Skip to main content

Thank you for visiting You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser (or turn off compatibility mode in Internet Explorer). In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript.

High areal capacity battery electrodes enabled by segregated nanotube networks


Increasing the energy storage capability of lithium-ion batteries necessitates maximization of their areal capacity. This requires thick electrodes performing at near-theoretical specific capacity. However, achievable electrode thicknesses are restricted by mechanical instabilities, with high-thickness performance limited by the attainable electrode conductivity. Here we show that forming a segregated network composite of carbon nanotubes with a range of lithium storage materials (for example, silicon, graphite and metal oxide particles) suppresses mechanical instabilities by toughening the composite, allowing the fabrication of high-performance electrodes with thicknesses of up to 800 μm. Such composite electrodes display conductivities up to 1 × 104 S m−1 and low charge-transfer resistances, allowing fast charge-delivery and enabling near-theoretical specific capacities, even for thick electrodes. The combination of high thickness and specific capacity leads to areal capacities of up to 45 and 30 mAh cm−2 for anodes and cathodes, respectively. Combining optimized composite anodes and cathodes yields full cells with state-of-the-art areal capacities (29 mAh cm−2) and specific/volumetric energies (480 Wh kg−1 and 1,600 Wh l−1).

This is a preview of subscription content, access via your institution

Relevant articles

Open Access articles citing this article.

Access options

Rent or buy this article

Prices vary by article type



Prices may be subject to local taxes which are calculated during checkout

Fig. 1: Fabrication of hierarchical composite electrodes.
Fig. 2: Segregated networks based on different active materials.
Fig. 3: Effect of mechanical reinforcement on achievable thickness.
Fig. 4: Electrochemical characterization of segregated network electrodes with high mass loading.
Fig. 5: Electrochemical performance of full-cell lithium-ion batteries made by pairing 2 μm-Si/7.5 wt%CNT composite anodes with NMC811/0.5 wt%CNT composite cathodes.

Data availability

The datasets generated during and/or analysed during the current study are available from the corresponding author on reasonable request.


  1. Dunn, B., Kamath, H. & Tarascon, J. M. Electrical energy storage for the grid: a battery of choices. Science 334, 928–935 (2011).

    Article  Google Scholar 

  2. Chiu, R. C., Garino, T. J. & Cima, M. J. Drying of granular ceramic films. 1. Effect of processing variables on cracking behavior. J. Am. Ceram. Soc. 76, 2257–2264 (1993).

    Article  Google Scholar 

  3. Singh, K. B. & Tirumkudulu, M. S. Cracking in drying colloidal films. Phys. Rev. Lett. 98, 218302 (2007).

    Article  Google Scholar 

  4. Danner, T. et al. Thick electrodes for Li-ion batteries: a model based analysis. J. Power Sources 334, 191–201 (2016).

    Article  Google Scholar 

  5. Wang, G. P., Zhang, Q. T., Yu, Z. L. & Qu, M. Z. The effect of different kinds of nano-carbon conductive additives in lithium ion batteries on the resistance and electrochemical behavior of the LiCoO2 composite cathodes. Solid State Ion. 179, 263–268 (2008).

    Article  Google Scholar 

  6. Tian, R. et al. Quantifying the factors limiting rate-performance in battery electrodes. Nat. Commun. 10, 1933 (2019).

    Article  Google Scholar 

  7. Higgins, T. M. et al. A commercial conducting polymer as both binder and conductive additive for silicon nanoparticle-based lithium-ion battery negative electrodes. ACS Nano 10, 3702–3713 (2016).

    Article  Google Scholar 

  8. Sander, J. S. et al. High-performance battery electrodes via magnetic templating. Nat. Energy 1, 16099 (2016).

    Article  Google Scholar 

  9. Salvatierra, R. V. et al. Silicon nanowires and lithium cobalt oxide nanowires in graphene nanoribbon papers for full lithium ion battery. Adv. Energy Mater. 6, 1600918 (2016).

    Article  Google Scholar 

  10. Peled, E. et al. Tissue-like silicon nanowires-based three-dimensional anodes for high-capacity lithium ion batteries. Nano Lett. 15, 3907–3916 (2015).

