Journal
NATURE CHEMISTRY
Volume 10, Issue 9, Pages 924-931Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/s41557-018-0100-1
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Funding
- National Science Fund for Distinguished Young Scholars [21325105]
- National Natural Science Foundation of China [21590795, 21401199, 21790050, 21790051]
- National Key Research and Development Program of China [2016YFB0600903, 2016YFA0200104]
- Chinese Academy of Sciences (CAS) Interdisciplinary Innovation Team
- Australian Research Council (ARC) Discovery Project [160104817]
- Foundation for State Key Laboratory of Biochemical Engineering
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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 O-2 adsorption 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.
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