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Few-layer graphdiyne doped with sp-hybridized nitrogen atoms at acetylenic sites for oxygen reduction electrocatalysis
- Source :
- Nature Chemistry; September 2018, Vol. 10 Issue: 9 p924-931, 8p
- Publication Year :
- 2018
-
Abstract
- The oxygen reduction reaction (ORR) is a fundamental reaction for energy storage and conversion. It has mainly relied on platinum-based electrocatalysts, but the chemical doping of carbon-based materials has proven to be a promising strategy for preparing metal-free alternatives. Nitrogen doping in particular provides a diverse range of nitrogen forms. Here, we introduce a new form of nitrogen doping moieties —sp-hybridized nitrogen (sp-N) atoms into chemically defined sites of ultrathin graphdiyne, through pericyclic replacement of the acetylene groups. The as-prepared sp-N-doped graphdiyne catalyst exhibits overall good ORR performance, in particular with regards to peak potential, half-wave potential and current density. Under alkaline conditions it was comparable to commercial Pt/C, and showed more rapid kinetics. And although its performances are a bit lower than those of Pt/C in acidic media they surpass those of other metal-free materials. Taken together, experimental data and density functional theory calculations suggest that the high catalytic activity originates from the sp-N dopant, which facilitates O2adsorption and electron transfer on the surface of the catalyst. This incorporation of chemically defined sp-N atoms provides a new synthetic route to high-performance carbon-based and other metal-free catalysts. Heteroatom doping is a widely used modification method for carbon-based catalysts. Now, chemically defined sp-hybridized nitrogen atoms have been selectively introduced to the acetylene groups in ultrathin graphdiynes, resulting in good catalytic activity for the oxygen reduction reaction in both alkaline and acidic media.
Details
- Language :
- English
- ISSN :
- 17554330 and 17554349
- Volume :
- 10
- Issue :
- 9
- Database :
- Supplemental Index
- Journal :
- Nature Chemistry
- Publication Type :
- Periodical
- Accession number :
- ejs50470952
- Full Text :
- https://doi.org/10.1038/s41557-018-0100-1