3D N-doped carbon framework with embedded CoS nanoparticles as highly active and durable oxygen reduction and evolution electrocatalyst

Abstract

Development of bifunctional non-metal electrocatalyst for oxygen reduction reactions (ORRs) and oxygen evolution reactions (OERs) with high efficiency, durable stability and low cost is a crucial and challenging issue. However, the heteroatom-doped carbon material including a carbon-based conductive additive would be easily oxidized under the high potential needed for driving the OER. Besides, the interaction between the heteroatom-doped carbon material that possesses electrocatalyst activity and a carbon-based conductive additive is weak, affecting the performance of the electrocatalyst. In this context, we introduce CoS nanoparticles into a three-dimensional N-doped carbon framework (CoS/NCF) by a morphology-retaining pyrolysis of polyaniline/CoS framework precursor, in which the polyaniline framework provides abundant functional groups to nucleate and grow CoS nanoparticles while retaining its interconnected three-dimensional porous structure. Benefiting from (i) the lower OER potential of CoS nanoparticles than the electro-oxidation decomposition potential of a carbon material and (ii) the strong affinity of CoS nanoparticles for a N-doped carbon framework, higher stability than commercial Pt/C system and greater catalytic activity towards ORR with an onset potential of about 0.921 V versus reversible hydrogen electrode (RHE) are observed. Furthermore, only a potential of 1.515 V versus RHE is required for achieving a current density of 10 mA cm^-2.