Quantifying capacity loss due to solid-electrolyte-interphase layer formation on silicon negative electrodes in lithium-ion batteries

• Published in: Journal of power sources Vol. 215; pp. 145 - 151
• Main Authors: Nadimpalli, Siva P.V., Sethuraman, Vijay A., Dalavi, Swapnil, Lucht, Brett, Chon, Michael J., Shenoy, Vivek B., Guduru, Pradeep R.
• Format: Journal Article
• Language: English
• Published: Amsterdam Elsevier B.V 01-10-2012; Elsevier
• Subjects: Applied sciences; Capacity loss; Direct energy conversion and energy accumulation; Electrical engineering. Electrical power engineering; Electrical power engineering; Electrochemical conversion: primary and secondary batteries, fuel cells; Exact sciences and technology; Lithium-ion battery; Si anode; Solid-electrolyte-interphase (SEI) layer; X-ray photoelectron spectroscopy (XPS); Capacity loss; Lithium-ion battery; Si anode; X-ray photoelectron spectroscopy (XPS); Solid-electrolyte-interphase (SEI) layer; Amorphous material; Anode; Alkaline storage battery; Solid electrolyte; Thin film; Lithiation; Photoelectron spectrometry; Silicon; Interphase; Cracking; Secondary cell; Experimental study; Lithium battery; Thickness; Crystalline material; Particle size distribution; Thin layer electrode; Surface area; Crack; X-ray photoelectron spectra; Planar technology
• ISSN: 0378-7753; 1873-2755
• DOI: 10.1016/j.jpowsour.2012.05.004

Charge lost per unit surface area of a silicon electrode due to the formation of solid-electrolyte-interphase (SEI) layer during initial lithiation was quantified, and the species that constitute this layer were identified. Coin cells made with Si thin-film electrodes were subjected to a combination of galvanostatic and potentiostatic lithiation and delithiation cycles to accurately measure the capacity lost to SEI layer formation. While the planar geometry of amorphous thin films allows accurate calculation of surface area, creation of additional surface by cracking was prevented by minimizing the thickness of the Si film. The cycled electrodes were analyzed with X-ray photoelectron spectroscopy to characterize the composition of the SEI layer. The charge lost due to SEI formation measured from coin cell experiments was found to be in good agreement with the first-cycle capacity loss during the initial lithiation of a Si(100) crystal with planar geometry. The methodology presented in this work is expected to provide a useful practical tool for battery-material developers in estimating the expected capacity loss due to first cycle SEI layer formation and in choosing an appropriate particle size distribution that balances mechanical integrity and the first cycle capacity loss in large volume expansion electrodes for lithium-ion batteries.
► A method to quantify capacity loss per unit area due to initial SEI formation on Si. ► Identify species that constitute the SEI layer. ► Reported data can be used to predict first-cycle capacity loss on any geometry.