Study on the oxygen adsorption property of nitrogen-containing metal-free carbon-based cathode catalysts for oxygen reduction reaction

被引:13
作者
Kiuchi, Hisao [1 ]
Niwa, Hideharu [1 ]
Kobayashi, Masaki [1 ,2 ]
Harada, Yoshihisa [1 ,2 ]
Oshima, Masaharu [1 ,2 ]
Chokai, Masayuki [3 ]
Nabae, Yuta [3 ]
Kuroki, Shigeki [3 ]
Kakimoto, Masa-aki [3 ]
Ikeda, Takashi [4 ]
Terakura, Kiyoyuki [3 ,5 ]
Miyata, Seizo [3 ]
机构
[1] Univ Tokyo, Dept Appl Chem, Bunkyo Ku, Tokyo 1138656, Japan
[2] Univ Tokyo, Synchrotsron Radiat Res Org, Sayo, Hyogo 6795165, Japan
[3] Tokyo Inst Technol, Dept Organ & Polymer Mat, Grad Sch Sci & Engn, Meguro Ku, Tokyo 1528552, Japan
[4] Japan Atom Energy Agcy, Synchorotron Radiat Res Unit, Quantum Beam Sci Directorate, Sayo, Hyogo 6795148, Japan
[5] JAIST, Res Ctr Integrated Sci, Nomi, Ishikawa 9231211, Japan
关键词
Oxygen reduction reaction; X-ray photoelectron spectroscopy; Oxygen adsorption; Electronic structure; Defects; ELECTROLYTE FUEL-CELLS; HIGH ELECTROCATALYTIC ACTIVITY; ACTIVATED CARBON; FUNCTIONAL-GROUPS; ALLOY CATALYSTS; IRON; NANOTUBES; GRAPHITE; POLYMERS; GRAPHENE;
D O I
10.1016/j.electacta.2012.06.036
中图分类号
O646 [电化学、电解、磁化学];
学科分类号
081704 ;
摘要
We study the characteristics of oxygen adsorption on metal-free carbon-based cathode catalysts derived from nitrogen-containing polyamide (PA) and nitrogen-free phenolic resin (PhRs). Electrochemical analysis and Raman spectroscopy showed higher 2-electron oxygen reduction reaction (ORR) activity and more defect sites in PA than PhRs. The increase in the amount of adsorbed oxygen in PA was also identified by oxygen adsorption isotherms. In situ X-ray photoelectron spectroscopy revealed that graphite-like nitrogen contributes to oxygen adsorption and C=O components are dominant in PA. These experimental results indicate that the adsorbed C=O components near the graphite-like nitrogen can be assigned as active sites for 2-electron ORR. (C) 2012 Elsevier Ltd. All rights reserved.
引用
收藏
页码:291 / 295
页数:5
相关论文
共 46 条
[1]   Oxygen plasma etching of carbon nano-structures containing nitrogen [J].
Acuna, J. J. S. ;
Figueroa, C. A. ;
da Costa, M. E. H. Maia ;
Paredez, P. ;
Ribeiro, C. T. M. ;
Alvarez, F. .
JOURNAL OF NON-CRYSTALLINE SOLIDS, 2006, 352 (9-20) :1314-1318
[2]   Oxygen etching mechanism in carbon-nitrogen (CNx) domelike nanostructures [J].
Acuna, J. J. S. ;
Figueroa, C. A. ;
Biggemann, D. ;
Kleinke, M. U. ;
Alvarez, F. .
JOURNAL OF APPLIED PHYSICS, 2008, 103 (12)
[3]   Novel carbon-supported Fe-N electrocatalysts synthesized through heat treatment of iron tripyridyl triazine complexes for the PEM fuel cell oxygen reduction reaction [J].
Bezerra, Cicero W. B. ;
Zhang, Lei ;
Lee, Kunchan ;
Liu, Hansan ;
Zhang, Jianlu ;
Shi, Zheng ;
Marques, Aldalea L. B. ;
Marques, Edmar P. ;
Wu, Shaohong ;
Zhang, Jiujun .
ELECTROCHIMICA ACTA, 2008, 53 (26) :7703-7710
[4]   XPS STUDIES OF THE OXYGEN-1S AND OXYGEN-2S LEVELS IN A WIDE-RANGE OF FUNCTIONAL POLYMERS [J].
BRIGGS, D ;
BEAMSON, G .
ANALYTICAL CHEMISTRY, 1993, 65 (11) :1517-1523
[5]   Hydrogen peroxide synthesis: An outlook beyond the anthraquinone process [J].
Campos-Martin, Jose M. ;
Blanco-Brieva, Gema ;
Fierro, Jose L. G. .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2006, 45 (42) :6962-6984
[6]   Origin of the large N is binding energy in X-ray photoelectron spectra of calcined carbonaceous materials [J].
Casanovas, J ;
Ricart, JM ;
Rubio, J ;
Illas, F ;
JimenezMateos, JM .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1996, 118 (34) :8071-8076
[7]   Preparation of carbon alloy catalysts for polymer electrolyte fuel cells from nitrogen-containing rigid-rod polymers [J].
Chokai, Masayuki ;
Taniguchi, Masataka ;
Moriya, Shogo ;
Matsubayashi, Katsuyuki ;
Shinoda, Tsuyoshi ;
Nabae, Yuta ;
Kuroki, Shigeki ;
Hayakawa, Teruaki ;
Kakimoto, Masa-aki ;
Ozaki, Jun-ichi ;
Miyata, Seizo .
JOURNAL OF POWER SOURCES, 2010, 195 (18) :5947-5951
[8]   A multiscale theoretical methodology for the calculation of electrochemical observables from ab initio data: Application to the oxygen reduction reaction in a Pt(111)-based polymer electrolyte membrane fuel cell [J].
de Morais, Rodrigo Ferreira ;
Sautet, Philippe ;
Loffreda, David ;
Franco, Alejandro A. .
ELECTROCHIMICA ACTA, 2011, 56 (28) :10842-10856
[9]   Activity benchmarks and requirements for Pt, Pt-alloy, and non-Pt oxygen reduction catalysts for PEMFCs [J].
Gasteiger, HA ;
Kocha, SS ;
Sompalli, B ;
Wagner, FT .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2005, 56 (1-2) :9-35
[10]   Nitrogen doping effects on the structure of graphene [J].
Geng, Dongsheng ;
Yang, Songlan ;
Zhang, Yong ;
Yang, Jinli ;
Liu, Jian ;
Li, Ruying ;
Sham, Tsun-Kong ;
Sun, Xueliang ;
Ye, Siyu ;
Knights, Shanna .
APPLIED SURFACE SCIENCE, 2011, 257 (21) :9193-9198