期刊
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
卷 37, 期 19, 页码 14103-14113出版社
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.ijhydene.2012.07.046
关键词
Copper phthalocyanine; Electrocatalysts; Oxygen reduction reaction; Heat treatment; Alkaline fuel cell
资金
- National Natural Science Foundation of China [21173039]
- Specialized Research Fund for the Doctoral Program of Higher Education, SRFD of China [20110075110001]
- opening Foundation of Zhejing Provincial Top Key Discipline, China [20110927]
- State Environmental Protection Engineering Center for Pollution Treatment and Control in Textile Industry of China
- Shanghai Leading Academic Discipline Project [B604]
The active, carbon-supported copper phthalocyanine (CuPc/C) nano-catalyst, as a novel cathode catalyst for oxygen reduction reaction, is synthesized via a combined solvent-impregnation along with the high temperature treatment. The catalytic activities of both pyrolyzed and unpyrolyzed catalysts are screened by linear sweep voltammetry (LSV) employing a rotating disk electrode (RDE) technique to quantitatively obtain the oxygen reduction reaction (ORR) kinetic constants and the reaction mechanisms. The results show that heat-treatment can significantly improve the ORR activity of the catalyst, and the optimal heat-treated temperature is around 800 degrees C, under which, an onset potential of 0.10 V and a half-wave potential of -0.05 V are achieved in alkaline electrolyte. Besides the ORR kinetic rate is increased, the ORR electron transfer number is also increased from 2.5 to 3.6 with increasing heat-treatment temperature from 600 to 800 degrees C. Also, the effect of catalyst loading in the catalyst layer on the corresponding ORR activity is also studied, and finds that increasing the catalyst loading, the catalyzed ORR kinetic current density can be significantly increased. For a fully understanding of this heat-treatment temperature effect, XRD, TEM, SEM-EDX, TG and XPS are used to identify the catalyst structure and composition. TG results demonstrated that the presence of Cu prevents phthalocyanine from thermal decomposition, thus contribute to higher nitrogen content which can form more Cu-N-x activity sites for the ORR. XPS analysis indicates that both pyridinic-N and graphitic-N may be responsible for the enhanced ORR activity. Copyright (C) 2012, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.
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