Plasmon-Accelerated Water Oxidation at Ni-Modified Au Nanodimers on TiO2 Single Crystals,ACS Energy Letters

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Plasmon-Accelerated Water Oxidation at Ni-Modified Au Nanodimers on TiO2 Single Crystals
ACS Energy Letters ( IF 19.3 ) Pub Date : 2021-11-15 , DOI: 10.1021/acsenergylett.1c02163
Kentaro Suzuki ₁ , Xiaowei Li ₁ , Takahiro Toda ₁ , Fumika Nagasawa ₁ , Kei Murakoshi ₁

Affiliation

The oxygen evolution reaction via water-splitting is essential in the solar production of chemical fuels. However, the high overpotential limits the conversion efficiency, even when precious metal catalysts are used to drive it. Plasmonic metal–semiconductor systems can potentially overcome this problem, because hot electrons generated by localized surface plasmon resonance are rapidly injected into the semiconductor, and concentrated hot holes oxidize water on the catalysts for oxygen evolution. Using Ni-modified Au/TiO₂, we investigated distinct Raman spectral characteristics of water-oxidation intermediates at electrochemical potentials near the flat-band potential of TiO₂. Specifically, in situ electrochemical surface-enhanced Raman spectroscopy was performed over the pH range 7–13. Significantly enhanced photocurrents at near-neutral conditions were generated with low-energy photons (1.58 eV), providing the first robust experimental evidence that nickel-based catalysts accelerated the four-electron multistep reaction via plasmon-assisted water oxidation.

中文翻译：

Ni修饰的Au纳米二聚体在TiO2单晶上的等离子体加速水氧化

通过水分解的析氧反应在太阳能生产化学燃料中是必不可少的。然而，高过电位限制了转换效率，即使使用贵金属催化剂来驱动它也是如此。等离子体金属-半导体系统可以潜在地克服这个问题，因为由局域表面等离子体共振产生的热电子被迅速注入半导体，并且集中的热空穴氧化催化剂上的水以释放氧气。使用 Ni 修饰的 Au/TiO ₂，我们在接近 TiO ₂平带电位的电化学电位下研究了水氧化中间体的不同拉曼光谱特性。具体来说，就地电化学表面增强拉曼光谱在 pH 值范围 7-13 内进行。低能光子 (1.58 eV) 在近中性条件下产生显着增强的光电流，这提供了第一个强有力的实验证据，即镍基催化剂通过等离子体辅助水氧化加速了四电子多步反应。

更新日期：2021-12-10

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