Issue 9, 2023

The impact of electrode conductivity on electrolyte interfacial structuring and its implications on the Na0/+ electrochemical performance

Abstract

Molecular and ionic assemblies at electrode/liquid electrolyte interfaces, i.e., the electric double layer (EDL), define battery performance by directing the formation of stable interphases. An unstable interphase can hamper metal-cation diffusion, lead to continuous electrolyte consumption, and also promote non-uniform electrochemical processes like dendrite formation. The co-selection of electrolyte chemistry and initial cycling conditions together are generally considered for the design of desirable interphases. At the same time, the dielectric nature of the electrode material is largely ignored, notwithstanding the high unreliability of the assumption that the nature of the EDL and the mechanism of the interphase formation at metallic and semiconductive electrodes are identical. Here we show that the dielectric nature of the charged electrode greatly affects the interfacial metal–anion–solvent composition; therefore, different interphase chemistry will be formed, suggesting different initial cycling conditions need to be established on a case-by-case basis to form the desired interphase. This phenomenon correlates with the metal ion solvation chemistry and the adsorption of species at the electrified electrode due to the competition of van der Waals and coulombic interactions.

Graphical abstract: The impact of electrode conductivity on electrolyte interfacial structuring and its implications on the Na0/+ electrochemical performance

Supplementary files

Article information

Article type
Paper
Submitted
18 mar 2023
Accepted
14 iyl 2023
First published
19 iyl 2023

Energy Environ. Sci., 2023,16, 3919-3931

The impact of electrode conductivity on electrolyte interfacial structuring and its implications on the Na0/+ electrochemical performance

D. A. Rakov, J. Sun, P. V. Cherepanov, K. Arano, P. C. Howlett, A. N. Simonov, F. Chen and M. Forsyth, Energy Environ. Sci., 2023, 16, 3919 DOI: 10.1039/D3EE00864A

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