卤化物作为纳米颗粒生长中的形状导向剂的功效的计算评估
A Computational Assessment of the Efficacy of Halides as Shape-Directing Agents in Nanoparticle Growth
摘要：
我们报告了一个全面的研究，解决了几个限制，阻碍使用原子模型作为工具，用于理解和改善湿化学合成和相关应用的金和钯纳米粒子的水溶液卤化物吸附。结合热力学建模与密度泛函理论（DFT）计算和实验数据被用来预测平衡形状的卤化物覆盖的纳米粒子作为化学环境的函数。为了确保现实和实验相关的结果，我们考虑溶剂的影响，包括一个大的邻位表面，几个吸附物覆盖以及十面体颗粒。虽然所观察到的稳定性不足以导致各向异性形状如纳米立方体的热力学稳定性，但卤化物覆盖的不均匀性表明获得这种形状作为动力学产物的可能性。关于技术挑战，我们表明，包括表面-溶剂相互作用导致预测形状的质的变化。此外，占非本地的功能水平上的相互作用产生更准确的描述表面系统。
英文摘要：
We report a comprehensive study of aqueous halide adsorption on nanoparticles of gold and palladium that addresses several limitations hampering the use of atomistic modeling as a tool for understanding and improving wet-chemical synthesis and related applications. A combination of thermodynamic modeling with density functional theory (DFT) calculations and experimental data is used to predict equilibrium shapes of halide-covered nanoparticles as a function of the chemical environment. To ensure realistic and experimentally relevant results, we account for solvent effects and include a large set of vicinal surfaces, several adsorbate coverages as well as decahedral particles. While the observed stabilization is not significant enough to result in thermodynamic stability of anisotropic shapes such as nanocubes, non-uniformity in the halide coverage indicates the possibility of obtaining such shapes as kinetic products. With regard to technical challenges, we show that inclusion of surface-solvent interactions lead to qualitative changes in the predicted shape. Furthermore, accounting for non-local interactions on the functional level yields a more accurate description of surface systems.
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