Flow‐Chemistry Based Green Synthesis of Graphene Oxide at Minutes Timescale

Abstract Graphene oxide (GO) is broadly investigated in the electrochemical field. However, for industrial applications, it still suffer from high pollution, low efficiency, poor production quality, and safety concerns associated with traditional synthesis methods. Herein, guided by theoretical analyses, a new oxygen‐atom‐transfer (OAT) mechanism for periodate oxidizing graphite is revealed, exhibiting controllable reaction activity, strong orbital interaction, and abundant electron transfer. Moreover, a flow chemistry strategy with high mass/heat transfer rates is designed to enhance interlayer diffusion and reaction dynamics between oxidants and graphite, ensuring the efficient synthesis of GO within several minutes. As a result, both low oxygen‐content GO with large size, and high oxygen‐content GO with adequate active sites can be precisely and safely synthesized. Benefitting from the controllability of oxygen content and lateral size, the as‐prepared GO sheets can be facilely assembled into fiber/film electrodes that present high mechanical flexibility, large electrical conductivity, and outstanding electrochemical performance.