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Chronoamperometry as an electrochemical in situ approach to investigate the electrolyte wetting process of lithium-ion cells

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Understanding and optimizing the electrolyte wetting of lithium-ion cells provides a high potential to reduce the manufacturing costs of lithium-ion cells. However, established methods to investigate the wetting of porous materials are not easily transferable to lithium-ion cells, since they neglect major paths in the wetting process. In this study, a novel method is proposed to in situ quantify the wetting progress in lithium-ion cells with graphite-based anodes. A constant potential is applied to the cell immediately after the electrolyte wetting process has been initiated and the current response is carefully analyzed as it reflects the progress of the electrolyte wetting process accompanied by SEI film formation. By applying this procedure, the influence of different separators, cell formats and ambient temperatures on the wetting time is investigated. Furthermore, the wetting behavior of laser-structured electrodes is investigated as well as of electrodes with ceramic multilayer coating which can replace the standard separator. The results demonstrate that the interface between the separator and the electrodes plays a dominant role and mainly influences the wetting process of a lithium-ion cell. The findings point out the importance of using in situ methods to analyze the wetting process of lithium-ion cells.

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  1. 1.

    In Fig. 6hmax is the longest dimension of the pouch bag cell. To find hmax, we assume that the electrolyte is penetrating the cell homogeneously from all four edges. This is realistic as the capillary tubes between cell stack and pouch bag foil are filled with electrolyte quickly and the capillary diameter for those is much bigger than the capillary diameters expected in the electrode stack. This is also supported by the measurements of Weydanz et al. in [5]. Therefore, hmax is defined as half the length of the anode, which is 25 mm for the standard cell dimension.


  1. 1.

    Scrosati B, Garche J (2010) Lithium batteries: status, prospects and future. J Power Sources 195(9):2419–2430. https://doi.org/10.1016/j.jpowsour.2009.11.048

  2. 2.

    Wood DL, Li J, Daniel C (2015) Prospects for reducing the processing cost of lithium-ion batteries. J Power Sources 275:234–242. https://doi.org/10.1016/j.jpowsour.2014.11.019

  3. 3.

    Knoche T, Surek F, Reinhart G (2016) A process model for the electrolyte filling of lithium-ion batteries. Procedia CIRP 41:405–410. https://doi.org/10.1016/j.procir.2015.12.044

  4. 4.

    Knoche T, Zinth V, Schulz M et al (2016) In situ visualization of the electrolyte solvent filling process by neutron radiography. J Power Sources 331:267–276. https://doi.org/10.1016/j.jpowsour.2016.09.037

  5. 5.

    Weydanz WJ, Reisenweber H, Gottschalk A et al (2018) Visualization of electrolyte filling process and influence of vacuum during filling for hard case prismatic lithium-ion cells by neutron imaging to optimize the production process. J Power Sources 380:126–134. https://doi.org/10.1016/j.jpowsour.2018.01.081

  6. 6.

    Wu M-S, Liao T-L, Wang Y-Y et al (2004) Assessment of the wettability of porous electrodes for lithium-ion batteries. J Appl Electrochem 34(8):797–805. https://doi.org/10.1023/B:JACH.0000035599.56679.15

  7. 7.

    Kühnel R-S, Obeidi S, Lübke M et al (2013) Evaluation of the wetting time of porous electrodes in electrolytic solutions containing ionic liquid. J Appl Electrochem 43(7):697–704. https://doi.org/10.1007/s10800-013-0558-x

  8. 8.

    Günter FJ, Habedank JB, Schreiner D et al (2018) Introduction to electrochemical impedance spectroscopy as a measurement method for the wetting degree of lithium-ion cells. J Electrochem Soc 165(14):A3249–A3256. https://doi.org/10.1149/2.0081814jes

  9. 9.

    Xie Y, Zou H, Xiang H et al (2016) Enhancement on the wettability of lithium battery separator toward nonaqueous electrolytes. J Membr Sci 503:25–30. https://doi.org/10.1016/j.memsci.2015.12.025

  10. 10.

