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

一氧化碳 催化作用 纳米颗粒 材料科学 双功能 铂金 化学工程 复合数 碳纤维 化学 无机化学 纳米技术 复合材料 有机化学 工程类
作者
Selim Alayoǧlu,Anand Udaykumar Nilekar,Manos Mavrikakis,Bryan W. Eichhorn
出处
期刊:Nature Materials [Nature Portfolio]
卷期号:7 (4): 333-338 被引量:1203
标识
DOI:10.1038/nmat2156
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 H2 streams containing 1,000 p.p.m. CO, H2 light-off is complete by 30 ∘C, which is significantly better than for traditional PtRu nano-alloys (85 ∘C), monometallic mixtures of nanoparticles (93 ∘C) and pure Pt particles (170 ∘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. To produce hydrogen by reforming hydrocarbons, efficient catalysts capable of removing carbon monoxide are needed. This can now be achieved via a preferential oxidation mechanism using nanoparticle catalysts consisting of a ruthenium core covered with platinum.
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