Building and identifying highly active oxygenated groups in carbon materials for oxygen reduction to H2O2
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- Building and identifying highly active oxygenated groups in carbon materials for oxygen reduction to H2O2
- Han, Gao-Feng; Li, Feng; Zou, Wei; Karamad, Mohammadreza; Jeon, Jong-Pil; Kim, Seong-Wook; Kim, Seok-Jin; Bu, Yunfei; Fu, Zhengping; Lu, Yalin; Siahrostami, Samira; Baek, Jong-Beom
- Issue Date
- NATURE PUBLISHING GROUP
- NATURE COMMUNICATIONS, v.11, no.1
- The one-step electrochemical synthesis of H2O2 is an on-site method that reduces dependence on the energy-intensive anthraquinone process. Oxidized carbon materials have proven to be promising catalysts due to their low cost and facile synthetic procedures. However, the nature of the active sites is still controversial, and direct experimental evidence is presently lacking. Here, we activate a carbon material with dangling edge sites and then decorate them with targeted functional groups. We show that quinone-enriched samples exhibit high selectivity and activity with a H2O2 yield ratio of up to 97.8 % at 0.75V vs. RHE. Using density functional theory calculations, we identify the activity trends of different possible quinone functional groups in the edge and basal plane of the carbon nanostructure and determine the most active motif. Our findings provide guidelines for designing carbon-based catalysts, which have simultaneous high selectivity and activity for H2O2 synthesis. The identity of catalytic sites for H2O2 generation in carbon-based materials remains controversial with limited experimental evidence to date. Here, the authors decorate various target functional groups on carbon materials and quinone-enriched samples exhibit the highest activity and selectivity.
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