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表面修饰合成金属间化合物-铂核壳型催化剂
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摘要
与化学无序的铂合金相比,化学有序的铂金属间化合物具有高合金化程度、均匀元素分布、特定电子结构、高催化活性和耐久性的优点。为提高铂金属间化合物的贵金属铂利用率和进一步提高其氧还原反应活性和耐久性,本文报道了合成由确定组分的金属间化合物为核和紧密排布的表面铂原子为壳构成的核壳型纳米颗粒。我们首先采用改进的多元醇方法制备化学无序的铂合金纳米颗粒,对其在氮气气氛下进行煅烧得到化学有序的铂金属间化合物。然后,对铂金属间化合物进行脱合金处理以及后续低温热处理,最终得到金属间化合物-紧密排布铂原子为壳的核壳结构催化剂。电化学研究表明,与商业Pt/C催化剂相比,所得核壳结构催化剂具有高的氧还原反应活性和耐久性。
Compared with chemical disordered platinum(Pt) alloy, chemically ordered Pt intermetallic possesses advantages of high degree of alloying, uniform elements distribution, specific electronic structure, and excellent electrochemical properties. In order to further improve the Pt utilization and its catalytic activity and durability for oxygen reduction reaction, this paper reported the synthesis of core-shell structure nanoparticles(NPs), which were composed of constituent-defined intermetallic core and closely arranged Pt atoms shell. We firstly synthesized chemically disordered Pt alloy NPs via modified polyol method, which were then annealed under nitrogen atmosphere to give chemically ordered Pt intermetallic NPs. Secondly, the intermetallic NPs were dealloyed by acid leaching followed by low temperature heat treatment to finally obtain intermetallic-Pt core shell structure catalyst. Electrochemical tests showed that the obtained core-shell structure catalyst showed improved catalytic activity and durability for oxygen reduction reaction compared with commercial Pt/C catalyst.
引文
[1]Wang,D.,Xin,H.L.,Hovden,R.,Wang,H.,Yu,Y.,Muller,D.A.,DiS alvo,F.J.,Abruna,H.D.Nat.Mater.2013,12:81.

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