Journal
JOURNAL OF POWER SOURCES
Volume 253, Issue -, Pages 342-348Publisher
ELSEVIER SCIENCE BV
DOI: 10.1016/j.jpowsour.2013.12.065
Keywords
Nuclear magnetic resonance (NMR); Li-7 dynamics; Anode; Lithium-ion battery; Silicon carbonitride; Polymer-derived ceramic
Funding
- DFG [GR3330/3-1, GR 4440/1-2, SFB 595/A4]
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We report Li-7, Si-29, and C-13 NMR studies of two different carbon-rich SiCN ceramics SiCN-1 and SiCN-3 derived from the preceramic polymers polyphenylvinylsilylcarbodiimide and polyphenylvinylsilazane, respectively. From the spectral analysis of the three nuclei, we find that only the C-13 spectrum is strongly influenced by Li insertion/extraction, suggesting that carbon phases are the major electrochemically active sites for Li storage. Temperature (T) and Larmor frequency (omega(L)) dependences of the Li-7 linewidth and spin-lattice relaxation rates T-1(-1) are described by an activated law with the activation energy E-A of 0.31 eV and the correlation time tau(0) in the high temperature limit of 1.3 ps. The 3/2 power law dependence of T-1(-1) on omega(L) which deviates from the standard Bloembergen, Purcell, and Pound (BPP) model implies that the Li motion on the mu s timescale is governed by continuum diffusion mechanism rather than jump diffusion. On the other hand, the rotating frame relaxation rate T-1 rho(-1) results suggest that the slow motion of Li on the ms timescale may be affected by complex diffusion and/or non-diffusion processes. (C) 2013 Elsevier B.V. All rights reserved.
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