Highly active electrocatalysts for oxygen reduction from carbon-supported copper-phthalocyanine synthesized by high temperature treatment

被引:86
作者
Ding, Lei [1 ]
Qiao, Jinli [1 ]
Dai, Xianfeng [1 ]
Zhang, Jing [1 ]
Zhang, Jiujun [2 ]
Tian, Binglun [3 ]
机构
[1] Donghua Univ, Coll Environm Sci & Engn, Shanghai 201620, Peoples R China
[2] Natl Res Council Canada, Vancouver, BC V7A 4T8, Canada
[3] Pearl Hydrogen Technol Co Ltd, Shanghai 201803, Peoples R China
基金
中国国家自然科学基金;
关键词
Copper phthalocyanine; Electrocatalysts; Oxygen reduction reaction; Heat treatment; Alkaline fuel cell; FE-BASED CATALYSTS; FUEL-CELL CONDITIONS; CATHODE CATALYSTS; STABILITY; PYROLYSIS; ALLOY; IRON; CU; NANOPARTICLES; SITES;
D O I
10.1016/j.ijhydene.2012.07.046
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
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.
引用
收藏
页码:14103 / 14113
页数:11
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