Issue 14, 2015

Adsorption of insoluble polysulfides Li2Sx (x = 1, 2) on Li2S surfaces

Abstract

In lithium–sulfur batteries, the growth of insulating discharge product Li2S film affects the cathode microstructure and the related electron as well as lithium ion transport properties. In this study, chemical reactions of insoluble lithium polysulfides Li2Sx (x = 1, 2) on crystal Li2S substrate are investigated by a first-principles approach. First-principles atomistic thermodynamics predicts that the stoichiometric (111) and (110) surfaces are stable around the operating cell voltage. Li2Sx adsorption is an exothermic reaction with the (110) surface being more active to react with the polysulfides than the stoichiometric (111) surface. There is no obvious charge transfer between the adsorbed molecule and the crystal Li2S substrate. Analysis of the charge density difference suggests that the adsorbate interacts with the substrate via a strong covalent bond. The growth mechanism of thermodynamically stable surfaces is investigated in the present study. It is found that direct Li2S deposition is energetically favored over Li2S2 deposition and reduction process.

Graphical abstract: Adsorption of insoluble polysulfides Li2Sx (x = 1, 2) on Li2S surfaces

Article information

Article type
Paper
Submitted
30 Dec 2014
Accepted
03 Mar 2015
First published
03 Mar 2015

Phys. Chem. Chem. Phys., 2015,17, 9032-9039

Adsorption of insoluble polysulfides Li2Sx (x = 1, 2) on Li2S surfaces

Z. Liu, D. Hubble, P. B. Balbuena and P. P. Mukherjee, Phys. Chem. Chem. Phys., 2015, 17, 9032 DOI: 10.1039/C4CP06118G

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