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首页> 外文期刊>Advanced Functional Materials >Porphyrin Conjugated Polymer with Periodic TypeⅡ-Like Heterojunctions and Single-Atom Catalytic Sites for Broadband-Responsive Hydrogen Evolution
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Porphyrin Conjugated Polymer with Periodic TypeⅡ-Like Heterojunctions and Single-Atom Catalytic Sites for Broadband-Responsive Hydrogen Evolution

机译：卟啉缀合的聚合物，具有周期性Ⅱ类异质结和宽带响应氢气进化的单原子催化位点

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摘要

A novel heterometallic Zn-/Co-porphyrin conjugated polymer (ZnCoP-F CP) with its Co-porphyrin bridging unit bearing two perfluorophenyls is synthesized via a Sonogashira coupling reaction. The resulting ZnCoP-F CP without the Pt cocatalyst exhibits broadband (UV-vis-NIR) light-driven hydrogen evolution activity of 83 mu mol h(-1), which is more than twice that (39 mu mol h(-1)) of its counterpart (ZnCoP CP) with the Co-porphyrin unit bearing two phenyls. Furthermore, an apparent quantum yield of 6.92%, 5.50%, 5.78%, 3.17%, and 0.73% is achieved from the ZnCoP-F CP illuminated at 400, 500, 550, 700, and 850 nm monochromatic light, respectively. The enhanced performance of ZnCoP-F CP can be attributed to the high electron-withdrawing capacity of its perfluorophenyls and the highly dispersed Co centers in Co-porphyrin bridging units serving as single-atom catalytic sites (CoN4), which facilitate the formation of periodic type II-like heterojunctions and the fast charge transfer from Zn-porphyrin to Co-porphyrin units for hydrogen evolution reaction. The broadband-responsive feature is due to the large pi-conjugated system through the whole 2D internal framework of the porphyrin polymer. This work opens a new path to fabricate porphyrin-based polymer with an efficient and broadband-responsive hydrogen evolution system.
机译：通过Sonogashira偶联反应合成具有其共卟啉桥接单元的新型杂核Zn /共卟啉缀合的聚合物（ZnCOP-FPC），其携带两个全氟苯基。没有Pt Cocatalyst的ZnCop-F CP表现出83μmolH（-1）的宽带（UV-Vis-nir）光驱动的氢进化活性，其大于两倍（39μmolH（-1） ）其对应物（Zncop CP）与携带两个苯基的共卟啉单位。此外，表观量子产率为6.92％，5.50％，5.78％，3.17％和0.73％，分别在400,500,550,700和850nm单色光照射的Zncop-F CP实现。 Zncop-F CP的增强性能归因于其全氟苯基的高电子 - 抽出能力和在用作单原子催化位点（CON4）的共卟啉桥接单元中的高度分散的CO中心，其有助于形成周期性II型异质杂交和从Zn-卟啉的快速电荷转移到用于氢化反应的共卟啉单位。宽带响应特征是由于卟啉聚合物的整个2D内部框架的大型PI缀合系统。这项工作开辟了一种新的途径，以制造基于卟啉的聚合物，具有高效宽带响应的氢进化系统。

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  • 来源
    《Advanced Functional Materials》 |2021年第16期|2009819.1-2009819.12|共12页
  • 作者

    Wang Jinming; Xu Lei; Wang Tingxia; Chen Shengtao; Jiang Zhuo; Li Renjie; Zhang Yuexing; Peng Tianyou;

  • 作者单位

    Wuhan Univ Minist Educ Coll Chem & Mol Sci Engn Res Ctr Organosilicon Cpds & Mat Wuhan 430072 Peoples R China;

    Wuhan Univ Minist Educ Coll Chem & Mol Sci Engn Res Ctr Organosilicon Cpds & Mat Wuhan 430072 Peoples R China|Wuhan Univ Res Inst Shenzhen 518057 Peoples R China;

    Wuhan Univ Minist Educ Coll Chem & Mol Sci Engn Res Ctr Organosilicon Cpds & Mat Wuhan 430072 Peoples R China;

    Wuhan Univ Minist Educ Coll Chem & Mol Sci Engn Res Ctr Organosilicon Cpds & Mat Wuhan 430072 Peoples R China|Wuhan Univ Res Inst Shenzhen 518057 Peoples R China;

    Wuhan Univ Minist Educ Coll Chem & Mol Sci Engn Res Ctr Organosilicon Cpds & Mat Wuhan 430072 Peoples R China;

    Wuhan Univ Minist Educ Coll Chem & Mol Sci Engn Res Ctr Organosilicon Cpds & Mat Wuhan 430072 Peoples R China;

    Hubei Univ Coll Chem & Chem Engn Wuhan 430072 Peoples R China;

    Wuhan Univ Minist Educ Coll Chem & Mol Sci Engn Res Ctr Organosilicon Cpds & Mat Wuhan 430072 Peoples R China|Wuhan Univ Res Inst Shenzhen 518057 Peoples R China;

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  • 正文语种 eng
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  • 关键词

    broadband spectral response; hydrogen evolution reaction; photocatalyst; porphyrin conjugated polymers; single#8208; atom catalytic sites;

    机译：宽带光谱响应;氢进化反应;光催化剂;卟啉缀合的聚合物;单＆＃8208;原子催化位点;

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