Fabrication of large-area and high-crystallinity photoreduced graphene oxide films via reconstructed two-dimensional multilayer structures

Graphene, the last representative sp(2) carbon material to be isolated, acts as an ideal material platform for constructing flexible electronic devices. Exploring a new method to fabricate high-quality graphene films with high throughput is essential for achieving greater performance with flexible electronic devices. Here, we report a facile coating and subsequent illumination method for mass-fabricating highly crystalline photoreduced graphene oxide (PRGO) films directly onto conductive substrates. The direct fabrication of PRGO films onto Cu foils with partial oxygenated groups, an intensive stacked highly crystalline structure, and reduced graphene oxide regions enable significant performance enhancements when used as supercapacitor electrodes compared with other graphene-only devices, exhibiting high specific capacitances of 275 F g(-1) at a scan rate of 10mVs(-1) and 167 F g(-1) at 1 V g(-1) with excellent rate capability. The as-established all-solid-state flexible supercapacitors exhibit superior flexibility and robust mechanical stability, resulting in a capacitance delay of only 2% after performing 100 bending cycles. The demonstrated PRGO films provide a promising material platform to realize a broad range of applications related to flexible electronics devices.