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Evaluating temperature dependent degradation mechanisms of silicon-graphite electrodes and the effect of fluoroethylene carbonate electrolyte additive

Journal Article · · Electrochimica Acta
 [1];  [1];  [1];  [2];  [1]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
+ Show Author Affiliations
Understanding and overcoming the relatively high rate of degradation observed with silicon (Si)-based anodes in lithium (Li)-ion batteries (LiBs) is crucial for developing cells with increased energy density. The capacity fade of Si-graphite (Gr) electrodes in electrolytes with and without 10 wt% fluoroethylene carbonate (FEC) is explored during cycling at temperatures of 25, 45, and 70 °C, focusing on the complex degradation modes arising from loss of active material, loss of Li inventory, and cell resistance growth. We first show the common half-cell testing cannot be used at elevated temperatures as the performance of Li metal overshadows the behavior of Si-Gr electrode. Symmetric cell configuration successfully eliminates the effect of foreign materials, and reveals that while the presence of FEC provides better passivation of Si, it also results in greater parasitic reactions at 70 °C and faster capacity fade. The electrolyte without FEC, on the other hand, shows higher capacity retention at 70 °C. Finally, we propose a multi-step test protocol which can successfully deconvolute the information on loss of Li inventory and of active material. By combining half-cell and symmetric cell test methods, we demonstrate that loss of active material is reduced at higher temperatures and the dominant mechanisms of capacity loss for Si-Gr electrodes at elevated temperatures is loss of Li inventory.
Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States); National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Sponsoring Organization:
USDOE; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office
Grant/Contract Number:
AC02-06CH11357; AC36-08GO28308
OSTI ID:
1818882
Alternate ID(s):
OSTI ID: 1820502
OSTI ID: 1845874
Report Number(s):
NREL/JA--5K00-78263; MainId:32180; UUID:d857b2a8-661f-4712-97ad-ba01b673476f; MainAdminID:60655
Journal Information:
Electrochimica Acta, Journal Name: Electrochimica Acta Vol. 394; ISSN 0013-4686
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

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Related Subjects

25 ENERGY STORAGE
Degradation mechanism
Electrochemical analysis
Fluoroethylene carbonate
Lithium-ion battery
Silicon-graphite anode
Silicon-graphite electrodes
Temperature