Reinold, Lukas Mirko (2016)
SiCN based Anode Materials for Lithium-Ion Batteries.
Technische Universität Darmstadt
Ph.D. Thesis, Primary publication
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Item Type: | Ph.D. Thesis | ||||
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Type of entry: | Primary publication | ||||
Title: | SiCN based Anode Materials for Lithium-Ion Batteries | ||||
Language: | English | ||||
Referees: | Riedel, Prof. Dr. Ralf ; Roth, Prof. Dr. Christina | ||||
Date: | 2016 | ||||
Place of Publication: | Darmstadt | ||||
Date of oral examination: | 23 December 2015 | ||||
Abstract: | This thesis deals with the investigation of polymer-derived silicon carbonitride based anode materials for their application in lithium-ion batteries. Carbon-rich silicon carbonitrides are obtained by a pyrolysis of different organosilicon precursors, namely poly(phenylvinylsilylcarbodiimide), poly(phenylvinylsilazane), poly(diphenylsilylcarbodiimide), poly(phenylsilsesquicarbodiimide) and poly(phenylsilsesquiazane). The materials are characterized by means of Raman spectroscopy, elemental analysis, X-ray diffraction and Galvanostatic Cycling with Potential Limitation. Promising results with respect to the capacity, rate capability and cycling stability have been obtained. Namely, silicon carbonitride derived from poly(phenylvinylsilazane) exhibits a 1st cycle specific delithiation capacity as high as 725 mAh/g and a specific capacity of 624 mAh/g after prolonged cycling. Extensive studies on the influence of the pyrolysis temperature between 800 °C and 1300 °C on the electrochemical behavior have been performed on the active materials derived from poly(phenylvinylsilylcarbodiimide) and poly(phenylvinylsilazane). It has been found that the pyrolysis temperature influences the hysteresis, the specific capacity, the rate capability and several aspects related to the stability of the prepared electrodes. Single Particle Measurements have been conducted, giving insight into the intrinsic properties of the materials, namely the charge transfer resistance and the minimum diffusion coefficient. These values are found to depend on the pyrolysis temperature, too. Solid state 29Si, 13C and 7Li Nuclear Magnetic Resonance measurements on poly(phenylvinylsilylcarbodiimide) and poly(phenylvinylsilazane) pyrolyzed at 1100 °C reveal that the free carbon phase acts as major storing site for the lithium ions and that lithium ion motion takes place via a continuum diffusion mechanism described by an activation law. Moreover, the prospects of silicon carbonitride as stabilizing matrix for prolonged electrochemical cycling of silicon nano powders are addressed. A variety of composites have been prepared differing in the organosilicon precursor, the ratios of compounds, presence/absence of conductive coatings and geometric structure. The highest cycling stability has been achieved for silicon nano particles located in a porous ceramic matrix. |
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URN: | urn:nbn:de:tuda-tuprints-54285 | ||||
Classification DDC: | 500 Science and mathematics > 500 Science 500 Science and mathematics > 530 Physics 500 Science and mathematics > 540 Chemistry 600 Technology, medicine, applied sciences > 620 Engineering and machine engineering |
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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 |
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Date Deposited: | 30 May 2016 10:02 | ||||
Last Modified: | 09 Jul 2020 01:17 | ||||
URI: | https://tuprints.ulb.tu-darmstadt.de/id/eprint/5428 | ||||
PPN: | 380971232 | ||||
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