在Au25 (SR) 18和Ag44 (SR) 30之间发生的集群间反应
K R Krishnadas1, Atanu Ghosh1, Ananya Baksi1
1DST Unit of Nanoscience (DST UNS) and Thematic Unit of Excellence, Department of Chemistry, Indian Institute of Technology Madras , Chennai, 600 036, India.
Journal of the American Chemical Society
|December 19, 2015
概括
贵金属集群经历自发的集群反应,交换原子和配体. 这一发现为合金和兴奋剂提供了方便的途径,推进了单层保护集群化学.
科学领域:
- 纳米化学
- 材料科学
- 物理化学
背景情况:
- 单层保护集群 (MPC) 是具有独特性质的原子精确纳米材料.
- 单个MPC之间的相互作用对于开发新材料和应用至关重要.
- 了解MPC中的反应机制对于它们的可控合成和功能化至关重要.
研究的目的:
- 展示原子精确的贵金属集群之间的集群反应的第一个例子.
- 研究这些反应的机制和热力学可行性.
- 探索集群间反应的合金化和异原子兴奋剂的潜力.
主要方法:
- 采用金 (Au25(SR) 18) 和银 (Ag44(SR) 30) 集群作为模型系统.
- 使用电喷离子和矩阵辅助激光脱离/离子质谱分析反应产物.
- 进行密度函数理论 (DFT) 计算以评估热力学可行性并提出反应机制.
主要成果:
- 在环境条件下观察到Au和Ag集群之间的自发集群反应.
- 在反应过程中证明了金属原子和配体交换.
- 轻易地将银的异原子化成黄金集群,包含多达20个银原子.
- 确定金属核-硫酸盐接口对反应启动和动力学至关重要.
结论:
- 集群间反应是制造合金贵金属集群的新途径.
- 这种方法为使用不同金属原子的MPC提供了一个有效的途径.
- 这些发现为单层保护集群及其应用奠定了基础.
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