AbstractWiring the active site of an enzyme directly to an electrode is the key to ensuring efficient electron transfer for the proper performance of enzyme-based bioelectronic systems. Iron-sulfur complexes, the first link between proteins and mediating molecules in the biological electron transport chain(s), possess an intrinsic electron transport capability. The authors demonstrate the application of inorganic iron-sulfur clusters (Fe-S) viz. FeS, FeS2, Fe2S3, and Fe3S4, as molecular wires to mediate electron transport between a glucose-selective redox enzyme and the gold electrode. It is shown that Fe-S can emulate the functionality of the natural electron transport chain. Voltammetric studies indicate a significant improvement in electron transport, surface coverage, and resilience achieved by the Fe-S-based glucose anodes when compared to a conventional pyrroloquinoline quinone (PQQ)-based electrode. The Fe-S-based glucose anodes showed glucose oxidation at a potential of +0.5 V vs. Ag/AgCl with Tris-HCl buffer (pH 8) acting as a carrier. The current densities positively correlated with the concentrations of glucose in the range 0.1–100 mM displaying detection limits of 0.77 mM (FeS), 1.22 mM (FeS2), 2.95 mM (Fe2S3), and 14.57 mM (Fe3S4). The metal-anchorable sulfur atom, the strong π-coordinating iron atom, the favorable redox properties, low cost, and natural abundance make Fe-S an excellent electron-mediating relay capable of wiring redox active sites to electrode surfaces. Graphical abstractSchematic representation of inorganic iron-sulfur clusters used as molecular wires to facilitate direct electron transfer between NAD-glucose dehydrogenase and the gold electrode. The iron-sulfur based glucose anodes improve current response to selectively sense glucose concentrations in the range 0.1–100 mM.

中文翻译：

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当用于连接基于 NAD-葡萄糖脱氢酶的氧化还原系统时，无机铁硫簇可增强电子传输

摘要将酶的活性位点直接连接到电极是确保有效电子转移以实现基于酶的生物电子系统正常性能的关键。铁硫复合物是蛋白质和生物电子传递链中介导分子之间的第一个链接，具有固有的电子传递能力。作者展示了无机铁硫簇 (Fe-S) 的应用，即。FeS、FeS2、Fe2S3 和 Fe3S4 作为分子线，介导葡萄糖选择性氧化还原酶和金电极之间的电子传输。结果表明，Fe-S 可以模拟天然电子传输链的功能。伏安研究表明电子传输、表面覆盖、与传统的基于吡咯并喹啉醌 (PQQ) 的电极相比，基于 Fe-S 的葡萄糖阳极实现的弹性和弹性。Fe-S 基葡萄糖阳极在 +0.5 V 电位下与 Ag/AgCl 相比显示葡萄糖氧化，Tris-HCl 缓冲液（pH 8）作为载体。电流密度与 0.1-100 mM 范围内的葡萄糖浓度呈正相关，检测限为 0.77 mM (FeS)、1.22 mM (FeS2)、2.95 mM (Fe2S3) 和 14.57 mM (Fe3S4)。金属可锚定的硫原子、强的 π 配位铁原子、良好的氧化还原性能、低成本和天然丰度使 Fe-S 成为一种优秀的电子介导继电器，能够将氧化还原活性位点连接到电极表面。图形摘要用作分子线以促进 NAD-葡萄糖脱氢酶和金电极之间直接电子转移的无机铁硫簇的示意图。基于铁硫的葡萄糖阳极改善了电流响应，以选择性地检测 0.1-100 mM 范围内的葡萄糖浓度。