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Nanostructured Si-C Composites As High-Capacity Anode Material For All-Solid-State Lithium-Ion Batteries

: Poetke, Stephanie; Hippauf, Felix; Baasner, Anne; Dörfler, Susanne; Althues, Holger; Kaskel, Stefan

Fulltext ()

Inorganic Chemistry (2021), Online First, 12 pp.
ISSN: 0020-1669
ISSN: 1520-510X
Journal Article, Electronic Publication
Fraunhofer IWS ()
all solid state battery; balancing; nanostructure; silicon carbon composites; thiophosphate solid electrolyte

Silicon carbon void structures (Si-C) are attractive anode materials for Lithium-ion batteries to cope with the volume changes of silicon during cycling. In this study, Si-C with varying Si contents (28 ‑ 37 %) are evaluated in all-solid-state batteries (ASSBs) for the first time. The carbon matrix enables enhanced performance and lifetime of the Si-C composites compared to bare silicon nanoparticles in half-cells even at high loadings of up to 7.4 mAh cm-2. In full cells with nickel-rich NCM (LiNi0.9Co0.05Mn0.05O2, 210 mAh g-1), kinetic limitations in the anode lead to a lowered voltage plateau compared to NCM half-cells. The solid electrolyte (Li6PS5Cl, 3 mS cm-1) does not penetrate the Si-C void structure resulting in less side reactions and higher initial coulombic efficiency compared to a liquid electrolyte (72.7 % vs. 31.0 %). Investigating the influence of balancing of full cells using 3-electrode ASSB cells revealed a higher delithiation of the cathode as a result of the higher cut-off voltage of the anode at high n/p ratios. During galvanostatic cycling, full cells with either a low or rather high overbalancing of the anode showed the highest capacity retention of up to 87.7 % after 50 cycles.