High durability of carbon nanotube-supported Pt electrocatalysts covered with silica layers for the cathode in a PEMFC

被引：71

作者：

Takenaka, Sakae ^{[1
]}

Matsumori, Hiroshi ^{[1
]}

Matsune, Hideki ^{[1
]}

Tanabe, Eishi ^{[2
]}

Kishida, Masahiro ^{[1
]}

机构：

[1] Kyushu Univ, Grad Sch Engn, Dept Chem Engn, Fukuoka 8190395, Japan

[2] Western Hiroshima Prefecture Ind Inst, Hiroshima 7390046, Japan

来源：

JOURNAL OF THE ELECTROCHEMICAL SOCIETY | 2008年 / 155卷 / 09期

关键词：

D O I：

10.1149/1.2952665

中图分类号：

O646 [电化学、电解、磁化学];

学科分类号：

081704 ;

摘要：

Multiwalled carbon nanotube (CNT)-supported Pt nanoparticles (Pt/CNT) were covered with silica layers by successive hydrolysis of 3-aminopropyl-triethoxysilane and tetraethoxysilane on CNTs with Pt metal precursors, followed by reduction with hydrogen. The Pt/CNT covered with silica layers (SiO2/Pt/CNT) was used as a cathode catalyst for a proton exchange membrane fuel cell (PEMFC). The activity of SiO2/Pt/CNT catalyst for the oxygen reduction reaction in a single-cell PEMFC was similar to that of Pt/CNT, in spite of the uniform coverage of Pt with silica layers, indicating that the coverage of Pt/CNT with silica layers did not appreciably decrease the catalytic activity. In addition, SiO2/Pt/CNT electrocatalyst showed high stability during potential cycling from 0.05 to 1.20 V vs reversible hydrogen electrode in an aqueous H2SO4 electrolyte, whereas Pt/CNT significantly deactivated during the experiment. The structural change of Pt species in these electrocatalysts during potential cycling was investigated by transmission electron microscopy images and Pt L-III-edge X-ray absorption fine structure. The crystallite size of Pt metal in SiO2/Pt/CNT did not change appreciably during the potential cycling, while Pt metal crystallites in Pt/CNT seriously aggregated. Silica layers enveloping Pt metal particles in SiO2/Pt/CNT prevent the dissolution and redeposition of Pt metal particles as well as the agglomeration of Pt metal particles on the supports. (C) 2008 The Electrochemical Society.

引用

页码：B929 / B936

页数：8

共 47 条

[1] DIRECT OBSERVATION OF SURFACE OXIDE FORMATION AND REDUCTION ON PLATINUM CLUSTERS BY TIME-RESOLVED X-RAY-ABSORPTION SPECTROSCOPY [J].

ALLEN, PG ;

CONRADSON, SD ;

WILSON, MS ;

GOTTESFELD, S ;

RAISTRICK, ID ;

VALERIO, J ;

LOVATO, M .

JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1995, 384 (1-2) :99-103

[2] Real-space multiple-scattering calculation and interpretation of x-ray-absorption near-edge structure [J].

Ankudinov, AL ;

Ravel, B ;

Rehr, JJ ;

Conradson, SD .

PHYSICAL REVIEW B, 1998, 58 (12) :7565-7576

[3] THE STRUCTURE AND ACTIVITY OF PT-CO ALLOYS AS OXYGEN REDUCTION ELECTROCATALYSTS [J].

BEARD, BC ;

ROSS, PN .

JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 1990, 137 (11) :3368-3374

[4] Scientific aspects of polymer electrolyte fuel cell durability and degradation [J].

Borup, Rod ;

Meyers, Jeremy ;

Pivovar, Bryan ;

Kim, Yu Seung ;

Mukundan, Rangachary ;

Garland, Nancy ;

Myers, Deborah ;

Wilson, Mahlon ;

Garzon, Fernando ;

Wood, David ;

Zelenay, Piotr ;

More, Karren ;

Stroh, Ken ;

Zawodzinski, Tom ;

Boncella, James ;

McGrath, James E. ;

Inaba, Minoru ;

Miyatake, Kenji ;

Hori, Michio ;

Ota, Kenichiro ;

Ogumi, Zempachi ;

Miyata, Seizo ;

Nishikata, Atsushi ;

Siroma, Zyun ;

Uchimoto, Yoshiharu ;

Yasuda, Kazuaki ;

Kimijima, Ken-ichi ;

Iwashita, Norio .

CHEMICAL REVIEWS, 2007, 107 (10) :3904-3951

[5] CARBON-SUPPORTED PLATINUM CATALYST ELECTRODES - CHARACTERIZATION BY TRANSMISSION ELECTRON-MICROSCOPY, X-RAY-ABSORPTION SPECTROSCOPY, AND ELECTROCHEMICAL HALF-CELL MEASUREMENT ON A PHOSPHORIC-ACID FUEL-CELL [J].

CHANG, JR ;

LEE, JF ;

LIN, SD ;

LIN, AS .

JOURNAL OF PHYSICAL CHEMISTRY, 1995, 99 (40) :14798-14804

[6] Supportless Pt and PtPd nanotubes as electrocatalysts for oxygen-reduction reactions [J].

Chen, Zhongwei ;

Waje, Mahesh ;

Li, Wenzhen ;

Yan, Yushan .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2007, 46 (22) :4060-4063

[7] Durability study Of Pt3Ni1 catalysts as cathode in PEM fuel cells [J].

Colón-Mercado, HR ;

Kim, H ;

Popov, BN .

ELECTROCHEMISTRY COMMUNICATIONS, 2004, 6 (08) :795-799

[8] Instability of Pt/C electrocatalysts in proton exchange membrane fuel cells - A mechanistic investigation [J].

Ferreira, PJ ;

la O', GJ ;

Shao-Horn, Y ;

Morgan, D ;

Makharia, R ;

Kocha, S ;

Gasteiger, HA .

JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 2005, 152 (11) :A2256-A2271

[9]

Fu Q, 2002, NANO LETT, V2, P329, DOI [10.1021/nl025513d, 10.1021/n1025513d]

[10] Heat-treated iron(III) tetramethoxyphenyl porphyrin supported on high-area carbon as an electrocatalyst for oxygen reduction - I. Characterization of the electrocatalyst [J].

Gojkovic, SL ;

Gupta, S ;

Savinell, RF .

JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 1998, 145 (10) :3493-3499

← 1 2 3 4 5 →