    Sheng Y, Fell CR, Son YK et al (2014) Effect of calendering on electrode wettability in lithium-ion batteries. Front Energy Res. https://doi.org/10.3389/fenrg.2014.00056

  11. 11.

    Jeon H, Yeon D, Lee T et al (2016) A water-based Al2O3 ceramic coating for polyethylene-based microporous separators for lithium-ion batteries. J Power Sources 315:161–168. https://doi.org/10.1016/j.jpowsour.2016.03.037

  12. 12.

    Kim SW, Ryou M-H, Lee YM et al (2016) Effect of liquid oil additive on lithium-ion battery ceramic composite separator prepared with an aqueous coating solution. J Alloys Compd 675:341–347. https://doi.org/10.1016/j.jallcom.2016.03.135

  13. 13.

    Yang P, Zhang P, Shi C et al (2015) The functional separator coated with core–shell structured silica–poly(methyl methacrylate) sub-microspheres for lithium-ion batteries. J Membr Sci 474:148–155. https://doi.org/10.1016/j.memsci.2014.09.047

  14. 14.

    Huang X, Hitt J (2013) Lithium-ion battery separators: development and performance characterization of a composite membrane. J Membr Sci 425–426:163–168. https://doi.org/10.1016/j.memsci.2012.09.027

  15. 15.

    Man C, Jiang P, Wong K-W et al (2014) Enhanced wetting properties of a polypropylene separator for a lithium-ion battery by hyperthermal hydrogen induced cross-linking of poly(ethylene oxide). J Mater Chem A 2(30):11980. https://doi.org/10.1039/C4TA01870B

  16. 16.

    Juang R-S, Liang C-H, Ma W-C et al (2014) Low-pressure ethane/nitrogen gas mixture plasma surface modification effect on the wetting and electrochemical performance of polymeric separator for lithium-ion batteries. J Taiwan Inst Chem Eng 45(6):3046–3051. https://doi.org/10.1016/j.jtice.2014.08.023

  17. 17.

    Pfleging W, Pröll J (2014) A new approach for rapid electrolyte wetting in tape cast electrodes for lithium-ion batteries. J Mater Chem A 2(36):14918. https://doi.org/10.1039/c4ta02353f

  18. 18.

    Cai J, Yu B (2011) A discussion of the effect of tortuosity on the capillary imbibition in porous media. Transp Porous Med 89(2):251–263. https://doi.org/10.1007/s11242-011-9767-0

  19. 19.

    Martic G, Coninck J de, Blake TD (2003) Influence of the dynamic contact angle on the characterization of porous media. J Colloid Interface Sci 263(1):213–216. https://doi.org/10.1016/S0021-9797(03)00283-2

  20. 20.

    Novák P, Joho F, Lanz M et al (2001) The complex electrochemistry of graphite electrodes in lithium-ion batteries. J Power Sources 97–98:39–46. https://doi.org/10.1016/S0378-7753(01)00586-9

  21. 21.

    Zhang S, Ding MS, Xu K et al (2001) Understanding solid electrolyte interface film formation on graphite electrodes. Electrochem Solid-State Lett 4(12):A206

  22. 22.

    Verma P, Maire P, Novák P (2010) A review of the features and analyses of the solid electrolyte interphase in Li-ion batteries. Electrochim Acta 55(22):6332–6341. https://doi.org/10.1016/j.electacta.2010.05.072

  23. 23.

    Tang M, Lu S, Newman J (2012) Experimental and theoretical investigation of solid-electrolyte-interphase formation mechanisms on glassy carbon. J Electrochem Soc 159(11):A1775–A1785. https://doi.org/10.1149/2.025211jes

  24. 24.

    Dougassa YR, Jacquemin J, El Ouatani L et al (2014) Viscosity and carbon dioxide solubility for LiPF6, LiTFSI, and LiFAP in alkyl carbonates: lithium salt nature and concentration effect. J Phys Chem B 118(14):3973–3980

  25. 25.

