原子精确的Ag29纳米集群的结构变化在次要联体的顺序连接和分离后
Jayoti Roy1, Amitabha Das2, Arijit Jana1
1DST Unit of Nanoscience (DST UNS) & Thematic Unit of Excellence (TUE), Department of Chemistry, Indian Institute of Technology Madras, Chennai 600036, India.
ACS nano
|January 28, 2025
概括
贵金属纳米集群 ([Ag29(L) [12]3-) 在与二次连接体 (L') 相互作用时经历结构变化. 添加更多的L'联体逐渐扩大纳米集群框架,即使在脱离后也留下结构足迹.
科学领域:
- 纳米材料科学 科学 纳米材料科学
- 表面化学 表面化学
- 计算化学的计算化学
背景情况:
- 了解联体稳定贵金属纳米集群 (NCs) 的结构动力学对于其应用至关重要.
- 干重组显著影响了在NCs中观察到的结构变化.
- 在NC表面上初级和二级配体之间的相互作用是研究的一个关键领域.
研究的目的:
- 为了研究联结体保护的[Ag29(L) 12) 3-NCs与二次联结体 (L') 相互作用时的动态行为.
- 为了描述基于NC的添加物的结构性质[Ag29(L) [12]L'n3-对于n=1-4.4的情况.
- 阐明NCs和二次连接体之间的非共价相互作用的性质.
主要方法:
- 实验技术:紫外可见 (UV-vis) 光谱学,高分辨率电喷射电离化质谱学 (ESI MS) 和离子移动性质谱学 (IM MS).
- 结合MS/MS IMS实验被用来探测碎片化行为.
- 计算方法:密度函数理论 (DFT) 的计算用于预测结构和相互作用.
主要成果:
- 实验确定的碰撞截面 (CCS) 显示,随着二次配体数量的单调增加 (n=1-4).
- DFT计算表明NCs和二次连接体之间存在弱非共价相互作用.
- 观察到NC的Ag-S主干框架的逐步扩展,并增加了二级配体的添加.
结论:
- 其次性连接物添加导致[Ag29(L) 12) 3 -纳米集群的显著结构变化.
- 观察到的结构变化与弱非共价相互作用和框架扩张相一致.
- 通过碰撞加热的二次带的气相分离会在纳米集群表面留下持久的结构"足迹".
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