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Carbon–carbon supercapacitors: Beyond the average pore size or how electrolyte confinement and inaccessible pores affect the capacitance

Lahrar, El Hassane and Simon, Patrice and Merlet, Céline Carbon–carbon supercapacitors: Beyond the average pore size or how electrolyte confinement and inaccessible pores affect the capacitance. (2021) Journal of Chemical Physics, 155 (18). 184703. ISSN 0021-9606

(Document in English)

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Official URL: https://doi.org/10.1063/5.0065150


Carbon–carbon supercapacitors are high power electrochemical energy storage systems, which store energy through reversible ion adsorption at the electrode–electrolyte interface. Due to the complex structure of the porous carbons used as electrodes, extracting structure–property relationships in these systems remains a challenge. In this work, we conduct molecular simulations of two model supercapacitors based on nanoporous electrodes with the same average pore size, a property often used when comparing porous materials, but different morphologies. We show that the carbon with the more ordered structure, and a well defined pore size, has a much higher capacitance than the carbon with the more disordered structure and a broader pore size distribution. We analyze the structure of the confined electrolyte and show that the ions adsorbed in the ordered carbon are present in larger quantities and are also more confined than for the disordered carbon. Both aspects favor a better charge separation and thus a larger capacitance. In addition, the disordered electrodes contain a significant amount of carbon atoms, which are never in contact with the electrolyte, carry a close to zero charge, and are thus not involved in the charge storage. The total quantities of adsorbed ions and degrees of confinement do not change much with the applied potential, and as such, this work opens the door to computationally tractable screening strategies.

Item Type:Article
Audience (journal):International peer-reviewed journal
Institution:French research institutions > Centre National de la Recherche Scientifique - CNRS (FRANCE)
Other partners > Collège de France (FRANCE)
Other partners > Ecole Nationale Supérieure de Chimie de Paris - ENSCP (FRANCE)
Other partners > Ecole Nationale Supérieure de Chimie de Montpellier - ENSCM (FRANCE)
Université de Toulouse > Institut National Polytechnique de Toulouse - Toulouse INP (FRANCE)
Other partners > Institut polytechnique de Grenoble (FRANCE)
Other partners > Université Paris Sciences & Lettres - PSL (FRANCE)
Other partners > Sorbonne Université (FRANCE)
Other partners > Université Grenoble Alpes - UGA (FRANCE)
Université de Toulouse > Université Toulouse III - Paul Sabatier - UT3 (FRANCE)
Other partners > Université de Nantes (FRANCE)
Other partners > Université de Picardie Jules Verne (FRANCE)
Other partners > Université de Pau et des Pays de l'Adour - UPPA (FRANCE)
Other partners > Université de Haute Alsace - UHA (FRANCE)
Other partners > Université de Montpellier (FRANCE)
Laboratory name:
Deposited On:22 Nov 2021 13:51

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