Abstract
A custom built reusable cell for in situ lithiation and mechanical deformation studies while in an X-ray tomograph was demonstrated, and the strain and volume changes of a composite graphite anode were computed from 3D X-ray microcomputed tomography data via Digital Volume Correlation (DVC). The test anode was a composite electrode comprised of a porous compliant matrix, graphite as the Li+ host material, 5-μm ZrO2 marker particles for use with DVC, and active carbon black to enhance electrical conductivity. The composite electrodes were hot-pressed to control their porosity, and in turn the mechanical integrity of the resulting material. This composite anode was included in a half-cell and lithiated in situ while in a tomograph, and intermittent 3D data were collected at different lithiation levels up to full gravimetric capacity. Strain measurements by DVC demonstrated relatively uniform expansion of the freestanding electrode with average normal strains in the three directions varying by 20%, while the internal shear strains were found to be negligible. The average experimental strains were about 75% of the theoretical value, as estimated by the rule of mixtures, which implies that ~25% of the normal strains in graphite, due to lithiation, are accommodated by the surrounding matrix.
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References
Tarascon J, Armand M (2001) Issues and challenges facing rechargeable lithium batteries. Nature 414:359–367
Scrosati B, Garche J (2010) Lithium batteries: status, prospects and future. J Power Sources 195(9):2419–2430
Wang GX, Ahn JH, Lindsay MJ, Sun L, Bradhurst DH, Dou SX, Liu HK (2001) Graphite-tin composites as anode materials for lithium-ion batteries. J Power Sources 98-98:211–215
Srinivasan V (2008) Batteries for vehicular applications. AIP conference proceedings 1044(1):283–296
Qi Y, Guo H, Hector LG, Timmons A (2010) Threefold increase in the young’s modulus of graphite negative electrode during lithium intercalation. J Electrochem Soc 157(5):A558
Kostecki R, McLarnon F (2003) Microprobe study of the effect of Li intercalation on the structure of graphite. J Power Sources 119-121:550–554
Markervich E, Salitra G, Levi MD, Aurbach D (2005) Capacity fading of lithiated graphite electrodes studied by a combination of electroanalytical methods, raman spectroscopy and SEM. J Power Sources 146(1-2):146–150
Chao S-C, Yen Y-C, Song Y-F, Chen Y-M, Wu H-C, Wu N-L (2010) A study on the interior microstructures of working Sn particle electrode of Li-ion batteries by in situ X-ray transmission microscopy. Electrochem Commun 12(2):234–237
Wilson JR, Cronin JS, Barnett SA, Harris SJ (2011) Measurement of three-dimensional microstructure in a LiCoO2 positive electrode. J Power Sources 196(7):3443–3447
Shearing PR, Brandon NP, Gelb J, Bradley R, Withers PJ, Marquis AJ, Cooper S, Harris SJ (2012) Multi length scale microstructural investigations of a commercially available Li-ion battery electrode. J Electrochem Soc 159(7):A1023–A1027
Shearing PR, Howard LE, Jergensen PS, Brandon NP, Harris SJ (2010) Characterization of the 3-dimensional microstructure of a graphite negative electrode from a Li-ion battery. Electrochem Commun 12(3):374–377
Ebner M, Marone F, Stampanoni M, Wood V (2013) Visualization and quantification of electrochemical and mechanical degradation in Li ion batteries. Science 342(6159):716–720
Ebner M, Geldmacher F, Marone F, Stampanoni M, Wood V (2013) X-ray tomography of porous, transition metal oxide based lithium ion battery electrodes. Adv Energy Mater 3(7):845–850
Eastwood DS, Yufit V, Gelb J, Gu A, Bradley RS, Harris SJ, Brett DJL, Brandon NP, Lee PD, Withers PJ, Shearing PR (2014) Lithiation-induced dilation map** in a lithium-ion battery electrode by 3D X-ray microscopy and digital volume correlation. Adv Energy Mater 4(1e7):1300506
Finegan DP, Tudisco E, Scheel M, Robinson JB, Taiwo OO, Eastwood DS, Lee PD, Michiel MD, Bay B, Hall S, Hinds G, Brett DJL, Shearing PR (2016) Quantifying bulk electrode strain and material displacement within lithium batteries via high-speed operando tomography and digital volume correlation. Adv Sci 3(1e11):1500332
