Glutathione-Capped Gold Nanoclusters as Photosensitizers. Visible Light-Induced Hydrogen Generation in Neutral Water
Glutathione-Capped Gold Nanoclusters as Photosensitizers. Visible Light-Induced Hydrogen Generation in Neutral Water
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DOI：
10.1021/ja5017365
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发表时间：
2014-04-23
影响因子：
15
通讯作者：
Kamat, Prashant V.
中科院分区：
文献类型：
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作者：
Chen, Yong-Siou;Kamat, Prashant V.
谷胱甘肽包覆的金属纳米团簇（Au-x-GSH NCs）表现出类似分子的性质，被用作光电化学电池（PEC）和光催化浆料反应器中的氢生成的光敏剂。这些金属纳米团簇的可逆还原（E-0 =-0.63V vs RHE）和氧化（E-0 = 0.97和1.51V vs RHE）电位使它们适合于驱动水裂解反应。在pH = 7的缓冲水溶液中，以介观TiO 2薄膜为阳极，Pt为对电极，在可见光（400-500 nm）激发下，观察到了明显的光电流活性。此外，在水性浆料体系中用Au-x-GSH NC敏化Pt/TiO 2纳米颗粒并用可见光照射以0.3mmol氢/h/g Au-x-GSH NC的速率产生H-2。当将牺牲供体如EDTA引入系统中时，H-2释放速率显著增强（类似于5倍）。利用金属纳米团簇作为光敏剂用于制氢为未来探索具有良好控制的金属原子和封端配体数目的其他金属纳米团簇奠定了基础。
Glutathione-capped metal nanoclusters (Au-x-GSH NCs) which exhibit molecular-like properties are employed as a photosensitizer for hydrogen generation in a photoelectrochemical cell (PEC) and a photocatalytic slurry reactor. The reversible reduction (E-0 = -0.63 V vs RHE) and oxidation (E-0 = 0.97 and 1.51 V vs RHE) potentials of these metal nanoclusters make them suitable for driving the water-splitting reaction. When a mesoscopic TiO2 film sensitized by Au-x-GSH NCs is used as the photoanode with a Pt counter electrode in aqueous buffer solution (pH = 7), we observe significant photocurrent activity under visible light (400-500 nm) excitation. Additionally, sensitizing Pt/TiO2 nanoparticles with Au-x-GSH NCs in an aqueous slurry system and irradiating with visible light produce H-2 at a rate of 0.3 mmol of hydrogen/h/g of Au-x-GSH NCs. The rate of H-2 evolution is significantly enhanced (similar to 5 times) when a sacrificial donor, such as EDTA, is introduced into the system. Using metal nanoclusters as a photosensitizer for hydrogen generation lays the foundation for the future exploration of other metal nanoclusters with well-controlled numbers of metal atoms and capping ligands.