The failure mechanism of nano-sized Si-based negative electrodes for lithium ion batteries
- 23 March 2011
- journal article
- research article
- Published by Royal Society of Chemistry (RSC) in Journal of Materials Chemistry
- Vol. 21 (17), 6201-6208
- https://doi.org/10.1039/c1jm10213c
Abstract
Understanding the failure mechanism of silicon based negative electrodes for lithium ion batteries is essential for solving the problem of low coulombic efficiency and capacity fading on cycling and to further implement this new very energetic material in commercial cells. To reach this goal, several techniques are used here: post mortem7Li MAS NMR and SEM, electrochemical impedance spectroscopy (EIS) and three-electrode-based electrochemical analysis. 7Li MAS NMR analyses of the charged batteries demonstrate that the major part of the lithium lost during the charge of batteries is not trapped in LixSi alloys but instead at the surface of the Si particles, likely as a degradation product of the liquid electrolyte. Observed by SEM, a dead electrode has a thick “SEI” layer at its surface. EIS and incremental capacity analyses demonstrate that the growth of this layer is responsible for the failure of the electrode through a continuous decrease of its active surface area associated with a rise of the electrode polarization. It is demonstrated that the main cause of capacity fade of Si-based negative electrodes is the liquid electrolyte degradation in the case of nano Si-particles formulated with the carboxymethyl cellulose (CMC) binder. This degradation results in the formation of a blocking layer on the active mass, which further inhibits lithium diffusion through the composite electrode.Keywords
This publication has 30 references indexed in Scilit:
- A review of the electrochemical performance of alloy anodes for lithium-ion batteriesJournal of Power Sources, 2011
- Interfacial structural stabilization on amorphous silicon anode for improved cycling performance in lithium-ion batteriesElectrochimica Acta, 2010
- Effect of electrochemical conditions on the performance worsening of Si/C composite anodes for lithium batteriesElectrochimica Acta, 2010
- Key Parameters Governing the Reversibility of Si/Carbon/CMC Electrodes for Li-Ion BatteriesChemistry of Materials, 2009
- On the activation and charge transfer kinetics of evaporated silicon electrode/electrolyte interfacesElectrochimica Acta, 2009
- Silicon Composite Electrode with High Capacity and Long Cycle LifeElectrochemical and Solid-State Letters, 2009
- Hierarchical and Resilient Conductive Network of Bridged Carbon Nanotubes and Nanofibers for High-Energy Si Negative ElectrodesElectrochemical and Solid-State Letters, 2009
- Nano- and bulk-silicon-based insertion anodes for lithium-ion secondary cellsJournal of Power Sources, 2007
- Failure Modes of Silicon Powder Negative Electrode in Lithium Secondary BatteriesElectrochemical and Solid-State Letters, 2004
- Colossal Reversible Volume Changes in Lithium AlloysElectrochemical and Solid-State Letters, 2001