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Unravelling the High-Activity Nature of Fe-N-C Electrocatalysts for Oxygen Reduction Reaction: The Extraordinary Synergy between Fe-Nx and Fe4N

58 Pages Posted: 17 Nov 2018 Publication Status: Under Review

See all articles by Xiang Ao

Xiang Ao

Huazhong University of Science and Technology - School of Optical and Electronic Information

Wei Zhang

Beijing University of Chemical Technology - Beijing Advanced Innovation Center for Soft Matter Science and Engineering

Zhishan Li

Huazhong University of Science and Technology - School of Optical and Electronic Information

Lin Lv

Huazhong University of Science and Technology - School of Optical and Electronic Information

Yunjun Ruan

Huazhong University of Science and Technology - School of Optical and Electronic Information

Zhenhua Chen

Chinese Academy of Sciences (CAS), Shanghai Institute of Applied Physics, Shanghai Synchrotron Radiation Facility

Kan-Hao Xue

Huazhong University of Science and Technology - School of Optical and Electronic Information; Huazhong University of Science and Technology - Wuhan National Laboratory for Optoelectronics

Hong-Hui Wu

University of Nebraska at Lincoln - Department of Chemistry

Wei-Hung Chiang

National Taiwan University of Science and Technology, College of Engineering, Department of Chemical Engineering

Xiangshui Miao

Huazhong University of Science and Technology - School of Optical and Electronic Information; Huazhong University of Science and Technology - Wuhan National Laboratory for Optoelectronics

Chundong Wang

Huazhong University of Science and Technology - School of Optical and Electronic Information

Xiao Cheng Zeng

Beijing University of Chemical Technology - Beijing Advanced Innovation Center for Soft Matter Science and Engineering; University of Nebraska at Lincoln - Department of Chemistry

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Abstract

The scarcity and weak durability of precious metal catalysts are among biggest obstacles to achieving cost-effective electrocatalysts in fuel cells. Hence, it is imperative to develop low-cost non-precious metal catalysts with comparable oxygen reduction reaction (ORR) activity to the precious metal catalysts. Herein, we report a highly effective strategy for facile synthesis of Fe/N-functionalized 3D porous carbon networks. A major advantage of the newly designed catalyst is that ultrafine Fe4N nanoparticles are grown and uniformly mounted on the carbon framework upon pyrolysis treatment at 800 °C, and co-existing with numerous in-situ formed Fe-Nx moieties in the carbon matrix, being evidenced by using X-ray absorption and photoelectron spectroscopy. The new electrocatalysts yield high ORR activity, comparable/superior to that of the state-of-the-art Fe/N-carbon based catalysts reported to date. Specifically, the catalysts show a half-wave potential of 0.890 V and a limited current density of 6.18 mA cm-2, both surpassing the commercial Pt/C. By resorting to the experimental measurements and density-functional theory (DFT) calculations, the synergistic effects between Fe-N4 moieties and the Fe4N support are identified for the first time, which play a key role in boosting catalytic performance of the Fe/N-functionalized porous carbon networks.

Suggested Citation

Ao, Xiang and Zhang, Wei and Li, Zhishan and Lv, Lin and Ruan, Yunjun and Chen, Zhenhua and Xue, Kan-Hao and Wu, Hong-Hui and Chiang, Wei-Hung and Miao, Xiangshui and Wang, Chundong and Zeng, Xiao Cheng, Unravelling the High-Activity Nature of Fe-N-C Electrocatalysts for Oxygen Reduction Reaction: The Extraordinary Synergy between Fe-Nx and Fe4N (November 16, 2018). Available at SSRN: https://ssrn.com/abstract=3285808 or http://dx.doi.org/10.2139/ssrn.3285808
This version of the paper has not been formally peer reviewed.

Xiang Ao

Huazhong University of Science and Technology - School of Optical and Electronic Information

Wuhan, 430074
China

Wei Zhang

Beijing University of Chemical Technology - Beijing Advanced Innovation Center for Soft Matter Science and Engineering

Beijing, 100029
China

Zhishan Li

Huazhong University of Science and Technology - School of Optical and Electronic Information

Wuhan, 430074
China

Lin Lv

Huazhong University of Science and Technology - School of Optical and Electronic Information

Wuhan, 430074
China

Yunjun Ruan

Huazhong University of Science and Technology - School of Optical and Electronic Information

Wuhan, 430074
China

Zhenhua Chen

Chinese Academy of Sciences (CAS), Shanghai Institute of Applied Physics, Shanghai Synchrotron Radiation Facility

Shanghai, 201204
China

Kan-Hao Xue

Huazhong University of Science and Technology - School of Optical and Electronic Information

Wuhan, 430074
China

Huazhong University of Science and Technology - Wuhan National Laboratory for Optoelectronics

1037 Luoyu Rd
Wuhan, 430074
China

Hong-Hui Wu

University of Nebraska at Lincoln - Department of Chemistry

Lincol, NE 68588
United States

Wei-Hung Chiang

National Taiwan University of Science and Technology, College of Engineering, Department of Chemical Engineering

Taipei, 10607
Taiwan

Xiangshui Miao

Huazhong University of Science and Technology - School of Optical and Electronic Information

Wuhan, 430074
China

Huazhong University of Science and Technology - Wuhan National Laboratory for Optoelectronics

1037 Luoyu Rd
Wuhan, 430074
China

Chundong Wang

Huazhong University of Science and Technology - School of Optical and Electronic Information ( email )

Wuhan, 430074
China

Xiao Cheng Zeng (Contact Author)

Beijing University of Chemical Technology - Beijing Advanced Innovation Center for Soft Matter Science and Engineering ( email )

Beijing, 100029
China

University of Nebraska at Lincoln - Department of Chemistry ( email )

Lincol, NE 68588
United States