- Title
- Unraveling the multivalent aluminium-ion redox mechanism in 3,4,9,10-perylenetetracarboxylic dianhydride (PTCDA)†
- Creator
- Canever, Nicolò; Nann, Thomas
- Relation
- Physical Chemistry Chemical Physics Vol. 24, Issue 10, p. 5886-5893
- Publisher Link
- http://dx.doi.org/10.1039/d1cp05716b
- Publisher
- Royal Society of Chemistry
- Resource Type
- journal article
- Date
- 2022
- Description
- Rechargeable Aluminium-organic batteries are an exciting emerging energy storage technology owing to their low cost and promising high performance, thanks to the ability to allow multiple-electron redox chemistry and multivalent Al-ion intercalation. In this work, we use a combination of Density Functional Theory (DFT) calculations and experimental methods to examine the mechanism behind the charge–discharge reaction of the organic dye 3,4,9,10-perylenetetracarboxylic dianhydride (PTCDA) in the 1,3-ethylmethylimidazolium (EMIm+) chloroaluminate electrolyte. We conclude that, contrary to previous reports claiming the intercalation of trivalent Al3+, the actual ionic species involved in the redox reaction is the divalent AlCl2+. While a less-than-ideal scenario, this mechanism still allows a theoretical transfer of four electrons per formula unit, corresponding to a remarkable specific capacity of 273 mA h g−1. However, the poor reversibility of the reaction and low cycle life of the PTCDA-based cathode, due to its solubility in the electrolyte, make it an unlikely candidate for a commercial application.
- Subject
- aluminium-ion batteries; energy storage; organic cathodes; perylenetetracarboxylic dianhydride (PTCDA)
- Identifier
- http://hdl.handle.net/1959.13/1469392
- Identifier
- uon:48227
- Identifier
- ISSN:1463-9076
- Rights
- x
- Language
- eng
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