Nitrogen-Doped Hollow Carbon Spheres as a Support for Platinum-Based Electrocatalysts

被引:114
作者
Galeano, Carolina [1 ]
Meier, Josef C. [2 ]
Soorholtz, Mario [1 ]
Bongard, Hans [1 ]
Baldizzone, Claudio [2 ]
Mayrhofer, Karl J. J. [2 ]
Schueth, Ferdi [1 ]
机构
[1] Max Planck Inst Kohlenforsch, Dept Heterogeneous Catalysis, D-45470 Mulheim, Germany
[2] Max Planck Inst Eisenforsch GmbH, Dept Interface Chem & Surface Engn, D-40237 Dusseldorf, Germany
来源
ACS CATALYSIS | 2014年 / 4卷 / 11期
关键词
electrocatalysis; nitrogen-doped carbon; platinum nanoparticles; stablity; fuel cells; OXYGEN REDUCTION REACTION; HIGH-SURFACE-AREA; TRANSMISSION ELECTRON-MICROSCOPY; FUEL-CELL ELECTROCATALYST; STABLE ELECTROCATALYSTS; CATALYST DEGRADATION; CNX NANOTUBES; PARTICLE-SIZE; PT-ALLOY; NANOPARTICLES;
D O I
10.1021/cs5003492
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
Platinum and platinum alloys supported on carbon materials are the state of the art electrocatalysts for the essential oxygen reduction reaction (ORR) in low-temperature fuel cells. The limited stability of such materials under the often detrimental operation conditions of fuel cells still remains a critical issue to improve. In this work, we explore the impact of nitrogen-doped carbon supports on the activity and stability of platinum-based fuel cell catalysts. We present a nitrogen-doped mesostructured carbon material, nitrogen-doped hollow carbon spheres (NHCS), as a support for platinum-based electrocatalysts. A detailed study of the electrochemical activity and stability was carried out for two Pt@NHCS materials i.e., as-made material (Pt@NHCS) with a Pt particle size smaller than 2 nm and the corresponding material after thermal treatment at 850 degrees C (Pt@NHCS triangle T) with a Pt particle size of ca. 23 nm. Activity in the ORR was studied by rotating disc electrode (RDE) thin-film measurements, and electrocatalyst stability was evaluated by accelerated aging tests under simulated startstop conditions. The performance of the NHCS-based materials was compared to the two corresponding nitrogen-free materials as well as to a standard Pt/Vulcan catalyst. The underlying degradation mechanisms of Pt@NHCS materials were investigated via identical location electron microscopy. Our results conclusively show that nitrogen doping of the carbon supports can offer benefits for achieving high initial mass activities due to improved high platinum dispersion; however, it was not found to necessarily lead to an improvement of the catalyst stability.
引用
收藏
页码:3856 / 3868
页数:13
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