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首页> 外文期刊>Advanced Functional Materials >Substantial Cyano-Substituted Fully sp(2)-Carbon-Linked Framework: Metal-Free Approach and Visible-Light-Driven Hydrogen Evolution
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Substantial Cyano-Substituted Fully sp(2)-Carbon-Linked Framework: Metal-Free Approach and Visible-Light-Driven Hydrogen Evolution

机译：大量用氰基取代的完全sp（2）-碳链接的框架：无金属方法和可见光驱动的氢气释放

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摘要

Polymeric semiconductors are emerging as a kind of competitive photocatalysts for hydrogen evolution due to their well-tunable structures, versatile functionalization, and low-cost processibility. In this work, a series of conjugated porous polymers with substantial cyano-substituted fully sp(2)-carbon frameworks are efficiently synthesized by using electron-deficient tricyanomesitylene as a key building block to promote an organic base-catalyzed Knoevenagel condensation with various aldehyde-substituted arenes. The resulting porous polymers feature donor-acceptor structures with-extended conjugation, rendering them with distinct semiconducting properties. They possess hierarchically porous structures, nanoscale morphologies, and intriguing wettability. These promising physical characters, finely tailorable by varying the arene units, are essentially relevant to the abundant cynao substituents over the whole frameworks. The as-prepared porous polymers exhibit excellent visible-light-driven photocatalytic activity for water-splitting hydrogen evolution with apparent quantum yield up to 2.0% at 420 nm or 1.9% at 470 nm, among the highest values yet reported for porous polymer-based photocatalysts, also representing the first example of such kinds of catalysts formed through a metal-free-catalyzed carbon-carbon coupling reaction.
机译：高分子半导体由于其结构良好的可调性，多功能的功能性和低成本的可加工性，正逐渐成为一种竞争性的氢析出光催化剂。在这项工作中，通过使用缺电子的三氰基三苯甲基作为关键的结构单元来促进有机碱催化的Knoevenagel与各种醛的缩合反应，可以有效地合成一系列具有大量氰基取代的全sp（2）-碳骨架的共轭多孔聚合物。取代的芳烃。所得的多孔聚合物的特征在于供体-受体结构具有扩展的共轭，使它们具有独特的半导体性能。它们具有分层的多孔结构，纳米级的形态和引人入胜的润湿性。这些有前途的物理特征，可通过改变芳烃单元进行精细调整，与整个框架上大量的西诺取代基本质上相关。所制备的多孔聚合物表现出出色的可见光驱动光分解水分解氢的光催化活性，表观量子产率在420 nm时高达2.0％或在470 nm时高达1.9％，是基于多孔聚合物的迄今报道的最高值。光催化剂，也代表通过无金属催化的碳-碳偶联反应形成的这类催化剂的第一个实例。

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  • 来源
    《Advanced Functional Materials》 |2017年第39期|1703146.1-1703146.8|共8页
  • 作者

    Bi Shuai; Lan Zhi-An; Paasch Silvia; Zhang Wenbei; He Yafei; Zhang Chao; Liu Feng; Wu Dongqing; Zhuang Xiaodong; Brunner Eike; Wang Xinchen; Zhang Fan;

  • 作者单位

    Shanghai Jiao Tong Univ, Sch Chem & Chem Engn, State Key Lab Met Matrix Composites, Shanghai 200240, Peoples R China;

    Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350002, Fujian, Peoples R China;

    Tech Univ Dresden, Ctr Adv Elect Dresden cfaed, D-01062 Dresden, Germany|Tech Univ Dresden, Dept Chem & Food Chem, D-01062 Dresden, Germany;

    Shanghai Jiao Tong Univ, Sch Chem & Chem Engn, State Key Lab Met Matrix Composites, Shanghai 200240, Peoples R China;

    Shanghai Jiao Tong Univ, Sch Chem & Chem Engn, State Key Lab Met Matrix Composites, Shanghai 200240, Peoples R China;

    Shanghai Jiao Tong Univ, Sch Chem & Chem Engn, State Key Lab Met Matrix Composites, Shanghai 200240, Peoples R China;

    Xi An Jiao Tong Univ, State Key Lab Mech Behav Mat, Xian 710049, Shaanxi, Peoples R China;

    Shanghai Jiao Tong Univ, Sch Chem & Chem Engn, State Key Lab Met Matrix Composites, Shanghai 200240, Peoples R China;

    Shanghai Jiao Tong Univ, Sch Chem & Chem Engn, State Key Lab Met Matrix Composites, Shanghai 200240, Peoples R China;

    Tech Univ Dresden, Ctr Adv Elect Dresden cfaed, D-01062 Dresden, Germany|Tech Univ Dresden, Dept Chem & Food Chem, D-01062 Dresden, Germany;

    Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350002, Fujian, Peoples R China;

    Shanghai Jiao Tong Univ, Sch Chem & Chem Engn, State Key Lab Met Matrix Composites, Shanghai 200240, Peoples R China;

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  • 关键词

    conjugated porous polymers; hydrogen evolution; photocatalyst; sp(2)-carbon frameworks; visible-light-driven catalysis;

    机译：共轭多孔聚合物;析氢;光催化剂;sp（2）-碳骨架;可见光驱动催化;

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