On the interaction of carbon electrodes and non conventional electrolytes in high-voltage electrochemical capacitors

Abstract

This study is essentially based on innovative electrolytes such as the organic salt N-methyl-N-butylpyrrolidinium tetrafluoroborate (Pyr14BF4) dissolved in propylene carbonate (PC) and the pure ionic liquid (N-butyl-N-methyl-pyrrolidinium bis(trifluoromethanesulfonyl)imide (Pyr14TFSI) and its solution in PC. Activated carbon cloths were used as self-standing binder-free electrodes. It is found that the presence of impurities in carbon electrodes may lead to electrolyte decomposition and electrode degradation which notably affect the electrochemical double-layer capacitor (EDLC) performance. Such processes greatly depend on the composition of both the electrode and the electrolyte, being much less significant with solvent-containing electrolytes. By raising the operation temperature to 60 °C, the EDLC performance in the ionic liquid Pyr14TFSI is notably improved due to a relevant decrease in the viscosity and increase in ionic conductivity. By contrast, the presence of impurities, e.g., Zn and Al, in the electrodes remarkably reduces the electrolyte stability and a thick layer of decomposition products completely covers the carbon fibers after cycling at high temperature. The ionic liquid in solution maintains the high maximum operative voltage of the net ionic liquid whereas its viscosity and ionic conductivity are close to those of the conventional Et4NBF4/PC. Furthermore, the presence of propylene carbonate as solvent prevents to some extent the ionic liquid degradation.