Monitoring Aging Effects in Graphite Bisulfates by Means of Raman Spectroscopy

Graphite bisulfate (GBS) compounds consist of graphite layers intercalated by HSO4- ions and H2SO4 molecules. Owing to electrostatic interactions with the graphene plane, HSO4- ions cause point defects in the graphite's crystalline structure, while H2SO4 molecules are free to move via diffusion in the spaces between the adjacent graphite sheets and segregate to form linear defects. In the present work, we report the results of our investigation using Raman spectroscopy on the temporal evolution of such defects on selected GBS samples over 84 months. Two characteristic lengths correlated with the average distance between defects have been estimated and their evolution with aging was investigated. The results show a decrease in the density of point-like defects after aging, regardless of the pristine structural configuration of the GBS samples, revealing a structural instability. This study can provide significant information for the technological development of industrial processes aimed to produce expanded graphite based on GBS precursors, where the aging of GBS is known to influence the efficiency and quality.