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Lithium dynamics in carbon-rich polymer-derived SiCN ceramics probed by nuclear magnetic resonance

Baek, Seung-Ho and Reinold, Lukas Mirko and Graczyk-Zajac, Magdalena and Riedel, Ralf and Hammerath, Franziska and Büchner, Bernd and Grafe, Hans-Joachim (2014):
Lithium dynamics in carbon-rich polymer-derived SiCN ceramics probed by nuclear magnetic resonance.
In: Journal of Power Sources, Elsevier Science Publishing, pp. 342-348, 253, ISSN 03787753,
[Online-Edition: http://dx.doi.org/10.1016/j.jpowsour.2013.12.065],
[Article]

Abstract

We report 7Li, 29Si, and 13C 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 13C 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 (ωL) dependences of the 7Li linewidth and spin-lattice relaxation rates View the MathML source are described by an activated law with the activation energy EA of 0.31 eV and the correlation time τ0 in the high temperature limit of 1.3 ps. The 3/2 power law dependence of View the MathML source on ωL which deviates from the standard Bloembergen, Purcell, and Pound (BPP) model implies that the Li motion on the μs timescale is governed by continuum diffusion mechanism rather than jump diffusion. On the other hand, the rotating frame relaxation rate View the MathML source results suggest that the slow motion of Li on the ms timescale may be affected by complex diffusion and/or non-diffusion processes.

Item Type: Article
Erschienen: 2014
Creators: Baek, Seung-Ho and Reinold, Lukas Mirko and Graczyk-Zajac, Magdalena and Riedel, Ralf and Hammerath, Franziska and Büchner, Bernd and Grafe, Hans-Joachim
Title: Lithium dynamics in carbon-rich polymer-derived SiCN ceramics probed by nuclear magnetic resonance
Language: English
Abstract:

We report 7Li, 29Si, and 13C 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 13C 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 (ωL) dependences of the 7Li linewidth and spin-lattice relaxation rates View the MathML source are described by an activated law with the activation energy EA of 0.31 eV and the correlation time τ0 in the high temperature limit of 1.3 ps. The 3/2 power law dependence of View the MathML source on ωL which deviates from the standard Bloembergen, Purcell, and Pound (BPP) model implies that the Li motion on the μs timescale is governed by continuum diffusion mechanism rather than jump diffusion. On the other hand, the rotating frame relaxation rate View the MathML source results suggest that the slow motion of Li on the ms timescale may be affected by complex diffusion and/or non-diffusion processes.

Journal or Publication Title: Journal of Power Sources
Volume: 253
Publisher: Elsevier Science Publishing
Uncontrolled Keywords: Nuclear magnetic resonance (NMR); 7Li dynamics; Anode; Lithium-ion battery; Silicon carbonitride; Polymer-derived ceramic
Divisions: 11 Department of Materials and Earth Sciences
11 Department of Materials and Earth Sciences > Material Science
11 Department of Materials and Earth Sciences > Material Science > Dispersive Solids
DFG-Collaborative Research Centres (incl. Transregio)
DFG-Collaborative Research Centres (incl. Transregio) > Collaborative Research Centres
Zentrale Einrichtungen
DFG-Collaborative Research Centres (incl. Transregio) > Collaborative Research Centres > CRC 595: Electrical fatigue
DFG-Collaborative Research Centres (incl. Transregio) > Collaborative Research Centres > CRC 595: Electrical fatigue > A - Synthesis
DFG-Collaborative Research Centres (incl. Transregio) > Collaborative Research Centres > CRC 595: Electrical fatigue > A - Synthesis > Subproject A4: Novel functional ceramics using anionic substitution in oxidic systems
Date Deposited: 08 Jan 2014 09:57
Official URL: http://dx.doi.org/10.1016/j.jpowsour.2013.12.065
Additional Information:

SFB 595 A4

Identification Number: doi:10.1016/j.jpowsour.2013.12.065
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