pp 1–9 | Cite as

Flexible current collector–free LiFePO4/carbon composite film for high-performance lithium-ion batteries

  • Xiaoshuo Liu
  • Weijing Qi
  • Tong Zou
  • Dinghuan Fan
  • Shouhui Guo
  • Yong Zhao
  • Li WangEmail author
Original Paper


A facile formation of free-standing LiFePO4/carbon (LiFePO4/C) composite film with flexibility and current collector–free is presented. This composite film has been prepared via a simple coating process by spreading out slurry onto a hydrophobic surface. Such free-standing film exhibits excellent flexibility and mechanical strength. The mechanical measurements show that the fracture strength and modulus of flexible film are up to 0.65 MPa and 109.6 MPa, respectively. The electrochemical properties of this film have been obtained in a half-cell configuration. The results display that the film delivers an initial discharge capacity of ~ 156 mAh/g at 0.1 C; the charge-discharge efficiency is as high as 98%. Moreover, at 10 C, the specific capacity can be kept at ~ 133 mAh/g, with very little capacity loss after 500 cycles (< 0.02‰ per cycle). The as-prepared flexible film is inexpensive and simple, providing a great potential for the commercialization of high-performance flexible lithium-ion batteries.


LiFePO4/carbon Lithium ion batteries Flexible Current collector–free 


Funding information

This study was financially supported by Natural Science Foundation of China (Grant Nos. 61474059 and 11727902). L.W. acknowledges Jiangxi Provincial Innovation Talents of Science and Technology (20165BCB18003).

Supplementary material

11581_2019_2869_MOESM1_ESM.docx (3.5 mb)
ESM 1 (DOCX 3586 kb)


