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Influence of the ionic coordination on the cathode reaction mechanisms of Al/S batteries

Influence of the ionic coordination on the cathode reaction mechanisms of Al/S batteries
Influence of the ionic coordination on the cathode reaction mechanisms of Al/S batteries
The lack of knowledge on electrochemical reaction pathways for Al/S batteries prevents the development of practical approaches to mitigate the irreversibility and poor cycling performances of this appealing secondary battery system, which is, in theory, scalable, inexpensive, and energy-dense. Different from the Li/S system, Al/S batteries use ionic liquids (ILs) as electrolytes. The choice of the IL, i.e., whether the IL is based on a conventional EMImCl-based electrolyte or in a deep eutectic mixture of aluminum chloride with urea (or any of its derivatives), strongly affects the electrochemical energy-storage performance of the cell. To shed some light on the Al/S battery chemistry, here, we present the computational electrochemistry research work to determine the most favorable reaction pathways and thermodynamically stable reaction intermediates. We also discuss the effect of the coordination of ionic species (originated from aluminum-containing deep eutectic electrolytes) with polysulfide intermediates, which lead to alterations in the reaction pathway and electrochemical behavior of the Al/S system. The spectroscopic signatures from various reaction intermediates are also reported and validated via comparison with experimental observations.
1932-7447
40-47
Bhowmik, Arghya
44e54375-dacb-4663-8f13-03def848f8e9
Carrasco-Busturia, David
13cc0d0f-6db3-4879-8571-453b46c491fe
Jankowski, Piotr
3341f3e1-5b73-4612-92c2-161f7a01734e
Raccichini, Rinaldo
7f943ecf-6b1b-4e4a-b222-8f3c27e679df
Garcia-Araez, Nuria
9358a0f9-309c-495e-b6bf-da985ad81c37
García-Lastra, Juan María
28dee415-d7d6-473f-a847-3becfc683c1e
Bhowmik, Arghya
44e54375-dacb-4663-8f13-03def848f8e9
Carrasco-Busturia, David
13cc0d0f-6db3-4879-8571-453b46c491fe
Jankowski, Piotr
3341f3e1-5b73-4612-92c2-161f7a01734e
Raccichini, Rinaldo
7f943ecf-6b1b-4e4a-b222-8f3c27e679df
Garcia-Araez, Nuria
9358a0f9-309c-495e-b6bf-da985ad81c37
García-Lastra, Juan María
28dee415-d7d6-473f-a847-3becfc683c1e

Bhowmik, Arghya, Carrasco-Busturia, David, Jankowski, Piotr, Raccichini, Rinaldo, Garcia-Araez, Nuria and García-Lastra, Juan María (2022) Influence of the ionic coordination on the cathode reaction mechanisms of Al/S batteries. The Journal of Physical Chemistry C, 126 (1), 40-47. (doi:10.1021/acs.jpcc.1c08426).

Record type: Article

Abstract

The lack of knowledge on electrochemical reaction pathways for Al/S batteries prevents the development of practical approaches to mitigate the irreversibility and poor cycling performances of this appealing secondary battery system, which is, in theory, scalable, inexpensive, and energy-dense. Different from the Li/S system, Al/S batteries use ionic liquids (ILs) as electrolytes. The choice of the IL, i.e., whether the IL is based on a conventional EMImCl-based electrolyte or in a deep eutectic mixture of aluminum chloride with urea (or any of its derivatives), strongly affects the electrochemical energy-storage performance of the cell. To shed some light on the Al/S battery chemistry, here, we present the computational electrochemistry research work to determine the most favorable reaction pathways and thermodynamically stable reaction intermediates. We also discuss the effect of the coordination of ionic species (originated from aluminum-containing deep eutectic electrolytes) with polysulfide intermediates, which lead to alterations in the reaction pathway and electrochemical behavior of the Al/S system. The spectroscopic signatures from various reaction intermediates are also reported and validated via comparison with experimental observations.

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AL-S battery-path-R1-clean - Accepted Manuscript
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Accepted/In Press date: 16 December 2021
e-pub ahead of print date: 5 January 2022

Identifiers

Local EPrints ID: 454907
URI: http://eprints.soton.ac.uk/id/eprint/454907
ISSN: 1932-7447
PURE UUID: 5c327cd0-9048-4cd4-bdc9-f70f50cfb94a
ORCID for Nuria Garcia-Araez: ORCID iD orcid.org/0000-0001-9095-2379

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Date deposited: 01 Mar 2022 17:43
Last modified: 05 Jan 2023 05:01

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Contributors

Author: Arghya Bhowmik
Author: David Carrasco-Busturia
Author: Piotr Jankowski
Author: Rinaldo Raccichini
Author: Juan María García-Lastra

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