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Free Thiols Regulate the Interactions and Self-Assembly of Thiol-Passivated Metal Nanoparticles
Nano Letters ( IF 9.6 ) Pub Date : 2021-02-03 , DOI: 10.1021/acs.nanolett.0c04147
Pan Sun 1 , Linsey M. Nowack 2 , Wei Bu 1 , Mrinal K. Bera 1 , Sean Griesemer 2 , Morgan Reik 2 , Joshua Portner 2 , Stuart A. Rice 2, 3 , Mark L. Schlossman 4 , Binhua Lin 1, 2
Affiliation  

Thiol ligands bound to the metallic core of nanoparticles determine their interactions with the environment and self-assembly. Recent studies suggest that equilibrium between bound and free thiols alters the ligand coverage of the core. Here, X-ray scattering and MD simulations investigate water-supported monolayers of gold-core nanoparticles as a function of the core-ligand coverage that is varied in experiments by adjusting the concentration of total thiols (sum of free and bound thiols). Simulations demonstrate that the presence of free thiols produces a nearly symmetrical coating of ligands on the core. X-ray measurements show that above a critical value of core-ligand coverage the nanoparticle core rises above the water surface, the edge-to-edge distance between neighboring nanoparticles increases, and the nanoparticle coverage of the surface decreases. These results demonstrate the important role of free thiols: they regulate the organization of bound thiols on the core and the interactions of nanoparticles with their surroundings.

中文翻译:

游离硫醇调节硫醇钝化金属纳米粒子的相互作用和自组装。

结合到纳米颗粒金属核上的硫醇配体决定了它们与环境和自组装的相互作用。最近的研究表明,结合的和游离的硫醇之间的平衡会改变核心的配体覆盖率。在这里,X射线散射和MD模拟研究了金核纳米颗粒的水支撑单分子层与核配体覆盖率的函数关系,在实验中,该调整是通过调整总硫醇的浓度(游离和结合的硫醇之和)而改变的。模拟表明,游离硫醇的存在在核心上产生了几乎对称的配体涂层。X射线测量表明,在核心配体覆盖率的临界值以上,纳米粒子核心在水表面上方升高,相邻纳米粒子之间的边到边距离增加,并且表面的纳米颗粒覆盖率降低。这些结果证明了游离硫醇的重要作用:它们调节核心上结合的硫醇的组织以及纳米颗粒与其周围环境的相互作用。
更新日期:2021-02-24
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