Photoelectrochemical Water Oxidation with Photosystem II Integrated in a Mesoporous; Indium Tin Oxide Electrode
Photoelectrochemical Water Oxidation with Photosystem II Integrated in a Mesoporous; Indium Tin Oxide Electrode
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DOI：
10.1021/ja301488d
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发表时间：
2012-05-23
影响因子：
15
通讯作者：
Reisner, Erwin
中科院分区：
文献类型：
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作者：
Kato, Masaru;Cardona, Tanai;Reisner, Erwin
我们报告的混合光阳极水氧化组成的蓝藻光系统II（PSII）从细长热聚球藻上介孔铟锡氧化物（mesoITO）电极。三维金属氧化物环境允许高蛋白质覆盖率（26倍于理想单层覆盖率）和从PSII到mesoITO的直接（无介体）电子转移。在红光照射期间，水的氧化发生在1.6 +/- 0.3 μ A cm（-2），相应的转换频率约为0.18 +/- 0.04（mol O-2）（mol PSII）（-1）s（-1）。机理研究与界面电子转移一致，该界面电子转移不仅发生在末端醌Q（B），而且发生在醌Q（A）通过非天然电子转移途径到ITO表面。
We report on a hybrid photoanode for water oxidation consisting of a cyanobacterial photosystem II (PSII) from Thermosynechococcus elongatus on a mesoporous indium-tin oxide (mesoITO) electrode. The three-dimensional metal oxide environment allows for high protein coverage (26 times an ideal monolayer coverage) and direct (mediator-free) electron transfer from PSII to mesoITO. The oxidation of water occurs with 1.6 +/- 0.3 mu A cm(-2) and a corresponding turnover frequency of approximately 0.18 +/- 0.04 (mol O-2) (mol PSII)(-1) s(-1) during red light irradiation. Mechanistic studies are consistent with interfacial electron transfer occurring not only from the terminal quinone Q(B), but also from the quinone Q(A) through an unnatural electron transfer pathway to the ITO surface.