超声辐射功率对声化学合成金纳米粒子的影响
Effect of ultrasonic irradiation power on sonochemical synthesis of gold nanoparticles
摘要：
在这项工作中，优化的尺寸分布和光学性质的胶体合成金纳米粒子（GNP）的使用建议的超声Tuerkevich-Frens方法。三个超声（20 kHz）辐照功率的效果进行了分析，作为尺寸和形状控制参数。GNP胶体溶液由氯金酸（HAuCl $_{4}$）和柠檬酸三钠（$\rm C_{6}H_{5}Na_{3}O_{7}\cdot 2H_{2}O$）在连续照射1小时下获得，无需任何加热或搅拌。每隔10分钟在UV-Vis光谱中监测表面等离子体共振（SPR），以发现局部SPR波长（$λ_{\rm LSPR}$）的最佳时间，并且210样品程序将$λ_{\rm LSPR}$局部化减少到20分钟，而150和60样品在60分钟内显示出$λ_{\rm LSPR}$。GNP的成核和生长表现出形状和尺寸分布的变化，这与溶液中的物理（空化，温度）和化学（自由基生成，pH值）条件有关。结果显示准球形GNP为五角十二面体（$λ_{\rm LSPR}$ =560 nm）、三角二十面体（$λ_{\rm LSPR}$ =535 nm）和四角六面体（$λ_{\rm LSPR}$ = 525 nm），尺寸范围为12-16 nm。超声辐照引起AuCl $_{2}^-$的电子在金表面迅速交换。在AuCl $_{4}^-$和Cl $^-$脱附后，配合物四氯金酸盐被柠檬酸盐还原，配合物AuCl $_{2}^-$之间的亲金作用，电子交换和金种子，新的金原子在表面的沉积促进了GNP的生长。这些机制通过空化效应和将能量传输到溶液中来增强，表明可以用这种简单的方法和最少的干扰来调节来自我们的纳米颗粒的等离子体响应。
英文摘要：
In this work, optimized size distribution and optical properties in colloidal synthesis of gold nanoparticles (GNPs) were obtained using a proposed ultrasonic Tuerkevich-Frens method. The effect of three ultrasound (20 kHz) irradiation powers has been analyzed as size and shape control parameter. The GNPs colloidal solutions were obtained from chloroauric acid (HAuCl$_{4}$) and trisodium citrate ($\rm C_{6}H_{5}Na_{3}O_{7}\cdot 2H_{2}O$) under continuous irradiation for 1 hour without any heat or stirring. The surface plasmon resonance (SPR) was monitored in the UV-Vis spectra every 10 minutes to found the optimal time for localized SPR wavelength ($λ_{\rm LSPR}$) and the 210 sample procedure reduces the $λ_{\rm LSPR}$ localization to 20 minutes, while 150 and 60 samples show $λ_{\rm LSPR}$ in 60 minutes. The nucleation and growth of GNPs showed changes in shape and size distribution, which were associated with physical (cavitation, temperature) and chemical (radical generation, pH) conditions in the solution. The results showed quasispherical GNPs as pentakis dodecahedron ($λ_{\rm LSPR}$=560 nm), triakis icosahedron ($λ_{\rm LSPR}$=535 nm), and tetrakis hexahedron ($λ_{\rm LSPR}$= 525 nm) in a size range from 12-16 nm. US irradiation induced a disproportionation process, electrons of AuCl$_{2}^-$ rapidly exchanged through the gold surface. After AuCl$_{4}^-$ and Cl$^-$ are desorbed and a complex tetrachloroaurate is recycled for the two-electron reduction by citrate, aurophilic interaction between complexes AuCl$_{2}^-$, electrons exchange and gold seeds, the deposition of new gold atoms on the surface promoting the growth of GNPs. These mechanisms are enhanced by the cavitation effects and transmitted energy into the solution, showing that the plasmonic response from our nanoparticles can be tuned with this simple method and minimum intrumentation.
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