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温度对金-铂双金属纳米颗粒合成的影响。

Temperature effect on the synthesis of Au-Pt bimetallic nanoparticles.

作者信息

Garcia-Gutierrez Domingo I, Gutierrez-Wing Claudia E, Giovanetti Lisandro, Ramallo-López José M, Requejo Félix G, Jose-Yacaman Miguel

机构信息

The Texas Materials Institute, The University of Texas at Austin, 1 University Station C2201, Building ETC, Room 8.102, Austin, Texas 78712-1063, USA.

出版信息

J Phys Chem B. 2005 Mar 10;109(9):3813-21. doi: 10.1021/jp048114a.

Abstract

Pt-Au bimetallic nanoparticles have been synthesized by the polyol method and stabilized with poly(vinylpyrrolidone) (PVP), modifying the temperature of synthesis. Interesting structure changes were observed in the nanoparticles as the temperature was varied. At lower temperatures no bimetallic nanoparticles were detected, but as the temperature increased bimetallic nanoparticles started to appear, commonly obtaining core-shell nanoparticles, always covered by the polymer. This originates the modification of the optical response of the system in the UV-visible region. An absorption peak centered at 520 nm at low temperatures was observed (100-110 degrees C); at higher temperatures (130-170 degrees C) there were non detectable absorption peaks, and finally at the two highest temperatures (180-190 degrees C) the reappearance of an absorption feature centered at 510 nm was noticed. These UV-visible results indirectly imply the composition of the surface of the particle. The structure of the particles has been determined using transmission electron microscopy and high-angle annular dark field (HAADF), the latter being a powerful technique to determine the structural composition of the particles and allowing a direct correlation of the optical response with their structural composition. X-ray absorption near-edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) studies were also performed on the samples and their results support the idea of a Pt(core)-Au(shell) structure with the elements segregated from each other. The combination of these experimental techniques with calculated UV-vis absorption spectra allowed, in a reliable way, the elucidation of the nanoparticles structure and elemental distribution.

摘要

通过多元醇法合成了铂-金双金属纳米颗粒,并用聚乙烯吡咯烷酮(PVP)进行稳定化处理,同时改变合成温度。随着温度变化,在纳米颗粒中观察到了有趣的结构变化。在较低温度下未检测到双金属纳米颗粒,但随着温度升高,双金属纳米颗粒开始出现,通常会得到核壳纳米颗粒,且总是被聚合物覆盖。这导致了该体系在紫外-可见光区域的光学响应发生改变。在低温(100-110摄氏度)下观察到一个以520纳米为中心的吸收峰;在较高温度(130-170摄氏度)下没有可检测到的吸收峰,最后在两个最高温度(180-190摄氏度)下,注意到以510纳米为中心的吸收特征再次出现。这些紫外-可见光谱结果间接暗示了颗粒表面的组成。使用透射电子显微镜和高角度环形暗场(HAADF)确定了颗粒的结构,后者是一种确定颗粒结构组成的强大技术,能够将光学响应与其结构组成直接关联起来。还对样品进行了X射线吸收近边结构(XANES)和扩展X射线吸收精细结构(EXAFS)研究,其结果支持了铂(核)-金(壳)结构且元素相互分离的观点。这些实验技术与计算得到的紫外-可见吸收光谱相结合,以可靠的方式阐明了纳米颗粒的结构和元素分布。

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