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首页> 外文期刊>Advanced energy materials >Tailor-Made Photoconductive Pyrene-Based Covalent Organic Frameworks for Visible-Light Driven Hydrogen Generation
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Tailor-Made Photoconductive Pyrene-Based Covalent Organic Frameworks for Visible-Light Driven Hydrogen Generation

机译：量身定制的基于光导P的可见光驱动氢共价有机骨架

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Covalent organic frameworks (COFs) have emerged as a new class of crystalline porous polymers displaying molecular tunability combined with structural definition. Here, a series of three conjugated, photoactive azine-linked COFs based on pyrene building blocks which differ in the number of nitrogen atoms in the peripheral aromatic units is presented. The structure of the COFs is analyzed by combined experimental and computational physisorption as well as quantum-chemical calculations, which suggest a slipped-stacked arrangement of the 2D layers. Photocurrents of up to 6 mu A cm(-2) with subsecond photoresponse times are measured on thin film samples for the first time. While all COFs are capable of producing hydrogen from water, their efficiency increases significantly with decreasing number of nitrogen atoms. The trending activities are rationalized by photoelectrochemical measurements and quantum-chemical calculations which suggest an increase in the thermodynamic driving force with decreasing nitrogen content to be the origin of the observed differences in hydrogen evolution activities.
机译：共价有机骨架（COF）已作为一类新的结晶多孔聚合物出现，该聚合物显示出分子可调性和结构定义。在此，提出了一系列基于pyr结构单元的共轭的三个共轭的，光敏性的嗪连接的COF，它们的周边芳族单元中的氮原子数不同。通过结合实验和计算的物理吸附以及量子化学计算来分析COF的结构，这表明二维层的滑动堆叠排列。首次在薄膜样品上测量亚秒级光响应时间下高达6μA cm（-2）的光电流。尽管所有COF都能够从水中产生氢，但其效率随着氮原子数量的减少而显着提高。通过光电化学测量和量子化学计算可以合理化趋势活动，这表明随着氮含量的降低，热力学驱动力的增加是观察到的氢逸出活动差异的根源。

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