  1. 1.
    Nishide H, Oyaizu K (2008) Toward flexible batteries. Science 319:737–738CrossRefGoogle Scholar
  2. 2.
    Zhang G, Han E, Zhu L, Jing Q (2015) Preparation of LiFe0.98M0.02PO4/C cathode material for lithium-ion battery. Ionics 21:319–324CrossRefGoogle Scholar
  3. 3.
    Qu G, Cheng J, Li X, Yuan D, Chen P, Chen X, Wang B, Peng H (2016) A fiber supercapacitor with high energy density based on hollow graphene/conducting polymer fiber electrode. Adv Mater 28:3646–3652CrossRefGoogle Scholar
  4. 4.
    Case MA, Burwick HA, Volpp KG, Patel MS (2015) Accuracy of smartphone applications and wearable devices for tracking physical activity data. JAMA 313:625–626CrossRefGoogle Scholar
  5. 5.
    Pushparaj VL, Shaijumon MM, Kumar A, Murugesan S, Ci L, Vajtai R, Linhardt RJ, Nalamasu O, Ajayan PM (2007) Flexible energy storage devices based on nanocomposite paper. Proc Natl Acad Sci U S A 104:13574–13577CrossRefGoogle Scholar
  6. 6.
    Subramanian Y, Kaliyappan K, Ramakrishnan KS (2017) Facile hydrothermal synthesis and characterization of Co2GeO4/r-GO@C ternary nanocomposite as negative electrode for Li-ion batteries. J Colloid Interf Sci 498:76–84CrossRefGoogle Scholar
  7. 7.
    Liu W, Chen Z, Zhou G, Sun Y, Lee HR, Liu C, Yao H, Bao Z, Cui Y (2016) 3D porous sponge-inspired electrode for stretchable lithium-ion batteries. Adv Mater 28:3578–3583CrossRefGoogle Scholar
  8. 8.
    Koo M, Park KI, Lee SH, Suh M, Jeon DY, Choi JW, Kang K, Lee KJ (2012) Bendable inorganic thin-film battery for fully flexible electronic systems. Nano Lett 12:4810–4816CrossRefGoogle Scholar
  9. 9.
    Liu W, Song MS, Kong B, Cui Y (2017) Flexible and stretchable energy storage: recent advances and future perspectives. Adv Mater 29:1603436CrossRefGoogle Scholar
  10. 10.
    Lui G, Li G, Wang X, Jiang G, Lin E, Fowler M, Yu A, Chen Z (2016) Flexible, three-dimensional ordered macroporous TiO2 electrode with enhanced electrode–electrolyte interaction in high-power Li-ion batteries. Nano Energy 24:72–77CrossRefGoogle Scholar
  11. 11.
    Liu QB, Liao SJ, Song HY, Liang ZX (2012) High-performance LiFePO4/C materials: effect of carbon source on microstructure and performance. J Power Sources 211:52–58CrossRefGoogle Scholar
  12. 12.
    Tian R, Liu H, Jiang Y, Chen J, Tan X, Liu G, Zhang L, Gu X, Guo Y, Wang H, Sun L, Chu W (2015) Drastically enhanced high-rate performance of carbon-coated LiFePO4 nanorods using a green chemical vapor deposition (CVD) method for lithium ion battery: a selective carbon coating process. ACS Appl Mater Interfaces 7:11377–11386CrossRefGoogle Scholar
  13. 13.
    Hamid NA, Wennig S, Hardt S, Heinzel A, Schulz C, Wiggers H (2012) High-capacity cathodes for lithium-ion batteries from nanostructured LiFePO4 synthesized by highly-flexible and scalable flame spray pyrolysis. J Power Sources 216:76–83CrossRefGoogle Scholar
  14. 14.
    Kim HS, Kam DW, Kim WS, Koo HJ (2011) Synthesis of the LiFePO4 by a solid-state reaction using organic acid as a reducing agent. Ionics 17:293–297CrossRefGoogle Scholar
  15. 15.
    Jia X, Chen Z, Suwarnasarn A, Rice L, Wang X, Sohn H, Zhang Q, Wu BM, Wei F, Lu Y (2012) High-performance flexible lithium-ion electrodes based on robust network architecture. Energy Environ Sci 5:6845–6849CrossRefGoogle Scholar
  16. 16.
    Hu L, Wu H, La Mantia F, Yang Y, Cui Y (2010) Thin, flexible secondary Li-ion paper batteries. ACS Nano 4:5843–5848CrossRefGoogle Scholar
  17. 17.
    Kretschmer K, Sun B, Xie X, Chen S, Wang G (2016) A free-standing LiFePO4–carbon paper hybrid cathode for flexible lithium-ion batteries. Green Chem 18:2691–2698CrossRefGoogle Scholar
  18. 18.
    Song JY, Lee HH, Hong WG, Huh YS, Lee YS, Kim HJ, Jun YS (2018) A polysulfide-infiltrated carbon cloth cathode for high-performance flexible lithium–sulfur batteries. Nanomaterials 8:90CrossRefGoogle Scholar
  19. 19.
    Ha SH, Shin KH, Park HW, Lee YJ (2018) Flexible lithium-ion batteries with high areal capacity enabled by smart conductive textiles. Small 14:1703418Google Scholar
  20. 20.
    Gao P, Xu S, Chen Z, Huang X, Bao Z, Lao C, Wu G, Mei Y (2018) Flexible and hierarchically structured sulfur composite cathode based on the carbonized textile for high-performance Li-S batteries. ACS Appl Mater Interfaces 10:3938–3947CrossRefGoogle Scholar
  21. 21.
    Gaikwad AM, Zamarayeva AM, Rousseau J, Chu H, Derin I, Steingart DA (2012) Highly stretchable alkaline batteries based on an embedded conductive fabric. Adv Mater 24:5071–5076CrossRefGoogle Scholar
  22. 22.
    Li N, Chen Z, Ren W, Li F, Cheng HM (2012) Flexible graphene-based lithium ion batteries with ultrafast charge and discharge rates. Proc Natl Acad Sci 109:17360–17365CrossRefGoogle Scholar
  23. 23.
    Wang F, Cai J, Yu J, Li C, Yang Z (2018) Simultaneous electrospinning and electrospraying: fabrication of a carbon nanofibre/MnO/reduced graphene oxide thin film as a high-performance anode for lithium-ion batteries. ChemElectroChem 5:51–61CrossRefGoogle Scholar
  24. 24.
