title: High correlation between oxidation loci on graphene oxide.
abstract: Recent experiments have shown the coexistence of both large unoxidized and oxidized regions on graphene oxide (GO), but the underlying mechanism for the formation of the GO atomic structure remains unknown. Now, using density functional calculations, 52 oxidation pathways for local pyrene structures on GO were identified, and a kinetic profile for graphene oxidation with a high correlation between oxidation loci was proposed, which is different from the conventional view, which entails a random distribution of oxidation loci. The high correlation is an essential nature of graphene oxidation processes and can be attributed to three crucial effects: 1) breaking of delocalized π bonds, 2) steric hindrance, and 3) hydrogen-bond formation. This high correlation leads to the coexistence of both large unoxidized and oxidized regions on GO. Interestingly, even in oxidized regions on GO, some small areas of sp(2)-hybridized domains, similar to "islands", can persist because of steric effects.
authors.affiliation: Department Division of Interfacial Water and Key Laboratory of Interfacial Physics and Technology, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201800 (China); University of Chinese Academy of Sciences, Beijing, 100049 (China).
authors.forename: Jinrong
authors.initials: J
authors.lastname: Yang
authors.forename: Guosheng
authors.initials: G
authors.lastname: Shi
authors.forename: Yusong
authors.initials: Y
authors.lastname: Tu
authors.forename: Haiping
authors.initials: H
authors.lastname: Fang
keywords: carbon; density functional calculations; graphene oxide; oxidation