Defect-Free Single-Layer Graphene by 10 s Microwave Solid Exfoliation and Its Application for Catalytic Water Splitting

Mass production of defect-free single-layer graphene flakes (SLGFs) by a cost-effective approach is still very challenging. Here, we report such single-layer graphene flakes (SLGFs) (>90%) prepared by a nondestructive, energy-efficient, and easy up-scalable physical approach. These high-quality graphene flakes are attributed to a novel 10 s microwave-modulated solid-state approach, which not only fast exfoliates graphite in air but also self-heals the surface of graphite to remove the impurities. The fabricated high-quality graphene films (∼200 nm) exhibit a sheet resistance of ∼280 Ω/sq without any chemical or physical post-treatment. Furthermore, graphene-incorporated Ni-Fe electrodes represent a remarkable ∼140 mA/cm² current for the catalytic water oxidation reaction compared with the pristine Ni-Fe electrode (∼10 mA/cm²) and a 120 mV cathodic shift in onset potential under identical experimental conditions, together with a faradic efficiency of >90% for an ideal ratio of H₂ and O₂ production from water. All these excellent performances are attributed to extremely high conductivity of the defect-free graphene flakes.