    Sachs W, Meyn V (1995) Pressure and temperature dependence of the surface tension in the system natural gas/water principles of investigation and the first precise experimental data for pure methane/water at 25 °C up to 46.8 MPa. Colloids Surf A 94(2–3): 291–301. https://doi.org/10.1016/0927-7757(94)03008-1

  26. 26.

    Ghatee MH, Zare M, Zolghadr AR et al (2010) Temperature dependence of viscosity and relation with the surface tension of ionic liquids. Fluid Phase Equilib 291(2):188–194. https://doi.org/10.1016/j.fluid.2010.01.010

  27. 27.

    Bernardin JD, Mudawar I, Walsh CB et al (1997) Contact angle temperature dependence for water droplets on practical aluminum surfaces. Int J Heat Mass Transf 40(5):1017–1033. https://doi.org/10.1016/0017-9310(96)00184-6

  28. 28.

    Petke FD, Ray BR (1969) Temperature dependence of contact angles of liquids on polymeric solids. J Colloid Interface Sci 31(2):216–227. https://doi.org/10.1016/0021-9797(69)90329-4

  29. 29.

    Neumann AW (1974) Contact angles and their temperature dependence: thermodynamic status, measurement, interpretation and application. Adv Colloid Interface Sci 4(2–3):105–191. https://doi.org/10.1016/0001-8686(74)85001-3

  30. 30.

    Zhmud T (2000) Dynamics of capillary rise. J Colloid Interface Sci 228(2):263–269. https://doi.org/10.1006/jcis.2000.6951

  31. 31.

    Fries N, Dreyer M (2008) An analytic solution of capillary rise restrained by gravity. J Colloid Interface Sci 320(1):259–263. https://doi.org/10.1016/j.jcis.2008.01.009

  32. 32.

    Cai J, Hu X, Standnes DC et al (2012) An analytical model for spontaneous imbibition in fractal porous media including gravity. Colloids Surf A 414:228–233. https://doi.org/10.1016/j.colsurfa.2012.08.047

  33. 33.

    Shin W-K, Kim D-W (2013) High performance ceramic-coated separators prepared with lithium ion-containing SiO2 particles for lithium-ion batteries. J Power Sources 226:54–60. https://doi.org/10.1016/j.jpowsour.2012.10.082

  34. 34.

    Dahbi M, Violleau D, Ghamouss F et al (2012) Interfacial properties of LiTFSI and LiPF 6 -based electrolytes in binary and ternary mixtures of alkylcarbonates on graphite electrodes and celgard separator. Ind Eng Chem Res 51(14):5240–5245. https://doi.org/10.1021/ie203066x

  35. 35.

    Sheng Y (2015) Investigation of electrolyte wetting in lithium ion batteries: effects of electrode pore structures and solution, Theses and Dissertations. https://dc.uwm.edu/etd/1080

  36. 36.

    Beyer S, Kobsch O, Pospiech D, Simon F, Peter C, Nikolowski K, Wolter M, Voit B (2019) Influence of surface characteristics on the penetration rate of electrolytes into model cells for lithium-ion batteries. J Adhes Sci Technol. https://doi.org/10.1080/01694243.2019.1686831

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The authors thank the German Federal Ministry for Economic Affairs and Energy BMWi (Bundesministerium für Wirtschaft und Energie) for financial support for the project 'Optilyt' (18380 BR/1) within the framework of the 'Co-operative Industrial Research' initiative IGF (Industrielle Gemeinschaftsforschung). Furthermore, the authors thank Beate Capraro, Stefan Börner and Adrian Goldberg for providing the modified electrodes.

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Correspondence to Sebastian Reuber.

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Peter, C., Nikolowski, K., Reuber, S. et al. Chronoamperometry as an electrochemical in situ approach to investigate the electrolyte wetting process of lithium-ion cells. J Appl Electrochem 50, 295–309 (2020). https://doi.org/10.1007/s10800-019-01383-2

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  • Lithium-ion battery
  • Electrolyte wetting
  • Lucas-Washburn
  • Wettability
  • Chronoamperometry