On the correlation between the porous structure and the electrochemical response of powdered and monolithic carbon aerogels as electrodes for capacitive deionization

The combined effect of resorcinol/catalyst (100≤R/C≤800) and resorcinol/water (0.04≤R/W≤0.13) molar ratio on the textural and capacitive properties of carbon aerogels with potential application for capacitive deionization has been evaluated. Activated and pyrolyzed aerogels were synthesized by the sol-gel polymerization of resorcinol-formaldehyde mixtures and dried in supercritical conditions. Data show that high R/C and R/W molar ratios lead to materials with large pores in the mesopore range, whereas the surface area and micropore volumes remain somewhat the same. The activation of the aerogels increased the differences in the specific surface and micropore volumes due to the development of microporosity. This effect was more remarkable for the samples with low R/C whatever the R/W ratio, indicating that the carbon aerogel obtained using high amounts of catalyst are more prone to be activated. Regarding the electrochemical features of the aerogels, low capacitance values were measured in aerogels combining low R/W and high R/C and reciprocally low R/C and high R/W molar ratios, due to their higher resistance. Polarization resistances were found to be slightly higher for the pyrolyzed than for activated aerogels, and followed a decreasing trend with the mesoporosity, indicating the outstanding contribution of the mesoporous network to provide a good kinetic response. The desalting capacity of monolithic aerogels showed a simultaneous dependence with the surface area and the resistivity of the electrodes, pointing out the importance of performing electrochemical measurements in adequate cell configurations (i.e., desalting units) upon the intended application.
The authors are indebted to the Spanish MICINN (contract IPT-2011-1450-310000 (ADECAR) and CTM2014/56670-R) for the financial support. We also thank the fruitful collaboration of Isolux Ingeniería, S.A., Fundación Imdea Energia and Proingesa.