Three-dimensional self-supporting superstructured double-sided nanoneedles arrays of iron carbide nanoclusters embedded in manganese, nitrogen co-doped carbon for highly efficient oxygen reduction reaction

Abstract

Nitrogen- and transition metal-dual doped carbon materials with low cost and high catalytic performances are considered as one of promising alternatives for noble metal catalysts in acceleration of oxygen reduction reaction (ORR). In this work, three-dimensional (3D) self-supporting superstructures of iron carbide (Fe₃C) nanoclusters entrapped in manganese (Mn)- and nitrogen (N)-dual doped carbon nanosheets covered with double-sided nanoneedles carbon arrays (Fe₃C/Mn,N-NCAs) are simply synthesized by a coordination pyrolysis method, in which dicyandiamide mainly behaves as nitrogen source and 1-(2-pyridylazo)-2-naphthol (PAN) as carbon source. Integration of the unique 3D self-supporting superstructures and synergistic effects of the multi-compositions, the as-obtained catalyst displays appealing ORR performance such as the much positive onset potential (E_onset = 0.98 V vs. RHE) and half-wave potential (E_1/2 = 0.88 V vs. RHE), as well as a just 10 mV negative shift in E_1/2 after 2000 cycles, surpassing commercial Pt/C. This work provides some valuable perspectives for preparation of high-efficiency and low-cost non-noble metal ORR electrocatalysts in energy transformation and storage correlated systems.

Keywords: Coordination pyrolysis; Doped carbon; Nanoneedles carbon arrays; Oxygen reduction reaction; Self-supporting superstructures.