Sicolo, Sabrina ; Albe, Karsten (2016)
First-principles calculations on structure and properties of amorphous Li5P4O8N3 (LiPON).
In: Journal of Power Sources, 331
doi: 10.1016/j.jpowsour.2016.09.059
Artikel, Bibliographie
Kurzbeschreibung (Abstract)
The structural, electronic and ion transport properties of an amorphous member of the LiPON family with non-trivial composition and cross-linking are studied by means of electronic structure calculations within Density Functional Theory. By a combination of an evolutionary algorithm followed by simulated annealing and alternatively by a rapid quenching protocol, structural models of disordered Li5P4O8N3 are generated, which are characterized by a local demixing in Li-rich and Li-poor layers. These structures have a composition close to what is found experimentally in thin films and contain all the expected diversely coordinated atoms, namely triply- and doubly-coordinated nitrogens and bridging and non-bridging oxygens. The issue of ionic conductivity is addressed by calculating defect formation energies and migration barriers of neutral and charged point defects. Li+ interstitials are energetically much preferred over vacancies, both when the lithium reservoir is metallic lithium and LiCoO2. The competitive formation of neutral Li interstitials when LiPON is contacted with metallic Li results in the chemical reduction of LiPON and the disruption of the network, as recently observed in experiments.
| Typ des Eintrags: | Artikel |
|---|---|
| Erschienen: | 2016 |
| Autor(en): | Sicolo, Sabrina ; Albe, Karsten |
| Art des Eintrags: | Bibliographie |
| Titel: | First-principles calculations on structure and properties of amorphous Li5P4O8N3 (LiPON) |
| Sprache: | Englisch |
| Publikationsjahr: | 12 September 2016 |
| Titel der Zeitschrift, Zeitung oder Schriftenreihe: | Journal of Power Sources |
| Jahrgang/Volume einer Zeitschrift: | 331 |
| DOI: | 10.1016/j.jpowsour.2016.09.059 |
| Kurzbeschreibung (Abstract): | The structural, electronic and ion transport properties of an amorphous member of the LiPON family with non-trivial composition and cross-linking are studied by means of electronic structure calculations within Density Functional Theory. By a combination of an evolutionary algorithm followed by simulated annealing and alternatively by a rapid quenching protocol, structural models of disordered Li5P4O8N3 are generated, which are characterized by a local demixing in Li-rich and Li-poor layers. These structures have a composition close to what is found experimentally in thin films and contain all the expected diversely coordinated atoms, namely triply- and doubly-coordinated nitrogens and bridging and non-bridging oxygens. The issue of ionic conductivity is addressed by calculating defect formation energies and migration barriers of neutral and charged point defects. Li+ interstitials are energetically much preferred over vacancies, both when the lithium reservoir is metallic lithium and LiCoO2. The competitive formation of neutral Li interstitials when LiPON is contacted with metallic Li results in the chemical reduction of LiPON and the disruption of the network, as recently observed in experiments. |
| Freie Schlagworte: | DFT; Interfaces; Li-ion batteries; LiPON; Lithium phosphate glasses; Solid electrolytes |
| Zusätzliche Informationen: | SFB 595 |
| Fachbereich(e)/-gebiet(e): | 11 Fachbereich Material- und Geowissenschaften 11 Fachbereich Material- und Geowissenschaften > Materialwissenschaft 11 Fachbereich Material- und Geowissenschaften > Materialwissenschaft > Fachgebiet Materialmodellierung Zentrale Einrichtungen Zentrale Einrichtungen > Hochschulrechenzentrum (HRZ) Zentrale Einrichtungen > Hochschulrechenzentrum (HRZ) > Hochleistungsrechner |
| Hinterlegungsdatum: | 29 Sep 2016 11:54 |
| Letzte Änderung: | 16 Sep 2018 21:26 |
| PPN: | |
| Sponsoren: | This work has been financially supported by the DFG center of excellence 595, “Electrical Fatigue in Functional Materials” and DFG project AL-578/19-1. The authors gratefully acknowledge the computing time granted by the Lichtenberg, High Performance Computer of TU Darmstadt. |
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