    Article  Google Scholar 

  11. Leveau, L. et al. Silicon nano-trees as high areal capacity anodes for lithium-ion batteries. J. Power Sources 316, 1–7 (2016).

    Article  Google Scholar 

  12. Yang, G. F., Song, K. Y. & Joo, S. K. Ultra-thick Li-ion battery electrodes using different cell size of metal foam current collectors. RSC Adv. 5, 16702–16706 (2015).

    Article  Google Scholar 

  13. Wang, J. S. et al. Formulation and characterization of ultra-thick electrodes for high energy lithium-ion batteries employing tailored metal foams. J. Power Sources 196, 8714–8718 (2011).

    Article  Google Scholar 

  14. Hu, L. B. et al. Lithium-ion textile batteries with large areal mass loading. Adv. Energy Mater. 1, 1012–1017 (2011).

    Article  Google Scholar 

  15. Elango, R., Demortiere, A., De Andrade, V., Morcrette, M. & Seznec, V. Thick binder-free electrodes for Li-ion battery fabricated using templating approach and spark plasma sintering reveals high areal capacity. Adv. Energy Mater. 8, 1703031 (2018).

    Article  Google Scholar 

  16. Choi, M. J. et al. Novel strategy to improve the Li-storage performance of micro silicon anodes. J. Power Sources 348, 302–310 (2017).

    Article  Google Scholar 

  17. Zhang, C. F. et al. Enabling flexible heterostructures for li-ion battery anodes based on nanotube and liquid-phase exfoliated 2D gallium chalcogenide nanosheet colloidal solutions. Small 13, 1701677 (2017).

    Article  Google Scholar 

  18. Liu, Y. P. et al. Electrical, mechanical and capacity percolation leads to high-performance MoS2/nanotube composite lithium ion battery electrodes. ACS Nano 10, 5980–5990 (2016).

    Article  Google Scholar 

  19. Jurewicz, I. et al. Locking carbon nanotubes in confined lattice geometries—a route to low percolation in conducting composites. J. Phys. Chem. B 115, 6395–6400 (2011).

    Article  Google Scholar 

  20. Sundaram, R. M. & Windle, A. H. One-step purification of direct-spun CNT fibers by post-production sonication. Mater. Des. 126, 85–90 (2017).

    Article  Google Scholar 

  21. Gabbett, C. et al. The effect of network formation on the mechanical properties of 1D:2D nano:nano composites. Chem. Mater. 30, 5245–5255 (2018).

    Article  Google Scholar 

  22. Ge, H. C. & Wang, J. C. Ear-like poly (acrylic acid)-activated carbon nanocomposite: a highly efficient adsorbent for removal of Cd(ii) from aqueous solutions. Chemosphere 169, 443–449 (2017).

    Article  Google Scholar 

  23. Wang, W. et al. Silicon decorated cone shaped carbon nanotube clusters for lithium ion battery anodes. Small 10, 3389–3396 (2014).

    Article  Google Scholar 

  24. Zhang, L. et al. A coordinatively cross-linked polymeric network as a functional binder for high-performance silicon submicro-particle anodes in lithium-ion batteries. J. Mater. Chem. C 2, 19036–19045 (2014).

    Article  Google Scholar 

  25. Assresahegn, B. D. & Belanger, D. Effects of the formulations of silicon-based composite anodes on their mechanical, storage and electrochemical properties. ChemSusChem 10, 4080–4089 (2017).

    Article  Google Scholar 

  26. Li, X. L. et al. Mesoporous silicon sponge as an anti-pulverization structure for high-performance lithium-ion battery anodes. Nat. Commun. 5, 4105 (2014).

    Article  Google Scholar 

  27. Yan, L. J. et al. In situ wrapping Si nanoparticles with 2D carbon nanosheets as high-areal-capacity anode for lithium-ion batteries. ACS Appl. Mater. Interfaces 9, 38159–38164 (2017).

    Article  Google Scholar 

  28. Krause, A. et al. High area capacity lithium-sulfur full-cell battery with prelitiathed silicon nanowire-carbon anodes for long cycling stability. Sci. Rep. 6, 27982 (2016).

