Computational Studies of the Structure, Behavior upon Heating, and Mechanical Properties of Graphite Oxide

A Monte Carlo based scheme for the formation of graphite oxide (GO) was developed and implemented. A Rosenbluth factor was used to select intermediate structures in an attempt to form stable, low-energy, and realistic GO. The scheme resulted in the production of GO that has an interplanar spacing of 5.8 A, in good agreement with the experimental value (5.97 A). Epoxide and hydroxyl functional groups dominate the basal planes, a finding that is consistent with experiment. Individual sheets are wrinkled with an average root-mean-square deviation of 0.33 ± 0.04 A. Hydrogen bonding between hydroxyl groups and between hydroxyl and epoxide groups has significant impact on the stability of many structures. Molecular dynamics simulations, guided by forces from electronic structure calculations, were performed to examine the behavior of GO when heated to room (300 K) and thermal exfoliation (1323 K) temperatures. Hydrogen-transfer reactions that catalyze the migration of epoxide groups were observed at both temper...

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