Graczyk-Zajac, Magdalena ; Reinold, Lukas ; Kaspar, Jan ; Sasikumar, Pradeep ; Soraru, Gian-Domenico ; Riedel, Ralf (2015)
New Insights into Understanding Irreversible and Reversible Lithium Storage within SiOC and SiCN Ceramics.
In: Nanomaterials, 5 (1)
doi: 10.3390/nano5010233
Artikel, Bibliographie
Kurzbeschreibung (Abstract)
Within this work we define structural properties of the silicon carbonitride (SiCN) and silicon oxycarbide (SiOC) ceramics which determine the reversible and irreversible lithium storage capacities, long cycling stability and define the major differences in the lithium storage in SiCN and SiOC. For both ceramics, we correlate the first cycle lithiation or delithiation capacity and cycling stability with the amount of SiCN/SiOC matrix or free carbon phase, respectively. The first cycle lithiation and delithiation capacities of SiOC materials do not depend on the amount of free carbon, while for SiCN the capacity increases with the amount of carbon to reach a threshold value at ~50% of carbon phase. Replacing oxygen with nitrogen renders the mixed bond Si-tetrahedra unable to sequester lithium. Lithium is more attracted by oxygen in the SiOC network due to the more ionic character of Si-O bonds. This brings about very high initial lithiation capacities, even at low carbon content. If oxygen is replaced by nitrogen, the ceramic network becomes less attractive for lithium ions due to the more covalent character of Si-N bonds and lower electron density on the nitrogen atom. This explains the significant difference in electrochemical behavior which is observed for carbon-poor SiCN and SiOC materials.
| Typ des Eintrags: | Artikel |
|---|---|
| Erschienen: | 2015 |
| Autor(en): | Graczyk-Zajac, Magdalena ; Reinold, Lukas ; Kaspar, Jan ; Sasikumar, Pradeep ; Soraru, Gian-Domenico ; Riedel, Ralf |
| Art des Eintrags: | Bibliographie |
| Titel: | New Insights into Understanding Irreversible and Reversible Lithium Storage within SiOC and SiCN Ceramics |
| Sprache: | Englisch |
| Publikationsjahr: | 24 Februar 2015 |
| Verlag: | MDPI AG, Schweiz |
| Titel der Zeitschrift, Zeitung oder Schriftenreihe: | Nanomaterials |
| Jahrgang/Volume einer Zeitschrift: | 5 |
| (Heft-)Nummer: | 1 |
| DOI: | 10.3390/nano5010233 |
| Kurzbeschreibung (Abstract): | Within this work we define structural properties of the silicon carbonitride (SiCN) and silicon oxycarbide (SiOC) ceramics which determine the reversible and irreversible lithium storage capacities, long cycling stability and define the major differences in the lithium storage in SiCN and SiOC. For both ceramics, we correlate the first cycle lithiation or delithiation capacity and cycling stability with the amount of SiCN/SiOC matrix or free carbon phase, respectively. The first cycle lithiation and delithiation capacities of SiOC materials do not depend on the amount of free carbon, while for SiCN the capacity increases with the amount of carbon to reach a threshold value at ~50% of carbon phase. Replacing oxygen with nitrogen renders the mixed bond Si-tetrahedra unable to sequester lithium. Lithium is more attracted by oxygen in the SiOC network due to the more ionic character of Si-O bonds. This brings about very high initial lithiation capacities, even at low carbon content. If oxygen is replaced by nitrogen, the ceramic network becomes less attractive for lithium ions due to the more covalent character of Si-N bonds and lower electron density on the nitrogen atom. This explains the significant difference in electrochemical behavior which is observed for carbon-poor SiCN and SiOC materials. |
| Zusätzliche Informationen: | SFB 595 A4 This article belongs to the Special Issue Ceramic Nanocomposites: Design Concepts towards Tailor-Made (Multi)Functionality and Prospective Energy-Related Applications |
| Fachbereich(e)/-gebiet(e): | 11 Fachbereich Material- und Geowissenschaften > Materialwissenschaft > Fachgebiet Disperse Feststoffe DFG-Sonderforschungsbereiche (inkl. Transregio) > Sonderforschungsbereiche > SFB 595: Elektrische Ermüdung > A - Synthese > Teilprojekt A4: Neue Funktionskeramiken durch Anionensubstitution in oxidischen Systemen 11 Fachbereich Material- und Geowissenschaften > Materialwissenschaft DFG-Sonderforschungsbereiche (inkl. Transregio) > Sonderforschungsbereiche > SFB 595: Elektrische Ermüdung > A - Synthese DFG-Sonderforschungsbereiche (inkl. Transregio) > Sonderforschungsbereiche > SFB 595: Elektrische Ermüdung 11 Fachbereich Material- und Geowissenschaften Zentrale Einrichtungen DFG-Sonderforschungsbereiche (inkl. Transregio) > Sonderforschungsbereiche DFG-Sonderforschungsbereiche (inkl. Transregio) |
| Hinterlegungsdatum: | 26 Feb 2015 09:35 |
| Letzte Änderung: | 27 Feb 2015 10:42 |
| PPN: | |
| Sponsoren: | Financial support from the German Research Foundation within SFB 595/A4 and SPP 1473/JP8 programs is greatly acknowledged., Ralf Riedel, Gian-Domenico Soraru and Pradeep Vallachira Warriam Sasikumaracknowledge the financial support from the EU through the Marie Curie ITN 7th Framework Programme, Functional Nitrides for Energy Applications (MC INT FUNEA), CT-264873. |
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