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The controllable synthesis of high-quality and large-area graphene by chemical vapor deposition (CVD) remains a challenge nowadays. The massive grain boundaries in graphene grown on polycrystalline Cu by CVD significantly reduce its carrier mobility, limiting its application in high-performance electronic devices. Here, we confirm that the synergetic pretreatment of Cu with electropolishing and surface oxidation is a more efficient way to further suppress the graphene nucleation density (GND) and to accelerate the growth rate of the gra