N-Doped Carbon Electrocatalyst: Marked ORR Activity in Acidic Media without the Contribution from Metal Sites?

Fantao Kong; Xiangzhi Cui; Yifan Huang; Heliang Yao; Yafeng Chen; Han Tian; Ge Meng; Chang Chen; Ziwei Chang; Jianlin Shi

doi:10.1002/anie.202116290

N-Doped Carbon Electrocatalyst: Marked ORR Activity in Acidic Media without the Contribution from Metal Sites?

Angew Chem Int Ed Engl. 2022 Apr 4;61(15):e202116290. doi: 10.1002/anie.202116290. Epub 2022 Feb 19.

Authors

Fantao Kong¹, Xiangzhi Cui^{1

2

3}, Yifan Huang⁴, Heliang Yao¹, Yafeng Chen⁵, Han Tian¹, Ge Meng^{1

2}, Chang Chen^{1

2}, Ziwei Chang⁶, Jianlin Shi^{1

2}

Affiliations

¹ State Key Lab of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai, 200050, P. R. China.
² Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing, 100049, P. R. China.
³ School of Chemistry and Materials Science, Hangzhou Institute for Advanced Study, University of Chinese Academy of Sciences, Hangzhou, 310021, P. R. China.
⁴ College of Chemistry and Materials Science, Shanghai Normal University, Shanghai, 200234, P. R. China.
⁵ Collaborative Innovation Center of Steel Technology, University of Science and Technology Beijing, Beijing, 100083, P. R. China.
⁶ School of Physical Science and Technology, Shanghai Tech University, Shanghai, 201210, P. R. China.

PMID: 35075773
DOI: 10.1002/anie.202116290

Abstract

Fe-N-C electrocatalysts have been demonstrated to be the most promising substitutes for benchmark Pt/C catalysts for the oxygen reduction reaction (ORR). Herein, we report that N-doped carbon materials with trace amounts of iron (0-0.08 wt. %) show excellent ORR activity and durability comparable and even superior to those of Pt/C in both alkaline and acidic media without significant contribution by the metal sites. Such an N-doped carbon (denoted as N-HPCs) features a hollow and hierarchically porous architecture, and more importantly, a noncovalently bonded N-deficient/N-rich heterostructure providing the active sites for oxygen adsorption and activation owing to the efficient electron transfer between the layers. The primary Zn-air battery using N-HPCs as the cathode delivers a much higher power density of 158 mW cm^-2 , and the maximum power density in the H₂ -O₂ fuel cell reaches 486 mW cm^-2 , which is comparable to and even better than those using conventional Fe-N-C catalysts at cathodes.

Keywords: Heterostructures; Intermolecular Electron Transfer; Nanocages; Oxygen Reduction Reaction; Synergistic Effects.

Abstract

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