Porous carbon nanosheets from biological nucleobase precursor as efficient pH-independent oxygen reduction electrocatalyst

Abstract Pyridinic-N configurations and intrinsic defects on nanocarbons have been regarded as potentially active-sites for the oxygen reduction reaction (ORR). In this work, a facile strategy is demonstrated to achieve pyridinic-N dominated porous carbon nanosheets with edge-enriched defective nature through the selection of the bio-precursor guanine as C/N sources. It is able to achieve high contents of pyridinic-N dominated (48.1% from gross N) species and the few-layers carbon architectures with hierarchical porosity by a template-free carbonization method. These 2D carbon structures are of low cost, scalable and economically attractive while based on renewable and highly abundant resources. As a result, the optimized catalyst delivers a significantly enhanced electrocatalytic performance for ORR under wide range of pH from alkaline to acid, i. e. possessing a 30 mV more positive half-wave potential (0.885 V) than Pt/C (0.855 V) catalyst in 0.1 M KOH, and very close activities to Pt/C in 0.1 M PBS and 0.1 M HClO4 solution. This ORR performance is attributed to the synergistic effects of unique graphene-like architecture, high porosity, and coexistences of high contents of pyridinic-N species and abundant edge/defect sites.