Boosting photocatalytic water oxidation by surface plasmon resonance of AgxAu1-x alloy nanoparticles
Boosting photocatalytic water oxidation by surface plasmon resonance of AgxAu1-x alloy nanoparticles
复制标题
Ag(x)Au1-x 合金纳米颗粒的表面等离子体共振促进光催化水氧化
DOI：
10.1016/j.nanoen.2021.106189
复制
发表时间：
2021-05-25
期刊：
影响因子：
17.6
通讯作者：
Li, Can
中科院分区：
文献类型：
--
作者：
Haider, Rida Shahzadi;Wang, Shengyang;Li, Can
表面等离子体共振（SPR）诱导的多金属纳米粒子光催化效果不明显，特别是在光诱导的水氧化反应中。本文报道了一种利用贵金属合金化（AgxAu1-x）制备工程化带结构的策略。负载金红石型TiO2的AgAu合金纳米颗粒的调制组成选择性地调整SPR波长和d波段位置。我们发现spr诱导的水氧化活性随AgxAu1-x/TiO2光催化剂中Au和Ag的比例而变化，在析氧速率和金属组成之间表现出“火山状”的关系。Ag0.6Au0.4/TiO2光催化剂表现出优异的水氧化性能，约为单个Ag和Au的3倍。合金的光发射光谱（PES）与态密度相关，揭示了d波段起始能量和SPR激发波长的敏感性。此外，合金的表面光电压（SPV）响应表明合金在热载子界面电荷分离方面具有优势。密度泛函理论（DFT）计算验证了实验结果，揭示了复杂的AgAu合金半导体（Ti-O-Au-Ag）的析氧作用以及电动力学模拟来追踪电场分量的分布。本研究通过光吸收、肖特基势垒高度和等离子体光催化剂的d带位置的综合效应，证明了跨合金成分的d带调谐对提高催化分数的关键作用。
Surface plasmon resonance (SPR) induced photocatalysis with multi-metallic nanoparticles stays indistinct, especially in photo-induced water oxidation reaction. Herein, we report a strategy of engineering band structure by noble metal alloying (AgxAu1-x). The modulated composition of AgAu alloy nanoparticles loaded on rutile TiO2 to selectively tune SPR wavelengths and d-band position. We found that SPR-induced water oxidation activity varies as a function of the ratio of Au and Ag in AgxAu1-x/TiO2 photocatalysts, exhibiting"volcano-like" relationship between the oxygen evolution production rate and the metal-composition. The Ag0.6Au0.4/TiO2 photocatalyst shows superior water oxidation performance about 3-folds of individual Ag and Au. Photoemission spectra (PES) of alloy are in correlation with density of states, revealing the sensitivity of d-band onset energies and SPR excitation wavelengths. Furthermore, surface-photovoltage (SPV) response of alloy signifies the superiority of alloy in interfacial charge separation of hot carriers. Density functional theory (DFT) calculations validate the experimental results by revealing complex AgAu alloy-semiconductor (Ti-O-Au-Ag) for oxygen evolution along with electrodynamic simulations to trace distribution of electric-field components. This work demonstrates critical role of d-band tuning across alloy composition for boosting catalytic fraction through the integrated effects of light absorption, Schottky barrier height and d-band position of the plasmonic photocatalysts.