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High Performance Reduction of H_2O_2 with an Electron Transport Decaheme Cytochrome on a Porous ITO Electrode

机译:多孔ITO电极上电子传输十面体细胞色素对H_2O_2的高效还原

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摘要

The decaheme cytochrome MtrC from Shewanella oneidensis MR-1 immobilized on an ITO electrode displays unprecedented H_2O_2 reduction activity. Although MtrC showed lower peroxidase activity in solution compared to horseradish peroxidase, the ten heme cofactors enable excellent electronic communication and a superior activity on the electrode surface. A hierarchical ITO electrode enabled optimal immobilization of MtrC and a high current density of 1 mA cm~(-2) at 0.4 V vs SHE could be obtained at pH 6.5 (E_(onset) = 0.72 V). UV-visible and Resonance Raman spectroelectrochemical studies suggest the formation of a high valent iron-oxo species as the catalytic intermediate. Our findings demonstrate the potential of multiheme cytochromes to catalyze technologically relevant reactions and establish MtrC as a new benchmark in biotechnological H_2O_2 reduction with scope for applications in fuel cells and biosensors.
机译:固定在ITO电极上的来自沙瓦氏假单胞菌MR-1的十血细胞色素MtrC显示出前所未有的H_2O_2还原活性。尽管与辣根过氧化物酶相比,MtrC在溶液中显示出较低的过氧化物酶活性,但十个血红素辅助因子可实现出色的电子通讯,并在电极表面具有出色的活性。分层的ITO电极能够实现MtrC的最佳固定化,并且在pH值为6.5(E_(setset)= 0.72 V)时,在0.4 V vs. SHE的条件下可以获得1 mA cm〜(-2)的高电流密度。紫外可见光谱和共振拉曼光谱电化学研究表明,形成了高价铁-氧代族化合物作为催化中间体。我们的发现表明,多血红素细胞色素具有催化技术相关反应的潜力,并确立了MtrC作为生物技术中H_2O_2还原的新基准,并在燃料电池和生物传感器中得到了广泛应用。

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  • 来源
    《Journal of the American Chemical Society》 |2017年第9期|3324-3327|共4页
  • 作者单位

    Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, United Kingdom;

    Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, United Kingdom;

    Institut fur Chemie, Technische Universität Berlin, Sekr. PC14, Straße des 17. Juni 135, D-10623 Berlin, Germany;

    School of Biomedical Sciences and the Astbury Centre, University of Leeds, Leeds LS2 9JT, United Kingdom;

    School of Chemistry and School of Biological Sciences, University of East Anglia, Norwich Research Park, Norwich NR4 7TJ, United Kingdom;

    Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, United Kingdom;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
  • 原文格式 PDF
  • 正文语种 eng
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  • 入库时间 2022-08-18 03:07:56

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