Role of Electronic Perturbation in Stability and Activity of Pt-Based Alloy Nanocatalysts for Oxygen Reduction

被引：253

作者：

Hwang, Seung Jun ^{[1
]}

Kim, Soo-Kil ^{[1
,3
]}

Lee, June-Gunn ^{[2
]}

Lee, Seung-Cheol ^{[2
]}

Jang, Jong Hyun ^{[1
]}

Kim, Pil ^{[6
]}

Lim, Tae-Hoon ^{[1
]}

Sung, Yung-Eun ^{[4
,5
]}

Yoo, Sung Jong ^{[1
]}

机构：

[1] Korea Inst Sci & Technol, Fuel Cell Res Ctr, Seoul 136791, South Korea

[2] Korea Inst Sci & Technol, Computat Sci Ctr, Seoul 136791, South Korea

[3] Chung Ang Univ, Sch Integrat Engn, Seoul 156756, South Korea

[4] Seoul Natl Univ, IBS, Ctr Nanoparticle Res, Seoul 151742, South Korea

[5] Seoul Natl Univ, Sch Chem Biol Engn, Seoul 151742, South Korea

[6] Chonbuk Natl Univ, Sch Chem Engn, Dept Hydrogen & Fuel Cell Engn, Jeonju, Jeonbuk, South Korea

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2012年 / 134卷 / 48期

关键词：

DENSITY-FUNCTIONAL THEORY; SURFACE-COMPOSITION; PLATINUM; ELECTROCATALYSIS; CATALYST; DISSOLUTION; TRENDS; METAL; ELECTROREDUCTION; SPECTROSCOPY;

D O I：

10.1021/ja307951y

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

The design of electrocatalysts for polymer electrolyte membrane fuel cells must satsify two equally important fundamental principles: optimization of electrocatalytic activity and long-term stability in acid media (pH <1) at high potential (0.8 V). We report here a solution-based approach to the preparation of Pt-based alloy with early transition metals and realistic parameters for the stability and activity of Pt3M (M = Y, Zr, Ti, Ni, and Co) nanocatalysts for oxygen reduction reaction (ORR). The enhanced stability and activity of Pt-based alloy nanocatalysts in ORR and the relationship between electronic structure modification and stability were studied by experiment and DFT calculations. Stability correlates with the d-band fillings and the heat of alloy formation of Pt3M alloys, which in turn depends on the degree of the electronic perturbation due to alloying. This concept provides realistic parameters for rational catalyst design in Pt-based alloy systems.

引用

页码：19508 / 19511

页数：4

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