Sicolo, Sabrina ; Fingerle, Mathias ; Hausbrand, René ; Albe, Karsten (2017)
Interfacial instability of amorphous LiPON against lithium: A combined Density Functional Theory and spectroscopic study.
In: Journal of Power Sources, 354
doi: 10.1016/j.jpowsour.2017.04.005
Artikel, Bibliographie
Kurzbeschreibung (Abstract)
The chemical instability of the glassy solid electrolyte LiPON against metallic lithium and the occurrence of side reactions at their interface is investigated by combining a surface science approach and quantum-mechanical calculations. Using an evolutionary structure search followed by a melt-quenching protocol, a model for the disordered structure of LiPON is generated and put into contact with lithium. Even the static optimization of a simple model interface suggests that the diffusion of lithium into LiPON is driven by a considerable driving force that could easily take place under experimental conditions. Calculated reaction energies indicate that the reduction and decomposition of LiPON is thermodynamically favorable. By monitoring the evolution of the LiPON core levels as a function of lithium exposure, the disruption of the LiPON network alongside the occurrence of new phases is observed. The direct comparison between UV photoelectron spectroscopy measurements and calculated electronic densities of states for increasing stages of lithiation univocally identifies the new phases as Li_2O, Li_3P and Li_3N. These products are stable against Li metal and form a passivation layer which shields the electrolyte from further decomposition while allowing for the diffusion of Li ions.
Interfacial instability of amorphous LiPON against lithium: A combined Density Functional Theory and spectroscopic study. Available from: https://www.researchgate.net/publication/316112203_Interfacial_instability_of_amorphous_LiPON_against_lithium_A_combined_Density_Functional_Theory_and_spectroscopic_study [accessed May 16, 2017].
| Typ des Eintrags: | Artikel |
|---|---|
| Erschienen: | 2017 |
| Autor(en): | Sicolo, Sabrina ; Fingerle, Mathias ; Hausbrand, René ; Albe, Karsten |
| Art des Eintrags: | Bibliographie |
| Titel: | Interfacial instability of amorphous LiPON against lithium: A combined Density Functional Theory and spectroscopic study |
| Sprache: | Englisch |
| Publikationsjahr: | 14 April 2017 |
| Titel der Zeitschrift, Zeitung oder Schriftenreihe: | Journal of Power Sources |
| Jahrgang/Volume einer Zeitschrift: | 354 |
| DOI: | 10.1016/j.jpowsour.2017.04.005 |
| Kurzbeschreibung (Abstract): | The chemical instability of the glassy solid electrolyte LiPON against metallic lithium and the occurrence of side reactions at their interface is investigated by combining a surface science approach and quantum-mechanical calculations. Using an evolutionary structure search followed by a melt-quenching protocol, a model for the disordered structure of LiPON is generated and put into contact with lithium. Even the static optimization of a simple model interface suggests that the diffusion of lithium into LiPON is driven by a considerable driving force that could easily take place under experimental conditions. Calculated reaction energies indicate that the reduction and decomposition of LiPON is thermodynamically favorable. By monitoring the evolution of the LiPON core levels as a function of lithium exposure, the disruption of the LiPON network alongside the occurrence of new phases is observed. The direct comparison between UV photoelectron spectroscopy measurements and calculated electronic densities of states for increasing stages of lithiation univocally identifies the new phases as Li_2O, Li_3P and Li_3N. These products are stable against Li metal and form a passivation layer which shields the electrolyte from further decomposition while allowing for the diffusion of Li ions. Interfacial instability of amorphous LiPON against lithium: A combined Density Functional Theory and spectroscopic study. Available from: https://www.researchgate.net/publication/316112203_Interfacial_instability_of_amorphous_LiPON_against_lithium_A_combined_Density_Functional_Theory_and_spectroscopic_study [accessed May 16, 2017]. |
| Freie Schlagworte: | Density Functional Theory; Electrolyte; Interface; Li-ion batteries; LiPON; Spectroscopy |
| Fachbereich(e)/-gebiet(e): | 11 Fachbereich Material- und Geowissenschaften 11 Fachbereich Material- und Geowissenschaften > Materialwissenschaft 11 Fachbereich Material- und Geowissenschaften > Materialwissenschaft > Fachgebiet Materialmodellierung 11 Fachbereich Material- und Geowissenschaften > Materialwissenschaft > Fachgebiet Oberflächenforschung Zentrale Einrichtungen Zentrale Einrichtungen > Hochschulrechenzentrum (HRZ) Zentrale Einrichtungen > Hochschulrechenzentrum (HRZ) > Hochleistungsrechner |
| Hinterlegungsdatum: | 16 Mai 2017 09:13 |
| Letzte Änderung: | 09 Okt 2017 10:02 |
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