Abstract
Doping with pyridinic nitrogen atoms is known as an effective strategy to improve the activity of carbon-based catalysts for the oxygen reduction reaction. However, pyridinic nitrogen atoms prefer to occupy at the edge or defect sites of carbon materials. Here, a carbon framework named as hydrogen-substituted graphdiyne provides a suitable carbon matrix for pyridinic nitrogen doping. In hydrogen-substituted graphdiyne, three of the carbon atoms in a benzene ring are bonded to hydrogen and serve as active sites, like the edge or defect positions of conventional carbon materials, on which pyridinic nitrogen can be selectively doped. The as-synthesized pyridinic nitrogen-doped hydrogen-substituted graphdiyne shows much better electrocatalytic performance for the oxygen reduction reaction than that of the commercial platinum-based catalyst in alkaline media and comparable activity in acidic media. Density functional theory calculations demonstrate that the pyridinic nitrogen-doped hydrogen-substituted graphdiyne is more effective than pyridinic nitrogen-doped graphene for oxygen reduction.
Highlights
Doping with pyridinic nitrogen atoms is known as an effective strategy to improve the activity of carbon-based catalysts for the oxygen reduction reaction
The details for the synthesis process of hydrogensubstituted graphdiyne (HsGDY) and N-doped HsGDY (N-HsGDY) are described in the Methods section (Supplementary Fig. 1a and Fig. 1a)
Fourier transform infrared spectroscopy (FT-IR) data (Supplementary Fig. 4) and Raman spectra (Supplementary Fig. 5) for triethynylbenzene confirmed the presence of aromatic ring units and acetylenic bonds in HsGDY
Summary
Doping with pyridinic nitrogen atoms is known as an effective strategy to improve the activity of carbon-based catalysts for the oxygen reduction reaction. In hydrogen-substituted graphdiyne, three of the carbon atoms in a benzene ring are bonded to hydrogen and serve as active sites, like the edge or defect positions of conventional carbon materials, on which pyridinic nitrogen can be selectively doped. Many heteroatom-doped carbon materials demonstrate high activity for ORR Among those catalysts, nitrogen (N)-doped carbon materials are some of the most efficient metal-free catalysts[3,4,5,6]. As the concentration of edges and defects is low in these carbon materials, it is difficult to selectively dope a sufficient amount of pyridinic nitrogen atoms This is a bottleneck in researching the catalysis mechanism and application of carbonbased materials. HsGDY is likely an ideal model carbon framework to selectively dope pyridinic N to obtain highly active metal-free ORR catalysts
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