Building and identifying highly active oxygenated groups in carbon materials for oxygen reduction to H2O2

• Published in: Nature communications Vol. 11; no. 1; pp. 1 - 9
• Main Authors: 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
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 05.05.2020; Nature Publishing Group; Nature Portfolio
• Subjects: 147/135; 147/143; 639/301/299/161/886; 639/638/563/979; 639/925/357/551; Active sites; Anthraquinone; Anthraquinones; Basal plane; Carbon; Catalysts; Chemical synthesis; Density functional theory; Electrochemistry; Functional groups; Humanities and Social Sciences; Hydrogen peroxide; multidisciplinary; Quinones; Science; Science (multidisciplinary); Selectivity
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-020-15782-z

The one-step electrochemical synthesis of H 2 O 2 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 H 2 O 2 yield ratio of up to 97.8 % at 0.75 V 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 H 2 O 2 synthesis. The identity of catalytic sites for H 2 O 2 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.