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Carbon-rich SiCN ceramics as high capacity/high stability anode material for lithium-ion batteries

Reinold, Lukas Mirko and Graczyk-Zajac, Magdalena and Gao, Yan and Mera, Gabriela and Riedel, Ralf (2013):
Carbon-rich SiCN ceramics as high capacity/high stability anode material for lithium-ion batteries.
In: Journal of Power Sources, Elsevier Science Publishing, pp. 224-229, 236, ISSN 03787753,
[Online-Edition: http://dx.doi.org/10.1016/j.jpowsour.2013.02.046],
[Article]

Abstract

Two classes of preceramic polymers, namely polysilazane and polysilylcarbodiimide, with branched and linear molecular structure were pyrolyzed at 1100 °C under argon atmosphere. The resulting nanostructured polymer-derived SiCN ceramics were characterized by means of elemental analysis, X-ray diffraction, scanning electron microscopy and Raman spectroscopy. All investigated ceramics are amorphous and contain a disordered free carbon phase of 2–2.5 nm in size. Electrochemical characterization reveals that the polysilazane-derived electrodes demonstrate higher capacity and stability during subsequent lithium insertion/extraction with different currents than those of the polysilylcarbodiimide-based electrodes. The highest lithium extraction capacity of 724 mA h g−1 is recovered for the sample derived from branched polysilazane whereas the best polysilylcarbodiimide-derived sample recovers 612 mA h g−1. Moreover, the polysilazane-derived samples deliver a higher fraction of capacity recovered below 1.5 V. The electrochemical performance is found to be dependent on the molecular structure (silazane vs. silylcarbodiimide) of the preceramic polymer, while there is no effect associated with the amount of branching (silsesquiazane vs. silazane and silsesquicarbodiimide vs. silylcarbodiimide). The influence of “micropore activity” and oxygen content on the electrochemical performance of polymer-derived silicon carbonitrides is addressed.

Item Type: Article
Erschienen: 2013
Creators: Reinold, Lukas Mirko and Graczyk-Zajac, Magdalena and Gao, Yan and Mera, Gabriela and Riedel, Ralf
Title: Carbon-rich SiCN ceramics as high capacity/high stability anode material for lithium-ion batteries
Language: English
Abstract:

Two classes of preceramic polymers, namely polysilazane and polysilylcarbodiimide, with branched and linear molecular structure were pyrolyzed at 1100 °C under argon atmosphere. The resulting nanostructured polymer-derived SiCN ceramics were characterized by means of elemental analysis, X-ray diffraction, scanning electron microscopy and Raman spectroscopy. All investigated ceramics are amorphous and contain a disordered free carbon phase of 2–2.5 nm in size. Electrochemical characterization reveals that the polysilazane-derived electrodes demonstrate higher capacity and stability during subsequent lithium insertion/extraction with different currents than those of the polysilylcarbodiimide-based electrodes. The highest lithium extraction capacity of 724 mA h g−1 is recovered for the sample derived from branched polysilazane whereas the best polysilylcarbodiimide-derived sample recovers 612 mA h g−1. Moreover, the polysilazane-derived samples deliver a higher fraction of capacity recovered below 1.5 V. The electrochemical performance is found to be dependent on the molecular structure (silazane vs. silylcarbodiimide) of the preceramic polymer, while there is no effect associated with the amount of branching (silsesquiazane vs. silazane and silsesquicarbodiimide vs. silylcarbodiimide). The influence of “micropore activity” and oxygen content on the electrochemical performance of polymer-derived silicon carbonitrides is addressed.

Journal or Publication Title: Journal of Power Sources
Volume: 236
Publisher: Elsevier Science Publishing
Uncontrolled Keywords: Lithium-ion battery; Polymer-derived ceramic; Silicon carbonitride; Anode; Polysilazane; Polysilylcarbodiimide
Divisions: 11 Department of Materials and Earth Sciences
11 Department of Materials and Earth Sciences > Material Science > Dispersive Solids
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
11 Department of Materials and Earth Sciences > Material Science
Zentrale Einrichtungen
DFG-Collaborative Research Centres (incl. Transregio) > Collaborative Research Centres
DFG-Collaborative Research Centres (incl. Transregio)
Date Deposited: 04 Apr 2013 09:38
Official URL: http://dx.doi.org/10.1016/j.jpowsour.2013.02.046
Additional Information:

SFB 595 A4

Identification Number: doi:10.1016/j.jpowsour.2013.02.046
Funders: We gratefully acknowledge the financial support of the German Research Foundation (DFG) SPP1473, SFB 595/A4 and Materials World Network Program between DFG and National Science Foundation (NSF)., We gratefully acknowledge the grant funded under the LOEWE-Zentrum AdRIA by the state of Hesse, Germany, and the Fonds der Chemischen Industrie, Frankfurt, Germany.
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