Polymer-Assisted Electrophoretic Synthesis of N-Doped Graphene-Polypyrrole Demonstrating Oxygen Reduction with Excellent Methanol Crossover Impact and Durability

The design and synthesis of metal-free catalysts with superior electrocatalytic activity, high durability, low cost, and under mild conditions is extremely desirable but remains challenging. To address this problem, a polymer-assisted electrochemical exfoliation technique of graphite in the presence of an aqueous acidic medium is reported. This simple, cost-effective, and mass-scale production approach could open the possibility for the synthesis of high-quality nitrogen-doped graphene-polypyrrole (NG-PPy). The NG-PPy catalyst displays an improved half wave potential (E-1/2=0.77 V) in alkaline medium compared with G-PPy (E-1/2=0.66 V). Most importantly, this catalyst demonstrates excellent stability with high methanol tolerance, and it outperforms the commercial Pt/C catalyst and other previously reported metal-free catalysts. The content of graphitic nitrogen atoms is the key factor for the enhancement of electrocatalytic activity towards oxygen reduction reactions (ORR). Interestingly, the NG-PPy catalyst can be used as a cathode material in a zinc-air battery, which demonstrates a higher peak power density (59 mW cm(-2)) than G-PPy (36.6 mW cm(-2)), highlighting the importance of the low-cost material synthesis approach towards the development of metal-free efficient ORR catalysts for fuel cell and metal-air battery applications. Remarkably, the polymer-assisted electrophoretic exfoliation of graphite with a high yield (approximate to 88 wt %) of few-layer graphene flakes could pave the way towards the mass production of high-quality graphene for a variety of applications.