Tianle Gong1, Ruoyu Qi1, Xundao Liu2, Hong Li3, Yongming Zhang1. 1. Shanghai Electrochemical Energy Devices Research Center, Shanghai Key Lab of Electrical Insulation and Thermal Aging, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai, 200240, People's Republic of China. 2. School of Material Science and Engineering, University of Jinan, Jinan, 250022, People's Republic of China. 3. Shanghai Electrochemical Energy Devices Research Center, Shanghai Key Lab of Electrical Insulation and Thermal Aging, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai, 200240, People's Republic of China. lh102@sjtu.edu.cn.
Abstract
Currently, the oxygen reduction reaction (ORR) mainly depends on precious metal platinum (Pt) catalysts. However, Pt-based catalysts have several shortcomings, such as high cost, scarcity, and poor long-term stability. Therefore, development of efficient metal-free electrocatalysts to replace Pt-based electrocatalysts is important. In this study, we successfully prepared nitrogen- and fluorine-codoped microporous carbon nanofibers (N, F-MCFs) via electrospinning polyacrylonitrile/polyvinylidene fluoride/polyvinylpyrrolidone (PAN/PVDF/PVP) tricomponent polymers followed by a hydrothermal process and thermal treatment, which was achieved for the first time in the literature. The results indicated that N, F-MCFs exhibit a high catalytic activity (Eonset: 0.94 V vs. RHE, E1/2: 0.81 V vs. RHE, and electron transfer number: 4.0) and considerably better stability and methanol tolerance for ORR in alkaline solutions as compared to commercial Pt/carbon (Pt/C, 20 wt%) catalysts. Furthermore, in acidic media, N, F-MCFs showed a four-electron transfer pathway for ORR. This study provides a new strategy for in situ synthesis of N, F-MCFs as highly efficient metal-free electrocatalysts for ORR in fuel cells.
Currently, then class="Chemical">oxygen reduction reaction (ORR) mainly depends on precious metal platinum (Pt) catalysts. However, Pt-based catalysts have several shortcomings, such as high cost, scarcity, and poor long-term stability. Therefore, development of efficient metal-free electrocatalysts to replace Pt-based electrocatalysts is important. In this study, we successfully prepared nitrogen- and fluorine-codoped microporous carbon nanofibers (N, F-MCFs) via electrospinning polyacrylonitrile/polyvinylidene fluoride/polyvinylpyrrolidone (PAN/PVDF/PVP) tricomponent polymers followed by a hydrothermal process and thermal treatment, which was achieved for the first time in the literature. The results indicated that N, F-MCFs exhibit a high catalytic activity (Eonset: 0.94 V vs. RHE, E1/2: 0.81 V vs. RHE, and electron transfer number: 4.0) and considerably better stability and methanol tolerance for ORR in alkaline solutions as compared to commercialPt/carbon (Pt/C, 20 wt%) catalysts. Furthermore, in acidic media, N, F-MCFs showed a four-electron transfer pathway for ORR. This study provides a new strategy for in situ synthesis of N, F-MCFs as highly efficient metal-free electrocatalysts for ORR in fuel cells.