Rohrer, Jochen and Vrankovic, Dragoljub and Cupid, Damian and Riedel, Ralf and Seifert, Hans J. and Albe, Karsten and Graczyk-Zajac, Magdalena (2017):
Si- and Sn-containing SiOCN-based nanocomposites as anode materials for lithium ion batteries: synthesis, thermodynamic characterization and modeling.
In: International Journal of Materials Research, 108 (11), pp. 920-932. Carl Hanser Verlag GmbH & Co. KG, ISSN 1862-5282,
DOI: 10.3139/146.111517,
[Article]

Abstract

Novel nanocomposites consisting of silicon/tin nanoparticles (n-Si/n-Sn) embedded in silicon carbonitride (SiCN) or silicon oxycarbide (SiOC) ceramic matrices are investigated as possible anode materials for Li-ion batteries. The goal of our study is to exploit the large mass specific capacity of Si/Sn (3 579 mAh g−1/994 mAh g−1), while avoiding rapid capacity fading due to the large volume changes of Si/Sn during Li insertion. We show that a large amount (∼30–40 wt.%) of disordered carbon phase is dispersed within the SiOC/SiCN matrix and stabilizes the Si/Sn nanoparticles with respect to extended reversible lithium ion storage. Silicon nanocomposites are prepared by mixing of a polymeric precursor with commercial and “home-synthesized” crystalline and amorphous silicon. Tin nanocomposites, in contrast, are prepared using a single precursor approach, which allows the in-situ generation of Sn nanoparticles homogeneously dispersed within the SiOC host. The best electrochemical stability along with capacities of 600 – 700 mAh g−1 is obtained when amorphous/porous silicon is used. Mechanisms contributing to the increase of storage capacity and the cycle stability are clarified by analyzing elemental composition, local solid-state structures, intercalation hosts and Li-ion mobility. Our work is supplemented by first-principles based atomistic modeling and thermochemical measurements.

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