Wet chemical synthesis of nitrogen-doped graphene towards oxygen reduction electrocatalysts without high-temperature pyrolysis

Abstract

The oxygen reduction reaction (ORR) is one of the important reactions not only in life processes but also in artificial energy conversion systems, such as fuel cells and metal/air batteries. As one of the non-precious ORR catalysts, N-doped carbon materials show an exciting activity, but most of them were universally synthesized by high-temperature pyrolysis or annealing up to 1100 °C in the past few decades, which makes the structural manipulation of the catalysts extremely difficult. Here, we propose that ORR active N-doped carbon catalysts could, in principle, be prepared via a sophisticated wet chemical reaction between a reactive graphitic carbon template (e.g. graphene oxide) and N-containing molecules (e.g. dicyandiamide) at temperatures as low as 180 °C. Without any high-temperature treatments, for example, the as-prepared N-doped reduced graphene oxide with additional Fe-containing nanoparticles showed an impressive ORR catalytic activity that was comparable to many previous N-doped carbon from high-temperature pyrolysis. Rational utilization of the graphitic carbon template, the N-containing molecules, and the wet chemical reactions may offer a low-temperature route to create interesting ORR electrocatalysts with easier surface properties manipulation.