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Herein, we report a improved method for the physical grafting of1-nitropyrene (Pyr-NO2) onto highly graphitized carbon onion. This is achievedthrough a lowering of the onset potential of the pyrene polymerization via insitu reduction of the NO2 group. The additional redox activity pertaining tothe reduced NO2 enables exceeding the faradaic capacity which is associatedwith the p-doping of the grafted pyrene backbone, as observed for pyrene,1-aminopyrene, and unreduced Pyr- NO2. Theoretical calculations demonstrate thecharge transfer and binding enthalpy capabilities of Pyr-NO2, which aresignificantly higher than those of the other two species, and which allow forimproved p-stacking on the carbon surface. Upon 20 wt % grafting of Pyr-NO2,the capacity of the electrode jumps from 20 mAh g-1 electrode to 38 mAh g-electrode, which corresponds to 110 mAh g-1 per mass of Pyr-NO2 and the averagepotential is increased by 200 mV. Very interestingly, this high performance isalso coupled with outstanding retention with respect to both the initialcapacity for more than 4000 cycles, as well as the power characteristics,demonstrating the considerable advantages of employing the present in situgrafting technique.

journal of materials chemistry. a

Improved electro-grafting of nitropyrene onto onion-like carbon via in  situ electrochemical reduction and polymerization: Tailoring redox energy  density of the supercapacitor positive electrode