期刊
ADVANCED FUNCTIONAL MATERIALS
卷 -, 期 -, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.202303667
关键词
bilayer solid-electrolyte interphase; fluorinated solvents; high-energy-density batteries; localized high-concentration electrolytes; Si microparticle anodes
Si microparticle (SiMP) anodes have lower production cost and higher tap density than their nanosized counterparts, but suffer from particle pulverization during cycling. A non-flammable localized high-concentration electrolyte (LHCE) is formulated using a fluorinated solvent to form a stable solid-electrolyte interphase on the SiMP anode, enabling stable cycling with high Coulombic efficiency. This LHCE also provides unprecedented cycling stability for high-energy-density batteries containing SiMP anodes and high-capacity cathodes.
Si microparticle (SiMP) anodes feature much lower production cost and higher tap density compared to their nanosized counterparts, which hold great promise for high-energy-density lithium-ion batteries, yet they suffer from unavoidable particle pulverization during repeated cycling, thus making their practical application extremely challenging. Herein, a non-flammable localized high-concentration electrolyte (LHCE) is rationally formulated using a fluorinated solvent, 2,2,2-trifluoroethyl methyl carbonate (FEMC), to induce fluorinated solvent-coupled anion-derived interfacial chemistry. Unlike other LHCEs, the FEMC-based LHCE is demonstrated to build a highly robust and stable F-rich inorganic-organic bilayer solid-electrolyte interphase on SiMP anode, which endows stable cycling of SiMP anode (approximate to 3.4 mAh cm(-2)) with an ultrahigh Coulombic efficiency of approximate to 99.7%. Coupled with its high anodic stability, the FEMC-based LHCE endows unprecedented cycling stability for high-energy-density batteries containing high-capacity SiMP anodes with Ni-rich LiNi8Mn1Co1O2 or 5 V-class LiNi0.5Mn1.5O4 cathodes. Remarkably, a 1.0 Ah-level SiMP||LiNi8Mn1Co1O2 pouch-cell stably operates for more than 200 cycles, representing the pioneering report in pouch cells containing SiMP anodes.
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