机械化学法合成金纳米粒子的热力学模型：对无溶剂法制备纳米粒子的启示
A Thermodynamics Model for Mechanochemical Synthesis of Gold Nanoparticles: Implications for Solvent-free Nanoparticle Production
摘要：
机械化学正在成为一种可持续的固相合成纳米材料和分子的方法，从活性药物成分到清洁技术材料。然而，我们仍然缺乏一个很好的模型来合理化实验观察，并在机械辅助固相纳米粒子合成过程中发挥作用的因素的机械理解。本文提出了一个结构相场晶体（XPFC）模型与弹道驱动力来描述这样一个过程，与金纳米粒子的生长在两个组件的混合物的具体例子。在模型的自由能背景下描述反应路径，并根据与实验条件密切对应的唯象模型参数进行动力学模拟，从而得出纳米颗粒生长动力学的结论。结果表明，弹道长期降低反应的活化能垒，使反应在一个温度制度与实验观察兼容。该模型还解释了与实验观察相一致的沉淀晶粒尺寸减小的机制。我们的模拟结果为机械合成提供了新的机理见解，并对纳米粒子的生产及其他方面产生了影响。
英文摘要：
Mechanochemistry is becoming an established method for the sustainable, solid-phase synthesis of scores of nano-materials and molecules, ranging from active pharmaceutical ingredients to materials for cleantech. Yet we are still lacking a good model to rationalize experimental observations and develop a mechanistic understanding of the factors at play during mechanically assisted, solid-phase nanoparticle synthesis. We propose herein a structural-phase-field-crystal (XPFC) model with a ballistic driving force to describe such a process, with the specific example of the growth of gold nanoparticles in a two component mixture. The reaction path is described in the context of free energy landscape of the model, and dynamical simulations are performed based on phenomenological model parameters closely corresponding to the experimental conditions, so as to draw conclusions on nanoparticle growth dynamics. It is shown that the ballistic term lowers the activation energy barrier of reaction, enabling the reaction in a temperature regime compatible with experimental observations. The model also explains the mechanism of precipitated grain size reduction that is consistent with experimental observations. Our simulation results afford novel mechanistic insights into mechanosynthesis with implications for nanaparticle production and beyond.
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