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- Solvation and Dynamics of Lithium Ions in Carbonate-Based Electrolytes during Cycling Followed by Operando Infrared Spectroscopy: The Example of NiSb 2 , a Typical Negative Conversion-Type Electrode Material for Lithium Batteries doi link

Auteur(s): Marino Cyril, Boulaoued Athmane, Fullenwarth Julien, Maurin D., Louvain Nicolas, Bantignies J.-L., Stievano Lorenzo, Monconduit Laure

(Article) Publié: The Journal Of Physical Chemistry C, vol. 121 p.26598 - 26606 (2017)


Ref HAL: hal-01661243_v1
DOI: 10.1021/acs.jpcc.7b06685
WoS: 000417671500003
Exporter : BibTex | endNote
14 Citations
Résumé:

Conversion-type electrode materials show extremely interesting performance in terms of capacity, which is however usually associated with bad Coulombic efficiency. The latter is mainly the consequence of the relentless evolution of solid electrolyte interphase (SEI) formed and/or dissolved during conversion/back-conversion reactions on the continuously reshaping active material surface. The thorough comprehension of the dynamic processes occurring during cycling in a working electrochemical cell, such as solvation/desolvation of ionic species and formation/dissolution of the SEI at the electrode/electrolyte interface, is thus of utmost relevance in the study of electrochemical mechanism and performance of conversion-type electrode materials. Operando Fourier transform infrared (FTIR) spectroscopy, one of the methods of choice for the study of such phenomena, was applied to study the dynamic interfacial properties of NiSb2, a representative intermetallic conversion-type electrode material for Li batteries, during cycling in the presence of a commercial electrolyte based on LiPF6 dissolved in a mixture of ethylene carbonate (EC) and dimethyl carbonate (DMC). Using a specifically developed in situ ATR-IR electrochemical cell, it was possible to correlate the electrochemical processes to the ratio between solvent molecules associated with Li+ ions and free solvent molecules and thus to follow the dynamic evolution of the concentration of lithium in the electrolyte during cycling.