Paz-Garcia JM, Taiwo OO, Tudisco E, Finegan DP, Shearing PR, Brett DJL, Hall SA (2016) 4D analysis of the microstructural evolution of Si-based electrodes during lithiation: time-lapse X-ray imaging and digital volume correlation. J Power Sources 320:196e203
Lee HH, Wang YY, Wan CC, Yang M-H, Wu H-C, Shieh D-T (2004) A fast formation process for lithium batteries. J Power Sources 134:118–123
An SJ, Li J, Daniel C, Mohanty D, Nagpure S, Wood DL III (2016) The state of understanding of the lithium-ion-battery graphite solid electrolyte interphase (SEI) and its relationship to formation cycling. Carbon 105:52–76
Gonzalez J, Lambros J (2016) A parametric study on the influence of internal speckle patterning for digital volume correlation in X-ray tomography applications. Exp Tech 40(5):1447–1459. https://doi.org/10.1007/s40799-016-0145-2
Antartis D, Dillon S, Chasiotis I (2015) Effect of porosity in electrochemical and mechanical properties of composite Li-ion anodes. J Compos Mater 49(15):1849–1862
Feldkamp LA, Davis LC, Kress JW (1984) Practical cone-beam algorithm. J Opt Soc Am 1(6):612–619
Limodin N, Réthoré J, Adrien J, Buffière JY, Hild F, Roux S (2010) Analysis and artifact correction for volume correlation measurements using tomographic images from a laboratory X-ray source. Exp Mech 51(6):959–970
Bay BK, Smith TS, Fyhrie DP, Saad M (1999) Digital volume correlation: three-dimensional strain map** using X-ray tomography. Exp Mech 39(3):217–226
Verhulp E, van Rietbergen B, Huiskes R (2004) A three-dimensional digital image correlation technique for strain measurements in microstructures. J Biomech 37(9):1313–1320
Bay BK (2008) Methods and applications of digital volume correlation. J Strain Anal Eng Des 43(8):745–760
Franck C, Hong S, Maskarinec SA, Tirrell DA, Ravichandran G (2007) Three-dimensional full-field measurements of large deformations in soft materials using confocal microscopy and digital volume correlation. Exp Mech 47(3):427–438
Germaneau A, Doumalin P, Dupre JC (2007) 3D strain field measurement by correlation of volume images using scattered light: recording of images and choice of marks. Strain 43:207–218
Germaneau A, Doumalin P, Dupré J-C (2008) Comparison between X-ray micro-computed tomography and optical scanning tomography for full 3D strain measurement by digital volume correlation. NDT&E Int 41(6):407–415
Gates M, Lambros J, Heath MT (2010) Towards high performance digital volume correlation. Exp Mech 51(4):491–507
Sutton MA, Orteu J-J, Schreir H (2009) Image correlation for shape, motion and deformation measurements: basic concepts, theory and applications. Springer, Berlin
Gates M, Heath MT, Lambros J (2015) High performance hybrid CPU and GPU parallel algorithm for digital volume correlation. Int J High Perform Comput Appl 29(1):92–106. https://doi.org/10.1177/1094342013518807
Kavan L, Attia A, Lenzmann F, Elder SH, Grätzel M (2000) Lithium insertion into zirconia-stabilized mesoscopic TiO2 (Anatase). J Electrochem Soc 147(8):2897–2902
Acknowledgments
This work was supported in part by the University of Illinois at Urbana Champaign Interdisciplinary Innovation Initiative (In3) Proposal Award #12027. Joseph Gonzalez also acknowledges that this material is based upon work supported by the National Science Foundation Graduate Research Fellowship under Grant No. DGE-1144245. Dimitris A. Antartis and Ioannis Chasiotis acknowledge the support by the Air Force Office for Scientific Research through Grants FA9550-12-1-0209 and FA9550-13-1-0149 with Dr. B.L. Lee as the program monitor.
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Gonzalez, J.F., Antartis, D.A., Martinez, M. et al. Three-Dimensional Study of Graphite-Composite Electrode Chemo-Mechanical Response using Digital Volume Correlation. Exp Mech 58, 573–583 (2018). https://doi.org/10.1007/s11340-018-0384-5
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DOI: https://doi.org/10.1007/s11340-018-0384-5