Cooperative Interactions between Surface Terminations Explain Photocatalytic Water Splitting Activity on SrTiO3
Cooperative Interactions between Surface Terminations Explain Photocatalytic Water Splitting Activity on SrTiO3
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表面终止之间的协同相互作用解释了 SrTiO3 上的光催化水分解活性
DOI：
10.1103/prxenergy.1.023002
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发表时间：
2022
期刊：
影响因子：
--
通讯作者：
Dawber, Matthew
中科院分区：
文献类型：
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作者：
Sharma, Vidushi;Bein, Benjamin;Lai, Amanda;Pamuk, Betül;Dreyer, Cyrus E.;Fernández-Serra, Marivi;Dawber, Matthew
是一种高效光催化剂，适用于紫外线照射下的整个水分解反应。然而，仍然缺乏对负责氧化和还原反应的活性表面位点的原子水平理解。在这里，我们对 SrO 和水溶剂化物 [001] 的光催化活性提出了统一的实验和计算说明。我们的实验结果表明，只有当两个末端同时暴露于水时，整个水分解反应才会在表面上进行。我们的模拟解释了这一点，表明光生空穴驱动的氧化主要发生在 SrO 表面，按四个单空穴转移反应的顺序，而终止影响光催化剂相对于水氧化电位的关键能带排列。目前的工作阐明了表面两种化学终端的相互依赖性，并对最大化可持续的太阳能驱动的水分解具有相应的影响。
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 andterminations of aqueous solvated [001]. Our experimental findings show that the overall water-splitting reaction proceeds on thesurface 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 thetermination 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 ofsurfaces, and has consequent implications for maximizing sustainable solar-driven water splitting.