Unraveling the multivalent aluminium-ion redox mechanism in 3,4,9,10-perylenetetracarboxylic dianhydride (PTCDA)

文献情報

出版日 2022-02-14

DOI 10.1039/D1CP05716B

インパクトファクター 3.676

著者

Nicolò Canever, Thomas Nann

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要旨

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.

掲載誌

Physical Chemistry Chemical Physics

CiteScore: 5.5

自己引用率: 10.3%

年間論文数: 3036

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