Issue 46, 2014

The role of native defects in the transport of charge and mass and the decomposition of Li4BN3H10

Abstract

Li4BN3H10 is of great interest for hydrogen storage and for lithium-ion battery solid electrolytes because of its high hydrogen content and high lithium-ion conductivity, respectively. The practical hydrogen storage application of this complex hydride is, however, limited due to irreversibility and cogeneration of ammonia (NH3) during the decomposition. We report a first-principles density-functional theory study of native point defects and defect complexes in Li4BN3H10, and propose an atomistic mechanism for the material's decomposition that involves mass transport mediated by native defects. In light of this specific mechanism, we argue that the release of NH3 is associated with the formation and migration of negatively charged hydrogen vacancies inside the material, and it can be manipulated by the incorporation of suitable electrically active impurities. We also find that Li4BN3H10 is prone to Frenkel disorder on the Li sublattice; lithium vacancies and interstitials are highly mobile and play an important role in mass transport and ionic conduction.

Graphical abstract: The role of native defects in the transport of charge and mass and the decomposition of Li4BN3H10

Article information

Article type
Paper
Submitted
17 Aug 2014
Accepted
08 Oct 2014
First published
14 Oct 2014

Phys. Chem. Chem. Phys., 2014,16, 25314-25320

Author version available

The role of native defects in the transport of charge and mass and the decomposition of Li4BN3H10

K. Hoang, A. Janotti and C. G. Van de Walle, Phys. Chem. Chem. Phys., 2014, 16, 25314 DOI: 10.1039/C4CP03677H

To request permission to reproduce material from this article, please go to the Copyright Clearance Center request page.

If you are an author contributing to an RSC publication, you do not need to request permission provided correct acknowledgement is given.

If you are the author of this article, you do not need to request permission to reproduce figures and diagrams provided correct acknowledgement is given. If you want to reproduce the whole article in a third-party publication (excluding your thesis/dissertation for which permission is not required) please go to the Copyright Clearance Center request page.

Read more about how to correctly acknowledge RSC content.

Social activity

Spotlight

Advertisements