrodes without affecting the graphite anode chemistry, respectively. A 65–120% improvement in charge rate acceptance (5.5 mAh/cm2) was achieved in the HOH electrodes compared to conventional electrodes. A restricted diffusion direct current polarization test determined that the HOH design improved ionic flow throughout porous electrodes. Altogether, the results of this study suggest that improved charge rate acceptance can be achieved by engineering electrode porosity to mitigate the effects of concentration polarization in high energy density graphite anodes. These findings can facilitate the development of higher energy and power density Li-ion batteries, while improving resilience against Li plating under severe charge conditions.


Li-ion battery High energy density HOH Tortuosity Concentratio-polarization Li plating 



This research was supported by the Ford University Research Program (2011-7027R). Authors YK and JS would also like to acknowledge initial support from the Michigan Economic Development Corporation and Dr. Mike Wixom.


  1. 1.
    Tarascon JM, Armand M (2001) Issues and challenges facing rechargeable lithium batteries. Nature 414:359–367CrossRefGoogle Scholar
  2. 2.
    Nyqvist B, Nilsson M (2012) Rapidly falling costs of battery packs for electric vehicles. Nat Clim Chang 5:329–332CrossRefGoogle Scholar
  3. 3.
    Van Norden R (2014) A better battery; chemists are reinventing rechargeable cells to drive down costs and boost capacity. Nature 507:26–28CrossRefGoogle Scholar
  4. 4.
    Buqa H, Goers D, Holzapfel M, Spahr ME, Novak P (2005) High rate capability of graphite negative electrodes for lithium-ion batteries. J Electrochem Soc 152:A474–A481CrossRefGoogle Scholar
  5. 5.
    Kang K, Ming YS, Breger J, Grey CP, Cedar G (2006) Electrodes with high power and high capacity for rechargeable lithium batteries. Science 311:977–981CrossRefGoogle Scholar
  6. 6.
    Thorat IV, Stephenson DE, Zacharias NA, Zaghib K, Harb JN, Wheeler DR (2009) Quantifying tortuosity in porous Li-ion battery materials. J Power Sources 188:592–600CrossRefGoogle Scholar
  7. 7.
    US Advanced Battery Consortium (USABC) goals for advanced batteries for EVs (2006). Available at:
  8. 8.
    Bae CJ, Erdonmez CK, Halloran JW, Chiang YM (2013) Design of battery electrodes with dual-scale porosity to minimize tortuosity and maximize performance. Adv Mater 25:1254–1258CrossRefGoogle Scholar
  9. 9.
    Kehrwald D (2011) Local tortuosity inhomogeneities in a lithium battery composite electrode. J Electochem Soc 158:A1393–A1399CrossRefGoogle Scholar
  10. 10.
    Jiang C, Hosono E, Zhou H (2006) Nanomaterials for lithium ion batteries. Nanotoday 1:28–33CrossRefGoogle Scholar
  11. 11.
    Nemani VP, Harris SJ, Smith KC (2015) Design of Bi-tortuous, anisotropic graphite anodes for fast ion-transport in Li-ion batteries. J Electochem Soc 162:A1415–A1423CrossRefGoogle Scholar
  12. 12.
    Ogihara N, Itou Y, Sasaki T, Takeuchi Y (2015) Impedance spectroscopy characterization of porous electrodes under different electrode thickness using a symmetric cell for high-performance lithium-ion batteries. J Phys Chem C 119:4612–4619CrossRefGoogle Scholar
  13. 13.
    Sakamoto JS, Dunn B (2002) Hierarchical battery electrodes based on inverted opal structures. J Mater Chem 12:2859–2861CrossRefGoogle Scholar
  14. 14.
    Zhang H, Yu X, Braun PV (2011) Three-dimensional bi-continuous ultrafast-charge and -discharge bulk battery electrodes. Nature Nanotechn Lett 6:277–281CrossRefGoogle Scholar
  15. 15.
    Qi Y, Harris SJ (2010) In situ observation of strains during lithiation of a graphite electrode. J Electrochem Soc 157:A741–A747CrossRefGoogle Scholar
  16. 16.
    Zhang SS, Ding MS, Xu K, Allen J, Jow TR (2001) Understanding solid electrolyte interface film formation on graphite electrodes. Electrochem Solid-State Lett 4:A206–A208CrossRefGoogle Scholar
  17. 17.
    Malard LM, Pimenta MA, Dresselhaus G, Dresselhaus MS (2009) Raman spectroscopy in graphene. Phys Rep 473:51–87CrossRefGoogle Scholar
  18. 18.
    Yaqub A, Lee YJ, Hwang MJ, Pervez SA, Farooq U, Choi JH, Doh CH (2014) Effects of electrode loading on low temperature performances of Li-ion batteries. Physica Status Solidi 211:2625–2630CrossRefGoogle Scholar
  19. 19.
    Huang CK, Sakamoto JS, Wolfenstine J, Surampudi S (2000) The limits of low-temperature performance of Li-ion cells. J Electrochem Soc 147:2893–2896CrossRefGoogle Scholar
  20. 20.
    Virkar AV, Chen J, Tanner CW, Kim JW (2000) The role of electrode microstructure on activation and concentration polarizations in solid oxide fuel cells. Solid State Ionics 131:189–198CrossRefGoogle Scholar
  21. 21.
    Doyle M, Newman J (1997) Analysis of capacity-rate data for lithium batteries using simplified models of the discharge process. J App Electrochem 27:846–856CrossRefGoogle Scholar
  22. 22.
    Newman J (1995) Optimization of porosity and thickness of a battery electrode by means of a reaction-zone model. J Electrochem Soc 142:91–101CrossRefGoogle Scholar
  23. 23.
    Yihang L, Zhang W, Zhu Y, Luo Y, Xu Y, Brown A, Culver JN et al (2013) Architecturing hierarchical function layers on self-assembled viral templates as 3D nano-array electrodes for integrated Li-ion microbatteries. Nano 13:293–300Google Scholar
  24. 24.
    Vijayaraghavan B, Ely DR, Chiang YM, Garcia-Garcia R, Edwin-Garcia R (2012) An analytical method to determine tortuosity in rechargeable battery electrodes. J. Electrochem. Soc 159:A548–A552CrossRefGoogle Scholar
  25. 25.
    Da-Wei W, Li F, Liu M, Lu GQ, Cheng H-M (2008) 3D aperiodic hierarchical porous graphitic carbon material for high-rate electrochemical capacitive energy storage. Angew Chemie 120:379–382CrossRefGoogle Scholar

Copyright information

© Springer-Verlag GmbH Germany, part of Springer Nature 2018

Authors and Affiliations

  • Yunsung Kim
    • 1
  • Andy Drews
    • 2
  • Rajeswari Chandrasekaran
    • 2
  • Ted Miller
    • 2
  • Jeff Sakamoto
    • 1
    Email author
  1. 1.Department of Mechanical EngineeringUniversity of MichiganAnn ArborUSA
  2. 2.Research and Advanced EngineeringFord Motor CompanyDearbornUSA

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