    Article  Google Scholar 

  29. Li, B., Li, S. M., Xu, J. J. & Yang, S. B. A new configured lithiated silicon–sulfur battery built on 3D graphene with superior electrochemical performances. Energy Environ. Sci. 9, 2025–2030 (2016).

    Article  Google Scholar 

  30. Shi, F. F. et al. Failure mechanisms of single-crystal silicon electrodes in lithium-ion batteries. Nat. Commun. 7, 11886 (2016).

    Article  Google Scholar 

  31. Nguyen, C. C. & Lucht, B. L. Development of electrolytes for Si–graphite composite electrodes. J. Electrochem. Soc. 165, A2154–A2161 (2018).

    Article  Google Scholar 

  32. Singh, M., Kaiser, J. & Hahn, H. Thick electrodes for high energy lithium ion batteries. J. Electrochem. Soc. 162, A1196–A1201 (2015).

    Article  Google Scholar 

  33. Singh, M., Kaiser, J. & Hahn, H. A systematic study of thick electrodes for high energy lithium ion batteries. J. Electroanal. Chem. 782, 245–249 (2016).

    Article  Google Scholar 

  34. Gallagher, K. G. et al. Optimizing areal capacities through understanding the limitations of lithium-ion electrodes. J. Electrochem. Soc. 163, A138–A149 (2016).

    Article  Google Scholar 

  35. Purvins, A., Papaioannou, I. T. & Debarberis, L. Application of battery-based storage systems in household-demand smoothening in electricity-distribution grids. Energy Convers. Manag. 65, 272–284 (2013).

    Article  Google Scholar 

  36. Yamada, M. et al. Performance of the ‘SiO’-carbon composite-negative electrodes for high-capacity lithium-ion batteries; prototype 14500 batteries. J. Power Sources 225, 221–225 (2013).

    Article  Google Scholar 

  37. Son, I. H. et al. Silicon carbide-free graphene growth on silicon for lithium-ion battery with high volumetric energy density. Nat. Commun. 6, 7393 (2015).

    Article  Google Scholar 

  38. Ma, L. et al. A guide to ethylene carbonate-free electrolyte making for Li-ion cells. J. Electrochem. Soc. 164, A5008–A5018 (2017).

    Article  Google Scholar 

Download references


All authors acknowledge the SFI-funded AMBER research centre (SFI/12/RC/2278) and the Advanced Microscopy Laboratory for the provision of facilities and thank R. Charifou, who performed XRD for the samples. J.N.C. thanks Science Foundation Ireland (SFI, 11/PI/1087), the European Research Council (AdvGr FUTUREPRINT) and the Graphene Flagship (grant agreement no. 785219) for funding. V.N. thanks the European Research Council (SoG 3D2D Print) and Science Foundation Ireland (PIYRA) for funding.

Author information

Authors and Affiliations



S.-H.P., P.J.K., J.N.C. and V.N. conceived the project. S.-H.P. and P.J.K. designed materials and experiments. S.-H.P. and P.J.K. fabricated composite electrodes. S.-H.P. performed electrochemical characterization. N.M. performed Raman analysis. S.-H.P., P.J.K., J.C. and R.T. analysed electrochemical data. J.C. and D.D. performed electron microscopic analysis. S.-H.P. and J.C.-F.Z. measured electrical conductivity. C.S.B. and P.M. performed mechanical measurement. S.-H.P. and J.N.C. wrote the manuscript. All authors discussed the results and commented on the manuscript.

Corresponding authors

Correspondence to Jonathan N. Coleman or Valeria Nicolosi.

Ethics declarations

Competing interests

The authors declare no competing interests.

Additional information

Publisher’s note: Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Supplementary information

Supplementary Information

Supplementary Figs. 1–28, Supplementary Tables 8, Supplementary Note 1, Supplementary references

Rights and permissions

Reprints and Permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Park, SH., King, P.J., Tian, R. et al. High areal capacity battery electrodes enabled by segregated nanotube networks. Nat Energy 4, 560–567 (2019).

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI:

This article is cited by


Quick links

Nature Briefing

Sign up for the Nature Briefing newsletter — what matters in science, free to your inbox daily.

Get the most important science stories of the day, free in your inbox. Sign up for Nature Briefing