    Shi Y, Wen L, Zhou G, Chen J, Pei S, Huang K, Cheng HM, Li F (2015) Graphene-based integrated electrodes for flexible lithium ion batteries. 2D Mater 2:024004CrossRefGoogle Scholar
  25. 25.
    Jabbour L, Chaussy D, Beneventi D, Destro M, Gerbaldi C, Penazzi N, Bodoardo C (2013) Flexible cellulose/LiFePO4 paper-cathodes: toward eco-friendly all-paper Li-ion batteries. Cellulose 20:571–582CrossRefGoogle Scholar
  26. 26.
    Leijonmarck S, Cornell A, Lindbergh G, Wågberg L (2013) Single-paper flexible Li-ion battery cells through a paper-making process based on nano-fibrillated cellulose. J Mater Chem A 1:4671–4677CrossRefGoogle Scholar
  27. 27.
    Wang Y, He ZY, Wang YX, Fan C, Peng QL, Chen JJ, Feng ZS (2018) Preparation and characterization of flexible lithium iron phosphate/graphene/cellulose electrode for lithium ion batteries. J Colloid Interface Sci 512:398–403CrossRefGoogle Scholar
  28. 28.
    Ding J, Fu S, Zhang R, Boon E, Lee W, Fisher FT, Yang EH (2017) Graphene—vertically aligned carbon nanotube hybrid on PDMS as stretchable electrodes. Nanotechnology 28:465302CrossRefGoogle Scholar
  29. 29.
    Huang L, Guan Q, Cheng J, Li C, Ni W, Wang Z, Zhang Y, Wang B (2018) Free-standing N-doped carbon nanofibers/carbon nanotubes hybrid film for flexible, robust half and full lithium-ion batteries. Chem Eng J 334:682–690CrossRefGoogle Scholar
  30. 30.
    Chen Z, To JW, Wang C, Lu Z, Liu N, Chortos A, Pan L, Wei F, Cui Y, Bao Z (2014) A three-dimensionally interconnected carbon nanotube–conducting polymer hydrogel network for high-performance flexible battery electrodes. Adv Energy Mater 4:1400207CrossRefGoogle Scholar
  31. 31.
    Cao S, Feng X, Song Y, Xue X, Liu H, Miao M, Fang J, Shi L (2015) Integrated fast assembly of free-standing lithium titanate/carbon nanotube/cellulose nanofiber hybrid network film as flexible paper-electrode for lithium-ion batteries. ACS Appl Mater Interfaces 7:10695CrossRefGoogle Scholar
  32. 32.
    Cao S, Feng X, Song Y, Liu H, Miao M, Fang J, Shi L (2016) In situ carbonized cellulose-based hybrid film as flexible paper anode for lithium-ion batteries. ACS Appl Mater Interfaces 8:1073–1079CrossRefGoogle Scholar
  33. 33.
    Hiura H, Ebbesen TW, Tanigaki K, Takahashi H (1993) Raman studies of carbon nanotubes. Chem Phys Lett 202:509–512CrossRefGoogle Scholar
  34. 34.
    Cui K, Hu S, Li Y (2016) Nitrogen-doped graphene-decorated LiVPO4F nanocomposite as high-voltage cathode material for rechargeable lithium-ion batteries. J Power Sources 325:465–473CrossRefGoogle Scholar
  35. 35.
    Muraliganth T, Murugan AV, Manthiram A (2008) Nanoscale networking of LiFePO4 nanorods synthesized by a microwave-solvothermal route with carbon nanotubes for lithium ion batteries. J Mater Chem 18:5661–5668CrossRefGoogle Scholar
  36. 36.
    Chen M, Kou K, Tu M, Hu J, Du X, Yang B (2017) Conducting reduced graphene oxide wrapped LiFePO4/C nanocrystal as cathode material for high-rate lithium secondary batteries. Solid State Ionics 310:95–99CrossRefGoogle Scholar
  37. 37.
    Gong H, Xue H, Wang T, He J (2016) In-situ synthesis of monodisperse micro-nanospherical LiFePO4/carbon cathode composites for lithium-ion batteries. J Power Sources 318:220–227CrossRefGoogle Scholar
  38. 38.
    Liu H, Miao C, Meng Y, He YB, Xu Q, Zhang X, Tang Z (2014) Optimized synthesis of nano-sized LiFePO4/C particles with excellent rate capability for lithium ion batteries. Electrochim Acta 130:322–328CrossRefGoogle Scholar
  39. 39.
    Li X, Luo D, Zhang X, Zhang Z (2015) Enhancement of electrochemical performances for LiFePO4/C with 3D-grape-bunch structure and selection of suitable equivalent circuit for fitting EIS results. J Power Sources 291:75–84CrossRefGoogle Scholar
  40. 40.
    Tian X, Zhou Y, Tu X, Zhang Z, Du G (2017) Well-dispersed LiFePO4 nanoparticles anchored on a three-dimensional graphene aerogel as high-performance positive electrode materials for lithium-ion batteries. J Power Sources 340:40–50CrossRefGoogle Scholar
  41. 41.
    Xiong QQ, Lou JJ, Teng XJ, Lu XX, Liu SY, Chi HZ, Ji ZG (2018) Controllable synthesis of N-C@ LiFePO4 nanospheres as advanced cathode of lithium ion batteries. J Alloys Compd 743:377–382CrossRefGoogle Scholar
  42. 42.
    Ha SH, Lee YJ (2015) Core–shell LiFePO4/carbon-coated reduced graphene oxide hybrids for high-power lithium-ion battery cathodes. Chem Eur J 21:2132–2138CrossRefGoogle Scholar
  43. 43.
    Wu YJ, Gu YJ, Chen YB, Liu HQ, Liu CQ (2018) Effect of lithium phosphate on the structural and electrochemical performance of nanocrystalline LiFePO4 cathode material with iron defects. Int J Hydrog Energy 43:2050–2056CrossRefGoogle Scholar

Copyright information

© Springer-Verlag GmbH Germany, part of Springer Nature 2019

Authors and Affiliations

  • Xiaoshuo Liu
    • 1
  • Weijing Qi
    • 1
  • Tong Zou
    • 1
  • Dinghuan Fan
    • 1
  • Shouhui Guo
    • 1
  • Yong Zhao
    • 1
  • Li Wang
    • 1
    Email author
  1. 1.Department of PhysicsNanchang UniversityNanchangChina

Personalised recommendations