title: Mechanism of Silicon Electrode Aging upon Cycling in Full Lithium-Ion Batteries.
abstract: Understanding the aging mechanism of silicon-based negative electrodes for lithium-ion batteries upon cycling is essential to solve the problem of low coulombic efficiency and capacity fading and further to implement this new high-capacity material in commercial cells. Nevertheless, such studies have so far focused on half cells in which silicon is cycled versus an infinite reservoir of lithium. In the present work, the aging mechanism of silicon-based electrodes is studied upon cycling in a full Li-ion cell configuration with LiCoO2 as the positive electrode. Postmortem analyses of both electrodes clearly indicate that neither one of them contains lithium and that no discernible degradation results from the cycling. The aging mechanism can be explained by the reduction of solvent molecules. Electrons extracted from the positive electrode are responsible for an internal imbalance in the cell, which results in progressive slippage of the electrodes and reduces the compositional range of cyclable lithium ions for both electrodes.
authors.affiliation: Institut des Matériaux Jean Rouxel, IMN, Université de Nantes, CNRS, 2 rue de la Houssinière, BP 32229, 44322, Nantes Cedex 3, France.
authors.forename: Nathalie
authors.initials: N
authors.lastname: Delpuech
authors.affiliation: Institut des Matériaux Jean Rouxel, IMN, Université de Nantes, CNRS, 2 rue de la Houssinière, BP 32229, 44322, Nantes Cedex 3, France. nicolas.dupre@cnrs-imn.fr.
authors.forename: Nicolas
authors.initials: N
authors.lastname: Dupre
authors.affiliation: Institut des Matériaux Jean Rouxel, IMN, Université de Nantes, CNRS, 2 rue de la Houssinière, BP 32229, 44322, Nantes Cedex 3, France.
authors.forename: Philippe
authors.initials: P
authors.lastname: Moreau
authors.affiliation: Umicore Group Research & Development, Kasteelstraat 7, Olen, Belgium.
authors.forename: Jean-Sebastian
authors.initials: JS
authors.lastname: Bridel
authors.affiliation: Institut des Matériaux Jean Rouxel, IMN, Université de Nantes, CNRS, 2 rue de la Houssinière, BP 32229, 44322, Nantes Cedex 3, France.
authors.forename: Joel
authors.initials: J
authors.lastname: Gaubicher
authors.affiliation: Institut des Matériaux Jean Rouxel, IMN, Université de Nantes, CNRS, 2 rue de la Houssinière, BP 32229, 44322, Nantes Cedex 3, France.
authors.forename: Bernard
authors.initials: B
authors.lastname: Lestriez
authors.affiliation: Institut des Matériaux Jean Rouxel, IMN, Université de Nantes, CNRS, 2 rue de la Houssinière, BP 32229, 44322, Nantes Cedex 3, France.
authors.forename: Dominique
authors.initials: D
authors.lastname: Guyomard
mesh_terms: D003035:Cobalt / Q000737:chemistry*; D011211:Electric Power Supplies; D004566:Electrodes; D008094:Lithium / Q000737:chemistry*; D010087:Oxides / Q000737:chemistry*; D012825:Silicon / Q000737:chemistry*
chemical_list: D010087:Oxides; C491691:lithium cobalt oxide; D003035:Cobalt; D008094:Lithium; D012825:Silicon
keywords: Li-ion cells; NMR spectroscopy; reaction mechanisms; silicon; solid-electrolyte interphase