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负载于落叶松阿拉伯半乳聚糖的钯纳米颗粒的胶态聚集体。

Colloidal aggregates of Pd nanoparticles supported by larch arabinogalactan.

机构信息

Institute of Macromolecular Compounds, Russian Academy of Sciences, Bolshoy Prospekt, 31, 199004 St.-Petersburg, Russia.

出版信息

J Phys Chem B. 2013 Feb 21;117(7):2134-41. doi: 10.1021/jp3118242. Epub 2013 Feb 11.

Abstract

Palladium nanoparticles (PdNPs) are used in catalysis, hydrogen storage, biomedicine, and so on. Arranging the self-assembly of PdNPs within colloidal aggregates is desirable for improving their consumer properties. Stable widely dispersed colloidal aggregates of larch arabinogalactan (LARB) containing nanosized (5-nm) PdNPs were obtained by reducing Pd ions in alkaline solutions of LARB. Centrifugation resulted in a set of LARB-PdNP colloids ranging from 60 to 240 nm. The colloids were studied by static light scattering (SLS) and dynamic light scattering (DLS). The SLS data presented as Kratki plots correspond to a particle scattering factor of linear rather than branched chains. The fractal dimension of the LARB-PdNP colloids was found by SLS to be d = 1.96, which is between the values for diffusion- and reaction-limited aggregation. This result is ascribed to the aggregate's internal motion, which is evident from the power-law exponent of the dependence of the DLS relaxation rate on the scattering vector, <Γ> ~ q(α) with α = 2.24. The structure-sensitive ratio of the radius of gyration to the hydrodynamic radius was found to vary within the interval of 0.8 ≤ R(g)/R(h) ≤ 1.2 corresponding, to the spherical form of LARB-PdNP colloids. A spiderweblike PdNP distribution pattern was observed by transmission electron microscopy. Insertion of PdNPs did not affect the fractal dimension, the power-law exponent α, or the architecture of the pristine LARB aggregates in water. The red shift of the surface plasmon extinction observed with increasing LARB-PdNP colloidal size indicates the collective optical response of the PdNP ensemble in the colloid.

摘要

钯纳米粒子(PdNPs)在催化、储氢、生物医药等领域得到了广泛应用。在胶体聚集体中排列 PdNPs 的自组装,有利于提高其消费性能。通过在 LARB 的碱性溶液中还原 Pd 离子,得到了含有纳米级(5nm)PdNPs 的稳定、广泛分散的 LARB 胶体聚集体。离心后得到一组 LARB-PdNP 胶体,粒径范围从 60nm 到 240nm。通过静态光散射(SLS)和动态光散射(DLS)研究胶体。SLS 数据以 Kratki 图表示,对应于线性而非支化链的粒子散射因子。通过 SLS 发现 LARB-PdNP 胶体的分形维数为 d=1.96,介于扩散和反应限制聚集之间。这一结果归因于聚集体的内部运动,这从 DLS 弛豫速率对散射矢量的幂律指数<Γ>~q(α),α=2.24 中可以明显看出。发现旋转半径与水动力半径的结构敏感比在 0.8≤R(g)/R(h)≤1.2 的范围内变化,对应于 LARB-PdNP 胶体的球形形式。透射电子显微镜观察到蜘蛛网状 PdNP 分布模式。PdNP 的插入并没有影响到原始 LARB 聚集在水中的分形维数、幂律指数α或结构。随着 LARB-PdNP 胶体尺寸的增加,观察到表面等离子体消光的红移,表明胶体中 PdNP 集合体的集体光学响应。

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