Monitoring Hot Holes in Plasmonic Catalysis on Silver Nanoparticles by Using an Ion Label.

IF 9.6 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Nano Letters Pub Date : 2024-09-18 Epub Date: 2024-09-03 DOI:10.1021/acs.nanolett.4c03265
Xiaomeng Du, Teng Wang, Yonglong Li, Aonan Zhu, Yanfang Hu, Aoxuan Du, Yan Zhao, Wei Xie
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Abstract

Energetic carriers generated by localized surface plasmon resonance (LSPR) provide an efficient way to drive chemical reactions. However, their dynamics and impact on surface reactions remain unknown due to the challenge in observing hot holes. This makes it difficult to correlate the reduction and oxidation half-reactions involving hot electrons and holes, respectively. Here we detect hot holes in their chemical form, Ag(I), on a Ag surface using surface-enhanced Raman scattering (SERS) of SO32- as a hole-specific label. It allows us to determine the dynamic correlations of hot electrons and holes. We find that the equilibrium of holes is the key factor of the surface chemistry, and the wavelength-dependent plasmonic chemical anode refilling (PCAR) effect plays an important role, in addition to the LSPR, in promoting the electron transfer. This method paves the way for visualizing hot holes with nanoscale spatial resolution toward the rational design of a plasmonic catalytic platform.

Abstract Image

利用离子标签监测银纳米粒子上等离子催化过程中的热洞
局域表面等离子体共振(LSPR)产生的高能载流子是驱动化学反应的有效途径。然而,由于在观察热洞方面的挑战,它们的动力学和对表面反应的影响仍然未知。这就很难将热电子和热空穴分别参与的还原和氧化半反应联系起来。在这里,我们利用 SO32- 作为空穴特异性标签的表面增强拉曼散射 (SERS) 技术,在白银表面检测化学形态为 Ag(I) 的空穴。这使我们能够确定热电子和空穴的动态相关性。我们发现空穴的平衡是表面化学的关键因素,除了 LSPR 外,波长依赖性质子化学阳极填充效应(PCAR)在促进电子转移方面也发挥了重要作用。这种方法为纳米级空间分辨率的热孔可视化铺平了道路,有助于合理设计质子催化平台。
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来源期刊
Nano Letters
Nano Letters 工程技术-材料科学:综合
CiteScore
16.80
自引率
2.80%
发文量
1182
审稿时长
1.4 months
期刊介绍: Nano Letters serves as a dynamic platform for promptly disseminating original results in fundamental, applied, and emerging research across all facets of nanoscience and nanotechnology. A pivotal criterion for inclusion within Nano Letters is the convergence of at least two different areas or disciplines, ensuring a rich interdisciplinary scope. The journal is dedicated to fostering exploration in diverse areas, including: - Experimental and theoretical findings on physical, chemical, and biological phenomena at the nanoscale - Synthesis, characterization, and processing of organic, inorganic, polymer, and hybrid nanomaterials through physical, chemical, and biological methodologies - Modeling and simulation of synthetic, assembly, and interaction processes - Realization of integrated nanostructures and nano-engineered devices exhibiting advanced performance - Applications of nanoscale materials in living and environmental systems Nano Letters is committed to advancing and showcasing groundbreaking research that intersects various domains, fostering innovation and collaboration in the ever-evolving field of nanoscience and nanotechnology.
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