Size selective incorporation of gold nanoparticles in diblock copolymer vesicle wall.
Size selective incorporation of gold nanoparticles in diblock copolymer vesicle wall.
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DOI：
10.1021/la402132x
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发表时间：
2013-08
期刊：
影响因子：
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通讯作者：
Jiangping Xu;Yuanyuan Han;J. Cui;Wei Jiang
中科院分区：
文献类型：
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作者：
Jiangping Xu;Yuanyuan Han;J. Cui;Wei Jiang
通过实验和自洽场模拟相结合的方法，系统地研究了聚合物泡囊壁在多大程度上可以嵌入不同尺寸的金纳米颗粒。实验和模拟结果都表明，AuNPs在囊壁或球形胶束中的位置与大小密切相关。AuNPs是否进入囊泡壁取决于AuNPs直径(D0)与囊泡壁厚度(d(W0))的比值。D0/d(W0)和lt；0.3的1-十二硫醇包覆的AuNPs(Au(X)R)将稳定地分散在囊壁中。对于聚苯乙烯包覆的金纳米粒子(Au(X)S)，根据相图提出了D0/d(W0)的判据，即D0/d(W0)<；0.5的Au(X)S粒子可以位于囊壁。反之，Au(X)R和Au(X)S更倾向于定位在球形胶束中。此外，还分别计算了体系的总自由能的贡献，揭示了AuNPs尺寸选择性分布的机理。结果表明，金纳米粒子从囊壁中逸出并在球形胶束中选择性分布是一个由熵驱动的过程。我们的研究为在稀溶液中制备纳米粒子/嵌段共聚聚合物杂化囊泡提供了重要的指导。
A systematic study is conducted to reveal how far the polymeric vesicle wall can embed gold nanoparticles (AuNPs) with different sizes by combining experiments and self-consistent field simulations. Both the experimental and simulative results indicate that the location of AuNPs in vesicle wall or in spherical micelle is heavily size dependent. Whether the AuNPs enter the vesicle wall or not is determined by a ratio of the diameter of AuNPs (D0) to the thickness of the vesicle wall (d(w0)). The 1-dodecanethiol-coated AuNPs (Au(x)R) with D0/d(w0) < 0.3 will stably disperse in the vesicle walls. For polystyrene-coated AuNPs (Au(x)S), a criterion of D0/d(w0) is proposed based on the phase diagram; i.e., the Au(x)S with D0/d(w0) < 0.5 can be located in the vesicle wall. Otherwise, the Au(x)R and the Au(x)S prefer to locate in spherical micelles. Moreover, the contributions of enthalpy and entropy to the total free energy of the system are respectively calculated to reveal the mechanism of the size selective distribution of AuNPs. The results demonstrate that the escape of AuNPs from vesicle walls and their selective distribution in spherical micelles is an entropy-driven process. Our study provides an important guideline for fabricating nanoparticle/block copolymer hybrid vesicles in dilute solution.