▎ 摘　　要

Controlling the chemistry of graphene is necessary to enable applications in materials and life sciences. Research beyond graphene oxide is targeted to avoid the highly defective character of the carbon framework. Herein, we show how to optimize the synthesis of oxo-functionalized graphene (oxo-G) to prepare high-quality monolayer flakes that even allow for direct transmission electron microscopy investigation at atomic resolution (HRTEM). The role of undesired residuals is addressed and sources are eliminated. HRTEM provides clear evidence for the exceptional integrity of the carbon framework of such oxo-G sheets. The patchy distribution of oxo-functionality on the nm-scale, observed on our highly clean oxo-G sheets, corroborates theoretical predictions. Moreover, defined electron-beam irradiation facilitates gentle de-functionalization of oxo-G sheets, a new route towards clean graphene, which is a breakthrough for localized graphene chemistry.