Heteroatom-doped carbon dots based catalysts for oxygen reduction reactions.

Carbon materials doped with heteroatoms are a class of cost-effective and stable electrocatalysts for oxygen reduction reactions (ORR), whose activities are mainly based on the heteroatom-related active sites. Besides the widely reported one-dimensional carbon nanotubes and two-dimensional graphene materials, carbon dots (CDs), as a new kind of zero-dimensional carbon materials, exhibit a range of unique structures and promising catalytic activities for ORR. In order to optimize the complex conditions of carbon-based catalysts, composites consisting of doped CDs and reduced graphene oxide (rGO) (designated as CD/rGO) are prepared hydrothermally, in comparison with directly doped rGO. All produced composites outperform their corresponding directly doped rGO counterparts in ORR measurements. It is noted that nitrogen and sulfur co-doped samples perform better than those doped by individual N or S. Mechanistic relationships between the ORR catalytic activities and the catalyst features are proposed, including type, location, bonding, fraction and synergistic effects of dopants, as well as the composition and structure of the carbon substrates. It is apparent that doping heteroatoms and constructing carbon substrates play a synergistic role in yielding high-performance carbon based catalysts.