Evaluation of the electrochemical and expansion performances of the Sn-Si/graphite composite electrode for the industrial use

Abstract

The future development of lithium-ion batteries for electric vehicles requires significantly higher energy density and this is largely dependent on the application of novel active materials with high specific capacity. Recently, Sn-Si hybrid materials have been shown to exhibit both high specific capacity and good cycle stability. In practice, Sn-Si materials are mixed with graphite to form composite anodes to further improve the stability. However, detailed investigations of Sn-Si/graphite anodes are scarce. This study examines the electrochemical and expansion performance of Sn-Si/graphite anodes and features a morphological, structural and chemical analysis. The percolation and lattice expansion models are shown to fit well for the capacity and expansion evolution law of the composite anodes, respectively, as a function of Sn-Si hybrid content. Based on a comparison with a conventional graphite anode, efficient Sn-Si/graphite composite anodes could be formed that achieve a high reversible capacity (450 mAh g^-1), a promising 1st Coulombic efficiency (75%) and stable cycling (cycling coulombic efficiency > 98%), thereby making them some of the most promising Sn-based anodes for industrial applications.

Keywords

Lithium-ion batteries / Sn-Si-C composite anode / anode expansion modelling / capacity retention modelling / industrial application

References

[1] Marom R,Leifer N,Aurbach D.A review of advanced and practical lithium battery materials.J Mater Chem2011;21:9938

[2] Zhang W.A review of the electrochemical performance of alloy anodes for lithium-ion batteries.J Power Sources2011;196:13-24

[3] Tao W,You Y.Strategies for improving the storage performance of silicon-based anodes in lithium-ion batteries.Nano Res2019;12:1739-49

[4] Whiteley JM,Kang CS,Oh KH.Tin networked electrode providing enhanced volumetric capacity and pressureless operation for all-solid-state Li-ion batteries.J Electrochem Soc2015;162:A711-5

[5] Whiteley JM,Piper DM.High-capacity and highly reversible silicon-tin hybrid anode for solid-state lithium-ion batteries.J Electrochem Soc2015;163:A251-4

[6] Courtney IA.Electrochemical and in situ X-ray diffraction studies of the reaction of lithium with tin oxide composites.J Electrochem Soc1997;144:2045-52

[7] Yan Y,Zhan Y.Nano-Sn embedded in expanded graphite as anode for lithium ion batteries with improved low temperature electrochemical performance.Electrochimica Acta2016;187:186-92

[8] Jin Z,Yu H,Huang X.A facile method to synthesize 3D structured Sn anode material with excellent electrochemical performance for lithium-ion batteries.Prog Nat Sci Mater Int2020;30:456-60

[9] Kierzek K,Béguin F.Towards the realistic silicon/carbon composite for Li-ion secondary battery anode.J Appl Electrochem2015;45:1-10

[10] Otero M,Leiva EPM,Friedrich A.Design-considerations regarding silicon/graphite and tin/graphite composite electrodes for lithium-ion batteries.Sci Rep2018;8:15851 PMCID:PMC6203704

[11] Wang G,Lindsay M.Graphite-Tin composites as anode materials for lithium-ion batteries.J Power Sources2001;97-98:211-5

[12] Wang G,Ahn J,Dou S.Electrochemical properties of nanosize Sn-coated graphite anodes in lithium-ion cells.J Appl Electrochem2004;34:187-90

[13] Fang T,Duh J.A novel composite negative electrode consist of multiphase Sn compounds and mesophase graphite powders for lithium ion batteries.J Power Sources2006;160:536-41

[14] Guo B,Tang K,Wang Z.Nano-Sn/hard carbon composite anode material with high-initial coulombic efficiency.J Power Sources2008;177:205-10

[15] Pol VG,Miller DJ.Sonochemical deposition of Sn, SnO₂ and Sb on spherical hard carbon electrodes for Li-Ion batteries.J Electrochem Soc2014;161:A777-82

[16] Shao Y,Grosseau P,Beneventi D.Use of lignocellulosic materials and 3D printing for the development of structured monolithic carbon materials.Compos. Part B Eng2018;149:206-15

[17] Mo R,Li F.Tin-graphene tubes as anodes for lithium-ion batteries with high volumetric and gravimetric energy densities.Nat Commun2020;11:1374 PMCID:PMC7069972

[18] Ding S,Zhang L.Organic molecule confinement reaction for preparation of the Sn nanoparticles@graphene anode materials in Lithium-ion battery.J Colloid Interface Sci2021;589:308-17

[19] Nakai H,Kita A.Investigation of the solid electrolyte interphase formed by fluoroethylene carbonate on Si electrodes.J Electrochem Soc2011;158:A798-801

[20] Moulder JF,Sobol PE. Handbook of X-ray photoelectron spectroscopy. Minnesota: Perkin-Elmer Corporation; 1992.

[21] Shao Y,Grosseau P,Beneventi D.Biocarbons from microfibrillated cellulose/lignosulfonate precursors: a study of electrical conductivity development during slow pyrolysis.Carbon2018;129:357-66

[22] Zhang N.Dissecting anode swelling in commercial lithium-ion batteries.J Power Sources2012;218:52-5

[23] Kasavajjula U,Appleby AJ.Nano- and bulk-silicon-based insertion anodes for lithium-ion secondary cells.J Power Sources2007;163:1003-39

[24] Kalnaus S,Daniel C.A study of lithium ion intercalation induced fracture of silicon particles used as anode material in Li-ion battery.J Power Sources2011;196:8116-24

[25] Schiele A,Mazilkin A.Silicon nanoparticles with a polymer-derived carbon shell for improved lithium-ion batteries: Investigation into volume expansion, gas evolution, and particle fracture.ACS Omega2018;3:16706-13 PMCID:PMC6643814

[26] Kobayashi N,Endo M.Silicon/soft-carbon nanohybrid material with low expansion for high capacity and long cycle life lithium-ion battery.J Power Sources2016;326:235-41

[27] Sheng Y,Son YK,Jiang J.Effect of calendering on electrode wettability in lithium-ion batteries.Front Energy Res2014;2:56

[28] Lu X,Bertei A.Microstructural evolution of battery electrodes during calendering.Joule2020;4:2746-68

[29] Lu X,Finegan DP.3D microstructure design of lithium-ion battery electrodes assisted by X-ray nano-computed tomography and modelling.Nat Commun2020;11:2079 PMCID:PMC7190643

[30] Moon J,Jung H.Interplay between electrochemical reactions and mechanical responses in silicon-graphite anodes and its impact on degradation.Nat Commun2021;12:2714 PMCID:PMC8113583

[31] Courtney IA,Mao O,Dahn JR.Ab initio calculation of the lithium-tin voltage profile.Phys Rev B1998;58:15583-8

[32] Im HS,Lim YR.Phase evolution of tin nanocrystals in lithium ion batteries.ACS Nano2013;7:11103-11

[33] Wu R,Zheng Y.Unveiling the intrinsic reaction between silicon-graphite composite anode and ionic liquid electrolyte in lithium-ion battery.J Power Sources2020;473:228481

[34] Limthongkul P,Dudney NJ.Electrochemically-driven solid-state amorphization in lithium-metal anodes.J Power Sources2003;119-121:604-9

[35] Forney MW,Staub JW,Landi BJ.Prelithiation of silicon-carbon nanotube anodes for lithium ion batteries by stabilized lithium metal powder (SLMP).Nano Lett2013;13:4158-63

[36] Chen L,Meng Y.Integrated structure of tin-based anodes enhancing high power density and long cycle life for lithium ion batteries.ACS Appl Energy Mater2020;3:9337-47