通过合成后取消在金属有机框架中产生明确的hexabenzocoronene
Jun-Sheng Qin1,2, Shuai Yuan1,3, Lei Zhang4
1Department of Chemistry , Texas A&M University , College Station , Texas 77843-3255 , United States.
Journal of the American Chemical Society
|January 10, 2019
概括
这项研究合成了一种基于的新型金属有机框架 (MOF),PCN-136,使用后合成修饰策略创建大型π结合系统. 这种增强的MOF表现出更好的光反应性质,并且在可见光下显示出高效的光催化二氧化碳减排.
科学领域:
- 材料科学
- 纳米技术
- 摄影化学
背景情况:
- 在金属有机框架 (MOF) 中结合大的 π 结合联体可以增强光物理和电化学特性.
- 在MOF中,强大的π-π相互作用和低溶解度的联联体往往阻碍了这些效应.
- 制定克服这些局限性的策略对于设计先进的功能MOF至关重要.
研究的目的:
- 合成一种基于的新型MOF (PCN-136),其中含有大量π-结合的六子.
- 通过后合成修饰方法克服与配体溶解性和π-π堆叠相关的挑战.
- 研究合成的MOF的增强光反应性质和光催化活性,以减少二氧化碳.
主要方法:
- 含有六片段的预制MOF (pbz-MOF-1) 的合成
- 芳香化驱动的后合成无效化,在MOF框架内形成六子冠链接体,从而产生PCN-136.
- 单晶X射线晶体,以确认结构转变和扩展π-结合的形成.
- 在可见光照射下对二氧化碳减少进行光催化评估.
主要成果:
- 通过单晶到单晶的合成后转化成功合成PCN-136,避免直接组装问题.
- 在MOF链接器中形成扩展的π-结合系统,显著增强光响应性.
- PCN-136在减少二氧化碳方面表现出高效的光催化作用,其性能优于前体MOF (pbz-MOF-1).
结论:
- 合成后修饰是一种有效的策略,可以将大型π结合系统纳入MOF,同时减轻可溶性和聚合问题.
- 由此产生的MOF,PCN-136,由于其扩展的π-结合,具有卓越的光响应特性.
- PCN-136作为可见光驱动的二氧化碳减排的有希望的固有光催化剂,突出了其在可持续化学中的潜力.
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