通过氧活性宿主吸收,捕获和释放有机金属酸
Iram F Mansoor1, Kaitlyn G Dutton1, Daniel A Rothschild1
1Department of Chemistry and Chemical Biology, Rutgers, The State University of New Jersey, 123 Bevier Road, Piscataway, New Jersey 08854, United States.
Journal of the American Chemical Society
|October 1, 2021
概括
研究人员开发了金属有机纳米, 通过微妙的刺激来精确控制客人的释放,
科学领域:
- 超分子化学
- 材料科学
- 纳米技术
背景情况:
- 主机-客人化学通常依赖于热力学上有利的客人吸收和释放的相互作用.
- 通过打开/关闭互动来控制客人的亲和力是纳米设计的一个关键挑战.
研究的目的:
- 设计金属有机纳米, 能够在热力学不利的环境中捕捉客人.
- 通过动力效应和微妙的刺激来控制客人的释放.
主要方法:
- 氨酸壁的阴离子纳米镜 (1a和1b主体) 的合成.
- 为快速吸收有机金属离子 (Cp*2Co+和Cp2Co+),将宿主降低到体状态.
- 使用银 (I) 离子 (Ag+) 重氧化宿主形成转移稳定的复合物.
- 实验和密度功能理论 (DFT) 研究以分析结合亲和和稳定机制.
主要成果:
- 减少的主体1a和1b迅速吸收有机金属酸Cp*2Co+和Cp2Co+.
- 与Ag+的再氧化捕获客体,形成一个月以上持久的转移稳定的阴离子-阴离子复合体 (Cp*2Co@1a和Cp2Co@1b).
- 通过静电相互作用和形状变化,PF6-离子动态稳定Cp*2Co@1a.
- 使用铁 (Fc+) 进行再氧化,与Ag+相比加速解离200倍.
结论:
- 在金属有机纳米中限制客人的新方法.
- 突出了动力效应和特定的 counterions 在稳定转移性宿主-客群的作用.
- 展示了超稳定复合体可以响应比热力学上有利的系统更微妙的刺激.
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