Electrocatalytic Activity and Stability of Nitrogen-Containing Carbon Nanotubes in the Oxygen Reduction Reaction

被引：511

作者：

Kundu, Shankhamala ^{[1
]}

Nagaiah, Tharamani Chikka

Xia, Wei ^{[1
]}

Wang, Yuemin ^{[1
]}

Van Dommele, Stefan ^{[2
]}

Bitter, Johannes Hendrik ^{[2
]}

Santa, Monika ^{[3
]}

Grundmeier, Guido ^{[3
]}

Bron, Michael ^{[1
]}

Schuhmann, Wolfgang

Muhler, Martin ^{[1
]}

机构：

[1] Ruhr Univ Bochum, Lab Ind Chem, D-44780 Bochum, Germany

[2] Univ Utrecht, Utrecht, Netherlands

[3] Max Planck Inst Eisenforsch GmbH, D-40237 Dusseldorf, Germany

来源：

JOURNAL OF PHYSICAL CHEMISTRY C | 2009年 / 113卷 / 32期

关键词：

IRON PHENANTHROLINE COMPLEXES; ELECTROLYTE FUEL-CELLS; HEAT-TREATED IRON; REACTION CATALYSTS; RAMAN MICROPROBE; O-2; REDUCTION; AREA CARBON; SURFACE; BLACK; FILMS;

D O I：

10.1021/jp811320d

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：

Nitrogen-containing carbon nanotubes (NCNTs) were prepared via pyrolysis of acetonitrile over cobalt catalysts at different temperatures to control the nitrogen content. The changes in the chemical and structural properties of undoped CNTs and NCNTs were investigated using high-resolution X-ray photoelectron and Raman spectroscopy. The NCNTs prepared at 550 degrees C had a higher amount of pyridinic groups and edge plane exposure than the ones prepared at 750 degrees C. The thermal stability and transformation of these nitrogen functional groups was studied using deconvoluted XP N 1s spectra. The NCNTs show a considerably higher activity in the oxygen reduction reaction in acidic electrolyte compared with undoped CNTs as demonstrated by cyclic voltammetry, rotating disk electrode measurements, and the redox-competition mode of scanning electrochemical microscopy (RC-SECM). Particularly, the NCNT sample prepared at 550 degrees C exhibited the highest activity, which was about 1 order of magnitude lower than that of a commercial Pt/C sample containing 20 wt % Pt. The oxygen reduction reaction (ORR) performance of this sample showed hardly any signs of deterioration after 3 days, as determined by voltammetric stability tests in H2SO4.

引用

页码：14302 / 14310

页数：9

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