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首页> 外文期刊>Physical chemistry chemical physics: PCCP >Reaction of porphyrin-based surface-anchored metal-organic frameworks caused by prolonged illumination
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Reaction of porphyrin-based surface-anchored metal-organic frameworks caused by prolonged illumination

机译:卟啉基表面锚定金属 - 有机框架的反应延长照明引起的

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摘要

Crystalline surface-anchored metal-organic framework (SURMOF) thin films made from porphyrin-based organic linkers have recently been used in both photon upconversion and photovoltaic applications. While these studies showed promising results, the question of photostability in this organic-inorganic hybrid material has to be investigated before applications can be considered. Here, we combine steady-state photoluminescence, transient absorption, and time-resolved electron paramagnetic resonance spectroscopy to examine the effects of prolonged illumination on a palladium-porphyrin based SURMOF thin film. We find that phototreatment leads to a change in the material's photoresponse caused by the creation of stable products of photodecomposition - likely chlorin - inside the SURMOF structure. When the mobile triplet excitons encounter such a defect site, a short-lived (80 ns) cation-anion radical pair can be formed by electron transfer, wherein the charges are localized at a porphyrin and the photoproduct site, respectively.
机译:最近在光子上变化和光伏应用中使用了由卟啉基有机接头制成的晶体表面锚定的金属 - 有机框架(Surmof)薄膜。虽然这些研究表明了有希望的结果,但在考虑应用之前必须研究该有机 - 无机混合材料中的光稳定性问题。这里,我们将稳态光致发光,瞬态吸收和时间分辨电子顺磁共振谱进行结合,以检查长期照射对钯 - 卟啉基薄膜的影响。我们发现光电放映导致材料光响应的变化,由稳定的光分解 - 可能的氯化氯 - 在Surmof结构内引起的。当移动三联激子遇到这样的缺陷部位时,可以通过电子转移形成短寿命(80ns)阳离子 - 阴离子自由基对,其中电荷分别在卟啉和光调节位点处定位。

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    Karlsruhe Inst Technol Inst Microstruct Technol Eggenstein Leopoldshafen Germany;

    Karlsruhe Inst Technol Inst Microstruct Technol Eggenstein Leopoldshafen Germany;

    Karlsruhe Inst Technol Inst Microstruct Technol Eggenstein Leopoldshafen Germany;

    Free Univ Berlin Fachbereich Phys Berlin Joint EPR Lab Berlin Germany;

    Free Univ Berlin Fachbereich Phys Berlin Joint EPR Lab Berlin Germany;

    Helmholtz Zentrum Berlin Mat &

    Energie GmbH Inst Nanospect Berlin Germany;

    Karlsruhe Inst Technol Inst Funct Interfaces Eggenstein Leopoldshafen Germany;

    Karlsruhe Inst Technol Inst Microstruct Technol Eggenstein Leopoldshafen Germany;

    Karlsruhe Inst Technol Inst Microstruct Technol Eggenstein Leopoldshafen Germany;

    Univ Dublin Sch Chem Trinity Biomed Sci Inst Trinity Coll Dublin Dublin Ireland;

    Univ Dublin Sch Chem Trinity Biomed Sci Inst Trinity Coll Dublin Dublin Ireland;

    Karlsruhe Inst Technol Inst Funct Interfaces Eggenstein Leopoldshafen Germany;

    Free Univ Berlin Fachbereich Phys Berlin Joint EPR Lab Berlin Germany;

    Karlsruhe Inst Technol Inst Microstruct Technol Eggenstein Leopoldshafen Germany;

    Karlsruhe Inst Technol Inst Microstruct Technol Eggenstein Leopoldshafen Germany;

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  • 正文语种 eng
  • 中图分类 物理学;化学;
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