Ru-Pt core-shell nanoparticles for preferential oxidation of carbon monoxide in hydrogen

被引:1191
作者
Alayoglu, Selim [1 ]
Nilekar, Anand U. [2 ]
Mavrikakis, Manos [2 ]
Eichhorn, Bryan [1 ]
机构
[1] Univ Maryland, Dept Chem & Biochem, College Pk, MD 20742 USA
[2] Univ Wisconsin, Dept Chem & Biol Engn, Madison, WI 53706 USA
关键词
D O I
10.1038/nmat2156
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 [物理化学]; 081704 [应用化学];
摘要
Most of the world's hydrogen supply is currently obtained by reforming hydrocarbons. 'Reformate' hydrogen contains significant quantities of CO that poison current hydrogen fuel-cell devices. Catalysts are needed to remove CO from hydrogen through selective oxidation. Here, we report first-principles-guided synthesis of a nanoparticle catalyst comprising a Ru core covered with an approximately 1-2-monolayer-thick shell of Pt atoms. The distinct catalytic properties of these well-characterized core-shell nanoparticles were demonstrated for preferential CO oxidation in hydrogen feeds and subsequent hydrogen light-off. For H-2 streams containing 1,000 p. p. m. CO, H-2 light-off is complete by 30 degrees C, which is significantly better than for traditional PtRu nano-alloys (85 degrees C), monometallic mixtures of nanoparticles (93 degrees C) and pure Pt particles (170 degrees C). Density functional theory studies suggest that the enhanced catalytic activity for the core-shell nanoparticle originates from a combination of an increased availability of CO-free Pt surface sites on the Ru@Pt nanoparticles and a hydrogen-mediated low-temperature CO oxidation process that is clearly distinct from the traditional bifunctional CO oxidation mechanism.
引用
收藏
页码:333 / 338
页数:6
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