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

Gao-Feng Han, Feng Li (), Wei Zou, Mohammadreza Karamad, Jong-Pil Jeon, Seong-Wook Kim, Seok-Jin Kim, Yunfei Bu, Zhengping Fu, Yalin Lu, Samira Siahrostami () and Jong-Beom Baek ()
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Gao-Feng Han: Ulsan National Institute of Science and Technology (UNIST)
Feng Li: Ulsan National Institute of Science and Technology (UNIST)
Wei Zou: University of Science and Technology of China (USTC)
Mohammadreza Karamad: University of Calgary, 2500 University Drive NW
Jong-Pil Jeon: Ulsan National Institute of Science and Technology (UNIST)
Seong-Wook Kim: Ulsan National Institute of Science and Technology (UNIST)
Seok-Jin Kim: Ulsan National Institute of Science and Technology (UNIST)
Yunfei Bu: School of Environmental Science and Engineering, Nanjing University of Information Science and Technology (NUIST), 219 Ningliu
Zhengping Fu: University of Science and Technology of China (USTC)
Yalin Lu: University of Science and Technology of China (USTC)
Samira Siahrostami: University of Calgary, 2500 University Drive NW
Jong-Beom Baek: Ulsan National Institute of Science and Technology (UNIST)

Nature Communications, 2020, vol. 11, issue 1, 1-9

Abstract: Abstract 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 0.75 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 H2O2 synthesis.

Date: 2020
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DOI: 10.1038/s41467-020-15782-z

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