Covalent immobilization of oriented photosystem II on a nanostructured electrode for solar water oxidation.

Covalent immobilization of oriented photosystem II on a nanostructured electrode for solar water oxidation.
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DOI:
10.1021/ja404699h
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发表时间:
2013-07-24
影响因子:
15
通讯作者:
Reisner E
Reisner E
中科院分区:
化学1区
文献类型:
--
作者:
Kato M;Cardona T;Rutherford AW;Reisner E

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光系统II(PSII)提供了一种生物和可持续的光化学水氧化为O2的途径,并可以为太阳能燃料(如H2)的产生提供质子和电子。我们提出了一种合理的策略,通过静电作用改善嗜热蓝细菌长形热霉菌PSII在纳米结构氧化铟锡(ITO)电极上的取向,并将PSII共价固定在电极上。在ITO电极上修饰了一层自组装单分子膜(SAM),该膜由带有悬挂的羧酸基的磷酸ITO连接物组成。带负电荷的羧酸盐通过库仑相互作用吸引PSII电子受体侧的正偶极子。通过酰胺键将PSII在其静电增强的取向上共价连接到SAM修饰的ITO电极上,进一步增强了PSII杂化光电电极的红光驱动、直接电子转移和稳定性。
Photosystem II (PSII) offers a biological and sustainable route of photochemical water oxidation to O2 and can provide protons and electrons for the generation of solar fuels, such as H2. We present a rational strategy to electrostatically improve the orientation of PSII from a thermophilic cyanobacterium, Thermosynechococcus elongatus, on a nanostructured indium tin oxide (ITO) electrode and to covalently immobilize PSII on the electrode. The ITO electrode was modified with a self-assembled monolayer (SAM) of phosphonic acid ITO linkers with a dangling carboxylate moiety. The negatively charged carboxylate attracts the positive dipole on the electron acceptor side of PSII via Coulomb interactions. Covalent attachment of PSII in its electrostatically improved orientation to the SAM-modified ITO electrode was accomplished via an amide bond to further enhance red-light-driven, direct electron transfer and stability of the PSII hybrid photoelectrode.
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