▎ 摘　　要

Edge-carboxylated graphene nanoplatelets (ECGnPs) were synthesized by the simple, efficient and eco-friendly ball-milling of graphite in the presence of dry ice and used as oxygen-rich metal-free counter electrodes (CEs) in organic dye-sensitized solar cells (DSSCs), for the first time. The resultant ECGnPs are soluble in many polar solvents including 2-propanol due to the polar nature of numerous carboxylic acids at edges, allowing an electrostatic spray (e-spray) to be deposited on fluorine-doped SnO2 (FTO)/glass substrates. The ECGnP-CE exhibited profound improvements in the electrochemical stability for the Co(bpy)(3)(2+/3+) redox couple compared to the platinum (Pt)-CE. The charge transfer resistance (R-CT), related to the interface between an electrolyte and a CE, was significantly reduced to 0.87 Omega cm(2), much lower than those of (Pt)-CE (2.19 Omega cm(2)), PEDOT: PSS-CE (2.63 Omega cm(2)) and reduced graphene oxide (rGO)-CE (1.21 Omega cm(2)). The DSSC based on the JK-303-sensitizer and ECGnP-CE displayed a higher photovoltaic performance ( FF, J(sc), and eta, 74.4%, 14.07 mA cm(-2) and 9.31%) than those with the Pt-CE (71.6%, 13.69 mA cm(-2) and 8.67%), PEDOT: PSS ( 68.7%, 13.68 mA cm(-2) and 8.25%) and rGO-CE (72.9%, 13.88 mA cm(-2) and 8.94%).