Investigation of the durability of a poly-p-phenylenediamine/carbon black composite for the oxygen reduction reaction

doi:10.1016/S1872-2067(15)61063-4

Chinese Journal of Catalysis ›› 2016, Vol. 37 ›› Issue (7): 1096-1102.DOI: 10.1016/S1872-2067(15)61063-4

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Investigation of the durability of a poly-p-phenylenediamine/carbon black composite for the oxygen reduction reaction

Xiaogang Su^a,b, Yingfang Yao^a,b,c, Juan Tian^c, Jianguo Liu^a,b,c,d, Zhongwei Wang^a,b, Yong You^a,b, Lin Huang^a,b,c, Congping Wu^a,b,c

a. College of Engineering and Applied Sciences, Nanjing University, Nanjing 210093, Jiangsu, China;
b. National Laboratory of Solid State Microstructures, Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing 210093, Jiangsu, China;
c. Kunshan Innovation Institute of Nanjing University, Suzhou 215347, Jiangsu, China;
d. Suzhou High-Tech Institute of Nanjing University, Suzhou 215123, Jiangsu, China

Received:2016-01-06 Revised:2016-02-02 Online:2016-06-17 Published:2016-06-17
Contact: Jianguo Liu
Supported by:
This work was supported by the National Natural Science Foundation of China (21476104), the Natural Science Foundation for Distinguished Young Scholars of Jiangsu Province (BK20150009), the Natural Science Foundation for Young Scholars of Jiangsu Province (BK20150396), the Soft Science Research Program of Jiangsu Province (BR2015009), the Nanotechnology Program of Suzhou (ZXG2013029), the Priority Academic Program Development (PAPD) of Jiangsu Higher Education Institutions, Qing Lan Project of Jiangsu Province, and the Fundamental Research Funds for the Central Universities, China.

Abstract

Abstract:

Nitrogen-doped carbon materials exhibiting high oxygen reduction reaction activity were prepared via the pyrolysis of a poly-p-phenylenediamine/carbon black composite. The as-synthesized catalyst showed excellent catalytic activity in alkaline solution, and outperformed commercial Pt/C in KOH solution (0.1 mol/L), as demonstrated by the higher current density and the more positive half-wave potential. Scanning electron microscopy and N₂ adsorption-desorption analyses indicated that a composite structure, in which the N-rich surface of the poly-p-phenylenediamine had an increased active center concentration and the high external surface area of the carbon black was conducive to the mass transport, is highly beneficial in terms of promoting the oxygen reduction reaction. However, the activity of this catalyst underwent an obvious decrease following exposure to air for 30 d. X-ray photoelectron spectroscopy showed that the oxygen content in the catalyst was increased by prolonged air exposure. O 1s spectrum showed increases in the C=O and C-O components, suggesting that atmospheric oxygen reacted with the catalyst. This oxidation leaded to the deactivation of active center, thus the catalytic activity decreased. Based on these results, the stability in air of nitrogen-doped carbon materials must be taken into consideration when assessing applications as alternatives to platinum-based materials.

Key words: Phenylenediamine, Carbon black, Composite structure, Oxygen reduction reaction, Durability

Xiaogang Su, Yingfang Yao, Juan Tian, Jianguo Liu, Zhongwei Wang, Yong You, Lin Huang, Congping Wu. Investigation of the durability of a poly-p-phenylenediamine/carbon black composite for the oxygen reduction reaction[J]. Chinese Journal of Catalysis, 2016, 37(7): 1096-1102.

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Investigation of the durability of a poly-p-phenylenediamine/carbon black composite for the oxygen reduction reaction

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