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首页> 外文期刊>Chemistry: A European journal >Photocatalytic Hydrogen Generation by Vesicle-Embedded [FeFe]Hydrogenase Mimics: A Mechanistic Study
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Photocatalytic Hydrogen Generation by Vesicle-Embedded [FeFe]Hydrogenase Mimics: A Mechanistic Study

机译：囊泡嵌入式[Fefe]氢酶模拟的光催化氢气产生：机械研究

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摘要

Artificial photosynthesis-the direct photochemical generation of hydrogen from water-is a promising but scientifically challenging future technology. Because nature employs membranes for photodriven reactions, the aim of this work is to elucidate the effect of membranes on artificial photocatalysis. To do so, a combination of electrochemistry, photocatalysis, and time-resolved spectroscopy on vesicleembedded [FeFe]hydrogenase mimics, driven by a ruthenium tris-2,2'-bipyridine photosensitizer, is reported. The membrane effects encountered can be summarized as follows: the presence of vesicles steers the reactivity of the [FeFe]- benzodithiolate catalyst towards disproportionation, instead of protonation, due to membrane characteristics, such as providing a constant local effective pH, and concentrating and organizing species inside the membrane. The maximum turnover number is limited by photodegradation of the resting state in the catalytic cycle. Understanding these fundamental productive and destructive pathways in complex photochemical systems allows progress towards the development of efficient artificial leaves.
机译：人造光合作用 - 水中氢的直接光化学产生 - 是未来技术的有希望但科学挑战。因为自然采用膜来用于光化反应，所以这项工作的目的是阐明膜对人工光催化的影响。为此，报道了通过钌Tris-2,2'-硼吡啶光敏剂驱动的vesceembedded的氢化酶模拟物的电化学，光催化和时间分辨光谱的组合。所遇到的膜效应可以概括如下：由于膜特性，囊泡的存在使得[FEFE] - 苯二甲酸辛酸盐催化剂的反应性，代替质子化，例如提供恒定的局部有效pH，并浓缩和组织膜内的种类。通过在催化循环中的静止状态的光降解限制最大变化数。了解复杂光化学系统中的这些基本生产力和破坏性途径允许进展到有效的人造叶子的发展。

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  • 来源
    《Chemistry: A European journal》 |2019年第61期|共9页
  • 作者

    René Becker; Tessel Bouwens; Esther C. F. Schippers; Toon van Gelderen; Michiel Hilbers; Sander Woutersen; Joost N. H. Reek;

  • 作者单位

    van't Hoff Institute for Molecular Sciences University of Amsterdam Science Park 904 Amsterdam 1098 XH (The Netherlands);

    van't Hoff Institute for Molecular Sciences University of Amsterdam Science Park 904 Amsterdam 1098 XH (The Netherlands);

    van't Hoff Institute for Molecular Sciences University of Amsterdam Science Park 904 Amsterdam 1098 XH (The Netherlands);

    van't Hoff Institute for Molecular Sciences University of Amsterdam Science Park 904 Amsterdam 1098 XH (The Netherlands);

    van't Hoff Institute for Molecular Sciences University of Amsterdam Science Park 904 Amsterdam 1098 XH (The Netherlands);

    van't Hoff Institute for Molecular Sciences University of Amsterdam Science Park 904 Amsterdam 1098 XH (The Netherlands);

    van't Hoff Institute for Molecular Sciences University of Amsterdam Science Park 904 Amsterdam 1098 XH (The Netherlands);

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 应用化学;
  • 关键词

    artificial photosynthesis; iron; photochemistry; time-resolved spectroscopy; vesicles;

    机译：人造光合作用;铁;光化学;时间分辨光谱;囊泡;

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