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Artificial Solid Electrolyte Interphase Formation on Si Nanoparticles through Radiolysis: Importance of the Presence of an Additive
journal contribution
posted on 2019-11-18, 20:36 authored by Chandra
S. Bongu, Suzy Surblé, John P. Alper, Adrien Boulineau, Jean-Frédéric Martin, Alexandre Demarque, Pierre-Eugène Coulon, Michel Rosso, François Ozanam, Sylvain Franger, Nathalie Herlin-Boime, Sophie Le CaërIn the context of energy transition, irradiation is a
powerful
tool to mimic quickly the modification of electrode materials upon
charge/discharge cycles in lithium-ion batteries. In this study, the
evolution of the surface of silicon nanoparticles upon irradiation
in two electrolytes, containing or not fluoroethylene carbonate (FEC),
was studied. In the presence of FEC, irradiation leads to the formation
of a homogeneous layer of a few nanometers thick, covering the whole
surface of the nanoparticles. The formation of an artificial solid
electrolyte interphase (SEI) layer through radiolysis is thus achieved.
Without FEC, only patches of degradation products are formed on the
nanoparticle surfaces for the same irradiation dose. In the absence
of FEC, LixPFyOz salts are formed. In the presence
of FEC, LixPOy, LiF, and Si–F bonds are generated. In both cases, the interphase
contains Li2CO3 and a polymer containing ethylene
carbonate units. Slightly different polymers are formed at the surface
of nanoparticles in the presence or absence of FEC, i.e., more cross-linked
in the former case. The elastomeric properties of the polymer formed
in the presence of FEC are thought to be responsible for the formation
of the homogeneous layer on the Si surfaces, leading to the generation
of an artificial solid SEI through the radiolysis process. This SEI,
however, prevents the efficient transfer of Li+ ions, and
more work is required to optimize its intrinsic (electro)chemical
properties.
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Li x PO yirradiation doseethylene carbonate unitsradiolysis processSi surfacessilicon nanoparticleselectrolyte interphasefluoroethylene carbonateelastomeric propertiesformationElectrolyte Interphase Formationpresencedegradation productsSEIFECLi x PF y O z saltselectrode materialspolymernanoparticle surfacesenergy transitionLi 2 CO 3Si Nanoparticleslithium-ion batteries
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