Direct Plasmon-Driven Photoelectrocatalysis
Direct Plasmon-Driven Photoelectrocatalysis
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DOI：
10.1021/acs.nanolett.5b02453
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发表时间：
2015-09-01
期刊：
影响因子：
10.8
通讯作者：
Thomann, Isabell
中科院分区：
文献类型：
--
作者：
Robatjazi, Hossein;Bahauddin, Shah Mohammad;Thomann, Isabell
利用热载流子的能量是一个新兴的研究领域，具有改进能量转换技术的潜力。(1-3) 在这里，我们提出了一种精心设计的新型等离子体光电极结构，通过高效、非辐射的等离子体衰变成热载流子来驱动光催化反应。与过去的工作相比，我们的架构没有利用肖特基结（肖特基结），肖特基结是收集热载流子的常用构建块。相反，我们观察到来自无肖特基结的大光电流，这是由于等离激元衰变时从等离激元金纳米粒子直接将热电子注入到反应物物质中而产生的。我们的方法的关键要素是（i）受光阻抗匹配概念启发的增加光吸收的架构，（4）（ii）通过选择性传输层进行载流子分离，以及（iii）有效的热载流子生成和从小等离子体金纳米粒子注入到吸附的水分子。我们还研究了不同粒径的热电子注入的量子效率，以阐明潜在的量子效应，同时保持等离子共振频率不变。有趣的是，我们的研究没有揭示所研究的颗粒尺寸和等离子共振的热电子产生和注入效率的差异。
Harnessing the energy from hot charge carriers is an emerging research area with the potential to improve energy conversion technologies.(1-3) Here we present a novel plasmonic photoelectrode architecture carefully designed to drive photocatalytic reactions by efficient, nonradiative plasmon decay into hot carriers. In contrast to past work, our architecture does not utilize a Schottky junction, the commonly used building block to collect hot carriers. Instead, we observed large photocurrents from a Schottky-free junction due to direct hot electron injection from plasmonic gold nanoparticles into the reactant species upon plasmon decay. The key ingredients of our approach are (i) an architecture for increased light absorption inspired by optical impedance matching concepts,(4) (ii) carrier separation by a selective transport layer, and (iii) efficient hot-carrier generation and injection from small plasmonic Au nanoparticles to adsorbed water molecules. We also investigated the quantum efficiency of hot electron injection for different particle diameters to elucidate potential quantum effects while keeping the plasmon resonance frequency unchanged. Interestingly, our studies did not reveal differences in the hot-electron generation and injection efficiencies for the investigated particle dimensions and plasmon resonances.