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On the Effect of Native SiO_2 on Si over the SPR-mediated Photocatalytic Activities of Au and Ag Nanoparticles

机译:关于天然SiO_2对SI对Au和Ag纳米粒子的SPR介导的光催化活性的影响

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摘要

In hybrid materials containing plasmonic nanoparticles such as Au and Ag, charge-transfer processes from and to Au or Ag can affect both activities and selectivity in plasmonic catalysis. Inspired by the widespread utilization of commercial Si wafers in surface-enhanced Raman spectroscopy (SERS) studies, we investigated herein the effect of the native SiO_2 layer on Si wafers over the surface plasmon resonance (SPR)-mediated activities of the Au and Ag nanoparticles (NPs). We prepared SERS-active plasmonic comprised of Au and Ag NPs deposited onto a Si wafer. Here, two kinds of Si wafers were employed: Si with a native oxide surface layer (Si/SiO_2) and Si without a native oxide surface layer (Si). This led to Si/SiO_2/Au, Si/SiO_2/Ag, Si/Au, and Si/Ag NPs. The SPR-mediated oxidation of p-aminothiophenol (PATP) to p,p’- dimercaptoazobenzene (DMAB) was employed as a model transformation. By comparing the performances and band structures for the Si/Au and Si/Ag relative to Si/SiO_2/Au and Si/SiO_2/Ag NPs, it was found that the presence of a SiO_2 layer was crucial to enable higher SPR-mediated PATP to DMAB conversions. The SiO_2 layer acts to prevent the charge transfer of SPR-excited hot electrons from Au or Ag nanoparticles to the Si substrate. This enabled SPR-excited hot electrons to be transferred to adsorbed O_2 molecules, which then participate in the selective oxidation of PATP to DMAB. In the absence of a SiO_2 layer, SPR-excited hot electrons are preferentially transferred to Si instead of adsorbed O_2 molecules, leading to much lower PATP oxidation.
机译:在含有等离子体纳米颗粒的杂交材料中,例如Au和Ag,来自Au或Ag的电荷转移方法可以影响等离子体催化的活动和选择性。灵感灵感来自在表面增强的拉曼光谱(SERS)研究中的商业Si晶片的广泛利用,我们研究了本文的表面等离子体共振(SPR)介导的Si晶片上的天然SiO_2层对Au和Ag纳米颗粒的活性的影响(NPS)。我们制备了由Au和Ag NP组成的Sers-Active等级,沉积在Si晶片上。这里,使用两种Si晶片:Si,具有天然氧化物表面层(Si / SiO_2)和没有天然氧化物表面层(Si)的Si。这导致Si / SiO_2 / Au,Si / SiO_2 / Ag,Si / Au和Si / Ag NPS。将P-氨基噻吩苯酚(Patp)的SPR介导的氧化氧化为P,P'-二巯基氮苯氮苯(DMAB)作为模型转化。通过比较Si / Au和Si / Ag的性能和带结构,相对于Si / SiO_2 / Au和Si / SiO_2 / Ag NPS,发现SiO_2层的存在至关重要,以实现更高的SPR介导的PATP到DMAB转换。 SiO_2层用来防止从Au或Ag纳米颗粒到Si衬底的SPR激发热电子的电荷转移。这使得能够转移到吸附的O_2分子中的SPR激发热电子,然后将PATP的选择性氧化成DMAB。在不存在SiO_2层的情况下,优先转移到Si而不是吸附的O_2分子的SPR激发热电子,导致较低的PATP氧化。

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  • 来源
    《Chemistry: A European journal》 |2017年第30期|共6页
  • 作者单位

    College of Science Donghua University Shanghai 201620 (P. R. China);

    Departamento de Química Fundamental Instituto de Química Universidade de Sáo Paulo Av. Prof. Lineu Prestes 748 05508-000 Sáo Paulo-SP (Brazil);

    Departamento de Físico-Química Instituto de Química Universidade Federal da Bahia Rua Bar?o de Jeremoabo 147 40170-115 Salvador-BA (Brazil);

    Departamento de Química Fundamental Instituto de Química Universidade de Sáo Paulo Av. Prof. Lineu Prestes 748 05508-000 Sáo Paulo-SP (Brazil);

    Department of Physics Shaoxing University Shaoxing 312000 (P. R. China);

    Departamento de Química Fundamental Instituto de Química Universidade de Sáo Paulo Av. Prof. Lineu Prestes 748 05508-000 Sáo Paulo-SP (Brazil);

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 应用化学;
  • 关键词

    gold; nanoparticles; photocatalysis; silver; surface plasmon resonance;

    机译:金;纳米粒子;光催化;银;表面等离子体共振;

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