Experimental and Dft Studies of Oxygen Reduction Reaction Promoted by Binary Site Fe/Co-N-C Catalyst in Acid

36 Pages Posted: 20 Oct 2021

See all articles by Yu Han

Yu Han

Xiamen University

Shuhu Yin

Xiamen University

Youhu Chen

Xiamen University

Chi Chen

Xiamen University

Wei Yan

Xiamen University

Xiaoyang Cheng

Xiamen University

Yanrong Li

Xiamen University

Tianen Zhang

Xiamen University

Jian Yang

Xiamen University

Yanxia Jiang

Xiamen University

Shigang Sun

Xiamen University

Date Written: 2021

Abstract

The cost and efficiency issues of cathodic electrocatalyst for oxygen reduction reaction (ORR) hinder a broad application of fuel cells. Therefore, it is necessary to develop highly efficient and sustainable ORR electrocatalysts of platinum group metal-free (PGM-free). The atomically dispersed FeCoNC-10 electrocatalysts were constructed by incorporating Fe phthalocyanine (FePc) molecules into bimetallic metal-organic frameworks (BMOF) followed by one-step pyrolysis. It showed remarkable ORR activity in acidic medium compared with FeNC and CoNC catalysts. The Fe-Co bimetallic sites were confirmed in FeCo-N-C, together with abundant isolated FeN 4 and CoN 4 sites. Theoretical study revealed that the bimetallic site can enhance O 2 adsorption and elongate O-O bond length rather than FeN 4 and CoN 4 . This can result in facile cleavage of the O-O bond and thus a direct 4e - ORR process. FeCoNC-10 catalyst showed enhanced ORR stability, due to very weak Fenton-type reaction related to Co species. Membrane electrode assemblies (MEAs) consisted of the FeCoNC-10 was applied in the cathode. It showed a peak power density of 100 mW cm -2 in a direct methanol fuel cells (DMFCs) with superior methanol tolerance. This work sheds light on the mechanism of atomically dispersed Fe/Co dual-doped carbon in enhancing ORR activity and stability, which enables the cost-effective ORR electrocatalyst design to achieve robust fuel cell performance.

Keywords: Oxygen reduction reaction, Platinum group metal-free (PGM-free), Bimetal active site, Acidic medium, Direct methanol fuel cell

Suggested Citation

Han, Yu and Yin, Shuhu and Chen, Youhu and Chen, Chi and Yan, Wei and Cheng, Xiaoyang and Li, Yanrong and Zhang, Tianen and Yang, Jian and Jiang, Yanxia and Sun, Shigang, Experimental and Dft Studies of Oxygen Reduction Reaction Promoted by Binary Site Fe/Co-N-C Catalyst in Acid (2021). Available at SSRN: https://ssrn.com/abstract=3946129 or http://dx.doi.org/10.2139/ssrn.3946129

Yu Han

Xiamen University ( email )

Xiamen, Fujian 361005
China

Shuhu Yin

Xiamen University ( email )

Xiamen, 361005
China

Youhu Chen

Xiamen University ( email )

Xiamen, 361005
China

Chi Chen

Xiamen University ( email )

Xiamen, 361005
China

Wei Yan

Xiamen University ( email )

Xiamen, 361005
China

Xiaoyang Cheng

Xiamen University ( email )

Xiamen, 361005
China

Yanrong Li

Xiamen University ( email )

Xiamen, 361005
China

Tianen Zhang

Xiamen University ( email )

Xiamen, 361005
China

Jian Yang

Xiamen University ( email )

Xiamen, 361005
China

Yanxia Jiang (Contact Author)

Xiamen University ( email )

Xiamen, 361005
China

Shigang Sun

Xiamen University ( email )

Xiamen, 361005
China

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