Local Structure, Electronic Behavior, and Electrocatalytic Reactivity of CO-Reduced Platinum-Iron Oxide Nanoparticles

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	Local Structure, Electronic Behavior, and Electrocatalytic Reactivity of CO-Reduced Platinum-Iron Oxide Nanoparticles
	Duchesne, Paul N. ; Chen, Guangxu ; Zheng, Nanfeng ; Zhang, Peng ; Zheng NF(郑南峰)
刊名	http://dx.doi.org/10.1021/jp4093496
	2013
关键词	RAY-ABSORPTION SPECTROSCOPY OXYGEN REDUCTION FUEL-CELLS ALLOY ELECTROCATALYSTS GROUP METALS CATALYSTS SURFACE TRANSITION DESIGN TEMPERATURE
英文摘要	NSERC Canada; NSERC; University of Washington; Canadian Light Source; APS; U.S. DOE [DE-AC02-06CH11357]; A series of platinum-iron oxide nanoparticles was synthesized using a "clean" CO-reduction method that employed different ratios of Pt-Fe precursor salts in oleylamine at elevated temperatures. High-resolution transmission electron microscopy (HRTEM) and energy-dispersive X-ray spectroscopy (EDS) studies revealed that nearly monodisperse (i.e., with relative standard deviations of less than 15%) nanoparticles with mean diameters of 3.5-4.4 nm and varied elemental compositions (Pt54Fe46 Pt70Fe30, and Pt87Fe13) were obtained. X-ray absorption near-edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) measurements at the Pt L-3- and Fe K-edges revealed that these nanoparticles all consisted of a Pt core with amorphous iron oxide on the surface. Furthermore, it was observed that the local structure (e.g., Pt-Pt bond distance and coordination number) and electronic behavior of the Pt-FeO nanoparticles (e.g., Pt d electron density and Fe valence state) are dependent on the Pt-Fe precursor ratios used in their synthesis. Quantum mechanical ab initio calculations were employed to interpret the results from X-ray spectroscopy and help elucidate the relationships between local structure and electronic properties in the nanoparticle samples. Finally, the surface reactivity of these nanoparticles in the oxygen reduction reaction (ORR) was explored, demonstrating higher electrocatalytic activity for all three platinum-iron oxide samples in comparison with a commercial Pt catalyst. The surface reactivity was also found to be sensitive to the Pt-Fe ratios of the nanoparticles and could be correlated with their local structure and electronic behavior.
语种	英语
出版者	AMER CHEMICAL SOC
内容类型	期刊论文
源URL	[http://dspace.xmu.edu.cn/handle/2288/88716]
专题	化学化工－已发表论文
推荐引用方式 GB/T 7714	Duchesne, Paul N.,Chen, Guangxu,Zheng, Nanfeng,et al. Local Structure, Electronic Behavior, and Electrocatalytic Reactivity of CO-Reduced Platinum-Iron Oxide Nanoparticles[J]. http://dx.doi.org/10.1021/jp4093496,2013.
APA	Duchesne, Paul N.,Chen, Guangxu,Zheng, Nanfeng,Zhang, Peng,&郑南峰.(2013).Local Structure, Electronic Behavior, and Electrocatalytic Reactivity of CO-Reduced Platinum-Iron Oxide Nanoparticles.http://dx.doi.org/10.1021/jp4093496.
MLA	Duchesne, Paul N.,et al."Local Structure, Electronic Behavior, and Electrocatalytic Reactivity of CO-Reduced Platinum-Iron Oxide Nanoparticles".http://dx.doi.org/10.1021/jp4093496 (2013).