Issue 12, 2024

Exploring carbon electrode parameters in Li–O2 cells: Li2O2 and Li2CO3 formation

Abstract

Ensuring the stability of the electrode and electrolyte in Li–O2 batteries and achieving a comprehensive understanding of parasitic side reaction management during cycling are key issues for the progress of this promising energy storage technology. Conditions that favour formation of either Li2O2 or Li2CO3 in Li–O2 cells on carbon-based electrodes were investigated. Operando Raman microscopy measurements and ex situ Raman and X-ray photoelectron spectroscopy (XPS) analyses were performed for Li–O2 systems using Li[ClO4]/DMSO as the electrolyte and carbon paper (CP) and carbon paper with carbon nanotubes (CPCNT) as electrodes. Using CP electrodes (either treated or untreated with O2 plasma), the major discharge product formed was Li2O2. In contrast, for CPCNT electrodes, the formation of Li2CO3 as the main discharge product was observed at lower capacities, then significant formation of Li2O2 proceeded at higher discharge capacities. XPS highlighted that the surface chemistry of the CPCNT electrode comprised fluorine and a variety of iron species, which could be linked to the promotion of Li2CO3 formation. Furthermore, it was observed that when Li2CO3 is the main discharge product, the active sites of functional groups on carbon surfaces that favour carbonate formation become coated/passivated. Consequently, the dominant reaction pathway then alters, leading to the growth of Li2O2 over the surface. These outcomes emphasized the important role in cycling stability of the active sites on carbon electrodes, arising from the synthesis process or possible contaminants.

Graphical abstract: Exploring carbon electrode parameters in Li–O2 cells: Li2O2 and Li2CO3 formation

Supplementary files

Article information

Article type
Paper
Submitted
12 Dec. 2023
Accepted
08 Febr. 2024
First published
21 Febr. 2024

J. Mater. Chem. A, 2024,12, 7215-7226

Exploring carbon electrode parameters in Li–O2 cells: Li2O2 and Li2CO3 formation

B. P. Sousa, C. G. Anchieta, T. M. C. Nepel, A. R. Neale, L. J. Hardwick, R. M. Filho and G. Doubek, J. Mater. Chem. A, 2024, 12, 7215 DOI: 10.1039/D3TA07701B

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