Influence of the PON4- structural units on the formation energies and transport properties of lithium phosphorus oxynitride: a DFT study. 2021

Pascal Henkel, and Jürgen Janek, and Doreen Mollenhauer
Institute of Physical Chemistry, Justus-Liebig University Giessen, 35392 Giessen, Germany. doreen.mollenhauer@phys.chemie.uni-giessen.de.

The potential of mobile applications for digital networking is constantly increasing. A key challenge is to ensure a reliable and long-term power supply. One possible solution is the use of all-solid-state thin-film lithium batteries which use amorphous lithium phosphorus oxynitride (LIPON) as solid electrolyte. It is well known that the electrochemical properties of this material are related to the amorphous state, which correlates with the nitrogen content. Due to the difficulty of calculating amorphous structures using first principles methods, three different LIPON structure models are considered in this study and the influence of the anion PON4- sublattice on the Li vacancy and Li interstitial formation as well as on the lithium ion transport is highlighted. While for all three model systems the migration energies of the energetically preferred Li vacancies increase with increasing complexity of the anion PON4- sublattice only slightly from 0.38 eV to 0.55 eV, the migration energies for the energetically preferred Li interstitials decrease with increasing complexity of the anion PON4- sublattice from 0.68 eV to 0.38 eV. Thus, it was found that the energetically preferred lithium ion (Li vacancy and Li interstitial ion) transport mechanism in LIPON can be explained on the basis of the present PON4- structural units. In the presence of isolated PON3 tetrahedra or periodic PO2N2 chains, the lithium vacancy diffusion dominates, whereas in the presence of periodic PON4- planes, the lithium interstitial diffusion becomes dominant.

UI MeSH Term Description Entries

Related Publications

Pascal Henkel, and Jürgen Janek, and Doreen Mollenhauer
November 2022, Chemical communications (Cambridge, England),
Pascal Henkel, and Jürgen Janek, and Doreen Mollenhauer
December 2020, Data in brief,
Pascal Henkel, and Jürgen Janek, and Doreen Mollenhauer
September 2018, Journal of the American Chemical Society,
Pascal Henkel, and Jürgen Janek, and Doreen Mollenhauer
August 2019, Scientific reports,
Pascal Henkel, and Jürgen Janek, and Doreen Mollenhauer
September 2019, Physical chemistry chemical physics : PCCP,
Pascal Henkel, and Jürgen Janek, and Doreen Mollenhauer
October 2012, Inorganic chemistry,
Pascal Henkel, and Jürgen Janek, and Doreen Mollenhauer
January 2015, Dalton transactions (Cambridge, England : 2003),
Pascal Henkel, and Jürgen Janek, and Doreen Mollenhauer
August 1990, Applied optics,
Pascal Henkel, and Jürgen Janek, and Doreen Mollenhauer
November 2021, Journal of fluorescence,
Copied contents to your clipboard!