Journal
ACS APPLIED NANO MATERIALS
Volume 2, Issue 11, Pages 6948-6959Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsanm.9b01433
Keywords
graphene quantum dots; laser ablation in liquid; photoluminescence; lifetime; oxygen reduction reaction; electrocatalysis
Funding
- National Science Foundation [1355438]
- Kentucky Science & Engineering Foundation [KSEF-3884-RDE-020]
- National Science Foundation Division of Chemistry [1800316]
- University of Kentucky Research Challenge Trust Fund
- Direct For Mathematical & Physical Scien [1800316] Funding Source: National Science Foundation
- Division Of Chemistry [1800316] Funding Source: National Science Foundation
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Nitrogen-doped graphene quantum dots (N-GQDs) have promising applications in catalysis and photoluminescence, but many existing synthetic methods require uses of harsh chemicals, long reaction times, and complicated purification steps and have poor control over the surface functional groups. Laser ablation in liquid (LAL) is a promising alternative method to prepare nanomaterials because of its fast production, use of fewer chemicals, simple purification, and fewer byproducts and its control of the product by precise tuning of laser ablation parameters. We report the use of LAL to produce N-GQDs from carbon nano-onions in aqueous solutions of ammonia, ethylenediamine, and pyridine. The choice of these dopants allowed for tuning the overall nitrogen content and the distribution of functional groups that led to the control over the photoluminescence emission wavelengths and lifetimes. High concentrations of amine groups tended to red-shift emission and exhibit shorter lifetimes, whereas pyridinic groups would blue-shift the emission and exhibit longer lifetimes. The N-GQDs also showed a promising performance as electrocatalysts for reducing oxygen to hydrogen peroxide, an important chemical widely used in industrial applications. The N-GQDs exhibited both low overpotentials and high selectivity for a two-electron oxygen reduction pathway.
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