论文标题
Srtio上的光催化水氧化$ _3 $ [001]表面
Photocatalytic water oxidation on SrTiO$_3$ [001] surfaces
论文作者
论文摘要
Srtio $ _3 $是在紫外线照射下进行总体水分反应的高效光催化剂。但是，仍然缺乏对负责氧化和还原反应的活性表面位点的原子级别的理解。在这里，我们提出了在SRO-和TIO $ _2 $ - 水溶液[001] srtio $ _3 $的终止下的光催化活性的统一实验和计算说明。我们的实验发现表明，仅当两种终止同时暴露于水时，总体抽水反应才会在SRTIO $ _3 $表面进行。我们的模拟解释了这一点，表明光生孔驱动的氧化主要发生在四个单孔转移反应的序列上，而TiO $ _2 $终止对光催化剂相对与水氧化潜力的关键带对对齐。目前的工作阐明了Srtio $ _3 $表面的两个化学终止的相互依赖性，因此对最大化可持续太阳能驱动的水分裂具有影响。
SrTiO$_3$ is a highly efficient photocatalyst for the overall water splitting reaction under UV irradiation. However, an atomic-level understanding of the active surface sites responsible for the oxidation and reduction reactions is still lacking. Here we present a unified experimental and computational account of the photocatalytic activity at the SrO- and TiO$_2$- terminations of aqueous-solvated [001] SrTiO$_3$. Our experimental findings show that the overall water-splitting reaction proceeds on the SrTiO$_3$ surface only when the two terminations are simultaneously exposed to water. Our simulations explain this, showing that the photogenerated hole-driven oxidation primarily occurs at SrO surfaces in a sequence of four single hole transfer reactions, while the TiO$_2$ termination effects the crucial band alignment of the photocatalyst relative to the water oxidation potential. The present work elucidates the interdependence of the two chemical terminations of SrTiO$_3$ surfaces, and has consequent implications for maximizing sustainable solar-driven water splitting.
