Nitrogen and atomic Fe dual-doped porous carbon nanocubes as superior electrocatalysts for acidic H2-O2 PEMFC and alkaline Zn-air battery

作者：Shi, Xiudong; Pu, Zonghua; Chi, Bin; Liu, Mingrui; Yu, Siyan; Zheng, Long; Yang, Lijun; Shu, Ting; Liao, Shijun^*

来源：Journal of Energy Chemistry, 2021, 59: 388-395.

DOI：10.1016/j.jechem.2020.11.026

• Gaseous doping
• Fe-N-x sites
• Fe single atoms
• Oxygen reduction reaction
• Electrocatalysts

Air cathodes with high electrocatalytic activity are vital for developing H-2/O-2 proton exchange membrane fuel cells (PEMFC) and Zn-air batteries. However, the state-of-the-art air cathodes suffer from either limited catalytic activity or high cost, which thus hinder their applications. Herein, we designed ZIF-8 derived nitrogen and atomic iron dual-doped porous carbon nanocubes as high-quality catalysts for ORR, through a novel gas-doping approach. The porous carbon nanocubic architecture and abundant Fe-Nx active species endow ZIF-8 derived single atomic iron catalyst (PCN-A@Fe SA) with superior catalytic activity, and surpass Pt/C and a majority of the reported catalysts. Both XAS and DFT calculations suggest that Fe2+N4 moieties are the main active centers that are favorable for oxygen affinity and OH* intermediate desorption, which can result in promising catalytic performance. Most importantly, PCN-A@Fe SA can achieve power density of 514 mW cm(-2) as cathodic catalyst in a PEMFC and discharge peak power density of 185 mW cm(-2) in an alkaline Zn-air battery. The outstanding performance is derived from both the high specific surface area and high-density of iron single atom in nitrogen doped nanocubic carbon matrix.

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