Cation desolvation-induced capacitance enhancement in reduced graphene oxide (rGO)

Kangkang Ge, Hui Shao, Encarnacion Raymundo-Piñero, Pierre-Louis Taberna () and Patrice Simon ()
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Kangkang Ge: Université Paul Sabatier, CIRIMAT UMR CNRS 5085
Hui Shao: i-Lab, CAS Center for Excellence in Nanoscience, Suzhou Institute of Nano-Tech and Nano-Bionics (SINANO), Chinese Academy of Sciences (CAS)
Encarnacion Raymundo-Piñero: Réseau sur le Stockage Electrochimique de l’Energie (RS2E)
Pierre-Louis Taberna: Université Paul Sabatier, CIRIMAT UMR CNRS 5085
Patrice Simon: Université Paul Sabatier, CIRIMAT UMR CNRS 5085

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract Understanding the local electrochemical processes is of key importance for efficient energy storage applications, including electrochemical double layer capacitors. In this work, we studied the charge storage mechanism of a model material - reduced graphene oxide (rGO) - in aqueous electrolyte using the combination of cavity micro-electrode, operando electrochemical quartz crystal microbalance (EQCM) and operando electrochemical dilatometry (ECD) tools. We evidence two regions with different charge storage mechanisms, depending on the cation-carbon interaction. Notably, under high cathodic polarization (region II), we report an important capacitance increase in Zn2+ containing electrolyte with minimum volume expansion, which is associated with Zn2+ desolvation resulting from strong electrostatic Zn2+-rGO interactions. These results highlight the significant role of ion-electrode interaction strength and cation desolvation in modulating the charging mechanisms, offering potential pathways for optimized capacitive energy storage. As a broader perspective, understanding confined electrochemical systems and the coupling between chemical, electrochemical and transport processes in confinement may open tremendous opportunities for energy, catalysis or water treatment applications in the future.

Date: 2024
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DOI: 10.1038/s41467-024-46280-1

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