在小金酸盐纳米集群中分子级联体效应
Daniel M Chevrier1, Lluís Raich2, Carme Rovira2,3
1Department of Chemistry , Dalhousie University , Halifax , Nova Scotia B3H 4R2 , Canada.
Journal of the American Chemical Society
|October 20, 2018
概括
黄金纳米集群上的保护性联体 (AuNC) 显著影响其结构和特性. 不同的配体,如环乙醇和谷,产生不同的表面特性,影响它们作为催化剂或生物医学应用.
科学领域:
- 纳米材料科学
- 表面化学
- 计算化学
背景情况:
- 硫酸盐保护的金纳米集群具有很大的表面积与体积比,使其表面连接物对调节性质至关重要.
- 在催化和传感应用中,了解体诱导的原子层结构变化对于优化Au NC至关重要.
- 目前关于特定的硫酸盐配体如何影响Au NC结构和溶液相行为的知识有限.
研究的目的:
- 研究不同保护对小金纳米集群 (Au18(SR) 14的结构和特性的影响.
- 阐明联体选择如何影响不同溶剂环境 (烯和水) 中的 Au NC 行为.
- 将结构发现与催化和生物医学中的潜在应用联系起来.
主要方法:
- 综合实验同步射线光谱与理论量子力学/分子力学 (QM/MM) 模拟.
- 研究了两种代表性配体:环乙醇酸 (异质) 和氨酸 (水友性).
- 在固体和溶液阶段分析了Au NC结构.
主要成果:
- 循环乙酸被多烯显著扰乱,在Au18上产生表面空洞和乱,这表明具有催化潜力.
- 在Au NC核心周围形成一个保护性外,最大限度地减少了溶剂诱导的结构变化,从而形成了硬化的表面.
- 这些AUNC的高稳定性和增强光发性在生物医学应用中可以由谷氨的优越保护来解释.
结论:
- 结合剂的选择决定了溶液中的 Au NC 的结构完整性和表面可达性.
- 环乙烯酸促进小分子相互作用,适合催化应用.
- 谷氨配体提供强大的封装,增强生物医学用途的稳定性和光发光.
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