Plasmon and Upconversion Mediated Broadband Spectral Response in TiO2 Inverse Opal Photocatalysts for Enhanced Photoelectrochemical Water Splitting
Plasmon and Upconversion Mediated Broadband Spectral Response in TiO2 Inverse Opal Photocatalysts for Enhanced Photoelectrochemical Water Splitting
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DOI：
10.1021/acsaem.9b00469
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发表时间：
2019-04
影响因子：
6.4
通讯作者：
Ramireddy Boppella;Filipe Marques Mota;J. Lim;Saji T. Kochuveedu;Sunghyun Ahn;Jiseok Lee;D. Kawaguchi;Keiji Tanaka;Dong Ha Kim
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文献类型：
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作者：
Ramireddy Boppella;Filipe Marques Mota;J. Lim;Saji T. Kochuveedu;Sunghyun Ahn;Jiseok Lee;D. Kawaguchi;Keiji Tanaka;Dong Ha Kim
通过战略性地利用等离子体和上转换纳米组件的光催化性能来收集低能光子是提高太阳能利用率的有前途的途径。在此，一个合理设计的三维复合光阳极集成近红外响应的上转换纳米晶体（UCN）和可见光响应的等离子体Au纳米粒子（NP）到三维TiO 2反蛋白石纳米结构（Au/UCN/TiO 2）已被证明，以扩大太阳能利用在紫外-可见-近红外范围。研究了掺Er ~（3+）或Tm ~（3+）的NaYF ~（4+）：Yb ~（3+）基UCN的近红外响应特性，以及UCN和Au交替引入的影响。随着Er-UCN的发射和Au的特征SPR带之间的扩展重叠，我们的三元Au/Er-UCN/TiO 2混合纳米结构揭示了在UV-vis-NIR照明下的光电流密度与原始TiO 2参考相比显著提高了10倍。Au的掺入对提高纳米晶的生长速率起到了关键作用。
Harvesting low-energy photons by strategically exploiting the photocatalytic properties of plasmonic and upconversion nanocomponents is a promising route to improve solar energy utilization. Herein, a rationally designed 3D composite photoanode integrating NIR-responsive upconversion nanocrystals (UCNs) and visible-responsive plasmonic Au nanoparticles (NPs) into 3D TiO2 inverse opal nanostructures (Au/UCN/TiO2) has been shown to extend the solar energy utilization in the UV–vis–NIR range. The NIR-responsive properties of NaYF4:Yb3+-based UCNs doped with Er3+ or Tm3+ ions, and the effect of an alternating sequential introduction of UCN and Au, have been assessed. With an extended overlap between the emission of Er-UCN and the characteristic SPR band of Au, our ternary Au/Er-UCN/TiO2 hybrid nanostructure unveiled a notable 10-fold improvement in photocurrent density under UV–vis–NIR illumination compared with a pristine TiO2 reference. The Au incorporation was confirmed to play a key role in enhancing the ...