从光激发的金属有机框架向Ru2的电子注入可见光驱动进化的二次构建单元
Guangxu Lan1, Yuan-Yuan Zhu1,2, Samuel S Veroneau1
1Department of Chemistry , The University of Chicago , 929 E 57th Street , Chicago , Illinois 60637 , United States.
Journal of the American Chemical Society
|March 27, 2018
概括
我们设计了新的金属有机框架, 这些MOF利用以为基础的二次构建单元和素配体在中性水中增强光催化.
科学领域:
- 材料科学
- 光催化
- 超分子化学
背景情况:
- 金属有机框架 (MOF) 是催化剂的有希望的材料.
- 开发高效的进化反应光催化剂对于可持续能源至关重要.
- 设计具有集成光采集和催化装置的MOF是一个活跃的研究领域.
研究的目的:
- 设计和合成包含Ru2二次构建单元 (SBU) 和氨酸连接体的新型MOF.
- 在这些新的MOF中研究可见光驱动的演化反应 (HER) 的机制.
- 建立用于光催化的多功能MOF的新策略.
主要方法:
- 合成Ru-TBP和Ru-TBP-Zn的MOF.
- 光物理特征 (例如吸收,排放,寿命测量).
- 电化学研究 (例如循环电压测量,光谱电化学) 来探测反应机制.
主要成果:
- 成功设计和合成了两个新的MOF,Ru-TBP和Ru-TBP-Zn.
- 在中性水中证明有效的可见光驱动HER.
- 通过Ru2 SBU确定激发的氧化火,作为最初的步骤,促进多电子转移.
- 阐明了催化循环中的关键中间体的能量.
结论:
- 在设计的MOF中,Ru2SBU和氨酸连接物相邻,可实现高效的光催化HER.
- 氧化灭机制是观察到的高活性的关键.
- 这项工作提出了为先进光催化创造协同效应的MOF的可行策略.
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