Probing of coupling effect induced plasmonic charge accumulation for water oxidation.
Probing of coupling effect induced plasmonic charge accumulation for water oxidation.
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水氧化耦合效应诱导等离子体电荷积累的探讨
DOI：
10.1093/nsr/nwaa151
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发表时间：
2021-06
影响因子：
20.6
通讯作者：
Li C
中科院分区：
文献类型：
--
作者：
Gao Y;Cheng F;Fang W;Liu X;Wang S;Nie W;Chen R;Ye S;Zhu J;An H;Fan C;Fan F;Li C
摘要 等离子体诱导光催化中氧化还原反应（特别是水氧化）的关键问题是人工光合作用反应位点表面累积电荷（电子或空穴）的浓度。然而，等离激元电荷在催化剂表面积累的位置以及如何提高活性位点的局部电荷密度仍然未知，因为很难确定等离激元诱导电荷的确切空间位置和局部密度，特别是对于空穴。在此，我们表明，在单粒子水平上，等离激元耦合诱导的空穴可以在纳米间隙区域的等离激元金纳米粒子二聚体/TiO2 界面处大量积累，局部增强的表面光电压直接证明了这一点。这种等离子体空穴的积累可以显着加速界面反应位点的水氧化反应（涉及多孔），与TiO2上高度分散的Au纳米粒子相比，光催化活性提高了近一个数量级。结合开尔文探针力显微镜和理论模拟，我们进一步阐明了局部累积空穴密度与局部近场增强的平方成正比。我们的研究结果促进了对等离激元系统中电荷如何空间分布以及反应位点的局部电荷密度在等离激元光催化中所起的具体作用的理解。
Abstract A key issue for redox reactions in plasmon-induced photocatalysis, particularly for water oxidation, is the concentration of surface-accumulating charges (electrons or holes) at a reaction site for artificial photosynthesis. However, where plasmonic charge accumulated at a catalyst's surface, and how to improve local charge density at active sites, remains unknown because it is difficult to identify the exact spatial location and local density of the plasmon-induced charge, particularly with regard to holes. Herein, we show that at the single particle level, plasmon-coupling-induced holes can be greatly accumulated at the plasmonic Au nanoparticle dimer/TiO2 interface in the nanogap region, as directly evidenced by the locally enhanced surface photovoltage. Such an accumulation of plasmonic holes can significantly accelerate the water oxidation reaction (multi-holes involved) at the interfacial reaction site, with nearly one order of magnitude enhancement in photocatalytic activities compared to those of highly dispersed Au nanoparticles on TiO2. Combining Kelvin probe force microscopy and theoretical simulation, we further clarified that the local accumulated hole density is proportional to the square of the local near-field enhancement. Our findings advance the understanding of how charges spatially distribute in plasmonic systems and the specific role that local charge density at reaction sites plays in plasmonic photocatalysis.
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