Revealing Isolated M-N3 C1 Active Sites for Efficient Collaborative Oxygen Reduction Catalysis

Feng Li; Gao-Feng Han; Yunfei Bu; Hyuk-Jun Noh; Jong-Pil Jeon; Tae Joo Shin; Seok-Jin Kim; Yuen Wu; Hu Young Jeong; Zhengping Fu; Yalin Lu; Jong-Beom Baek

doi:10.1002/anie.202008325

Revealing Isolated M-N₃ C₁ Active Sites for Efficient Collaborative Oxygen Reduction Catalysis

Angew Chem Int Ed Engl. 2020 Dec 21;59(52):23678-23683. doi: 10.1002/anie.202008325. Epub 2020 Oct 23.

Authors

Feng Li¹, Gao-Feng Han¹, Yunfei Bu², Hyuk-Jun Noh¹, Jong-Pil Jeon¹, Tae Joo Shin³, Seok-Jin Kim¹, Yuen Wu⁴, Hu Young Jeong³, Zhengping Fu⁵, Yalin Lu⁵, Jong-Beom Baek¹

Affiliations

¹ School of Energy and Chemical Engineering/Center for Dimension Controllable Organic Frameworks, Ulsan National Institute of Science and Technology, South Korea.
² Jiangsu Collaborative Innovation Center of Atmospheric Environment and Equipment Technology (CICAEET), Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control (AEMPC), School of Environmental Science and Technology, Nanjing University of Information Science and Technology, P. R. China.
³ UNIST Central Research Facilities, Ulsan National Institute of Science and Technology, South Korea.
⁴ Department of Chemistry, Hefei National Laboratory for Physical Sciences at Microscale, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), University of Science and Technology of China, P. R. China.
⁵ CAS Key Laboratory of Materials for Energy Conversion, Hefei National Laboratory for Physical Sciences at Microscale, University of Science and Technology of China, P. R. China.

PMID: 32959493
DOI: 10.1002/anie.202008325

Abstract

Single atom catalysts (SACs) are of great importance for oxygen reduction, a critical process in renewable energy technologies. The catalytic performance of SACs largely depends on the structure of their active sites, but explorations of highly active structures for SAC active sites are still limited. Herein, we demonstrate a combined experimental and theoretical study of oxygen reduction catalysis on SACs, which incorporate M-N₃ C₁ site structure, composed of atomically dispersed transition metals (e.g., Fe, Co, and Cu) in nitrogenated carbon nanosheets. The resulting SACs with M-N₃ C₁ sites exhibited prominent oxygen reduction catalytic activities in both acidic and alkaline media, following the trend Fe-N₃ C₁ > Co-N₃ C₁ > Cu-N₃ C₁ . Theoretical calculations suggest the C atoms in these structures behave as collaborative adsorption sites to M atoms, thanks to interactions between the d/p orbitals of the M/C atoms in the M-N₃ C₁ sites, enabling dual site oxygen reduction.

Keywords: active sites; collaborative catalysis; oxygen reduction reaction; single atom catalyst.

Abstract

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