Transient chemical and structural changes in graphene oxide during ripening

Graphene oxide (GO)—the oxidized form of graphene—is actively studied in various fields, such as energy, electronic devices, separation of water, materials engineering, and medical technologies, owing to its fascinating physicochemical properties. One major drawback of GO is its instability, which leads to the difficulties in product management. A physicochemical understanding of the ever-changing nature of GO can remove the barrier for its growing applications. Here, we evidencde the presence of intrinsic, metastable and transient GO states upon ripening. The three GO states are identified using a \(\pi -{\pi }^{*}\) $\pi -{\pi }^{*}$ transition peak of ultraviolet–visible absorption spectra and exhibit inherent magnetic and electrical properties. The presence of three states of GO is supported by the compositional changes of oxygen functional groups detected via X-ray photoelectron spectroscopy and structural information from X-ray diffraction analysis and transmission electron microscopy. Although intrinsic GO having a \(\pi -{\pi }^{*}\) $\pi -{\pi }^{*}$ transition at 230.5 ± 0.5 nm is stable only for 5 days at 298 K, the intrinsic state can be stabilized by either storing GO dispersions below 255 K or by adding ammonium peroxydisulfate.