Dye-Sensitized Hydrobromic Acid Splitting for Hydrogen Solar Fuel Production
Dye-Sensitized Hydrobromic Acid Splitting for Hydrogen Solar Fuel Production
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DOI：
10.1021/jacs.7b09367
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发表时间：
2017-11-08
影响因子：
15
通讯作者：
Meyer, Gerald J.
中科院分区：
文献类型：
--
作者：
Brady, Matthew D.;Sampaio, Renato N.;Meyer, Gerald J.
氢溴酸（HBr）作为一种廉价的氢气（H-2）太阳能燃料生产的原料，通过HBr分裂具有显着的潜力。采用一种新型的Ru-II多吡啶配合物作为溴氧化的光催化剂，对TiO 2或SnO 2/TiO 2核壳纳米粒子的介孔薄膜进行可见光敏化.这些薄膜作为光电极在染料敏化光电合成电池进行了测试。在1 N HBr（aq）中，光催化剂经历激发态电子注入和光驱动的Br-氧化。注入的电子在Pt电极处诱导质子还原。在100 mW cm（-2）白光照射下，在外加偏压下测得1.5 mA cm（-2）的持续光电流。测得Br-氧化的法拉第效率为71 ± 5%，H-2生成的法拉第效率为94.2%。在光照过程中维持12 μ mol·h（-1）的持续H-2产生速率。结果表明，HBr分裂的分子方法与可见光吸收复合物能够水溶液溴氧化和激发态电子注入。
Hydrobromic acid (HBr) has significant potential as an inexpensive feedstock for hydrogen gas (H-2) solar fuel production through HBr splitting. Mesoporous thin films of anatase TiO2 or SnO2/TiO2 core-shell nanoparticles were sensitized to visible light with a new Ru-II polypyridyl complex that served as a photocatalyst for bromide oxidation. These thin films were tested as photoelectrodes in dye-sensitized photoelectrosynthesis cells. In 1 N HBr (aq), the photocatalyst undergoes excited-state electron injection and light-driven Br- oxidation. The injected electrons induce proton reduction at a Pt electrode. Under 100 mW cm(-2) white-light illumination, sustained photocurrents of 1.5 mA cm(-2) were measured under an applied bias. Faradaic efficiencies of 71 +/- 5% for Br- oxidation and 94 2% for H-2 production were measured. A 12 mu mol h(-1) sustained rate of H-2 production was maintained during illumination. The results demonstrate a molecular approach to HBr splitting with a visible light absorbing complex capable of aqueous Br- oxidation and excited-state electron injection.