Chaulagain Narendra, Alam Kazi M, Kadian Sachin, Kumar Navneet, Garcia John, Manik Gaurav, Shankar Karthik
Department of Electrical and Computer Engineering, University of Alberta, 9211-116 Street, Edmonton, Alberta T6G 1H9, Canada.
Nanotechnology Research Centre, National Research Council Canada, 11421 Saskatchewan Drive, Edmonton, Alberta T6G 2M9, Canada.
ACS Appl Mater Interfaces. 2022 Jun 1;14(21):24309-24320. doi: 10.1021/acsami.2c02649. Epub 2022 May 21.
We report a unique photoanode architecture involving TiO, g-CN, and AuNPs wherein a synergistic enhancement of the photoelectrochemical (PEC) performance was obtained with photocurrent densities as high as 3 mA cm under AM1.5G 1 sun illumination. The PEC performance was highly stable and reproducible, and a photoresponse was obtained down to a photon energy of 2.4 eV, close to the interband damping threshold of Au. The photocurrent enhancement was maximized when the Au plasmon band strongly overlapped the g-CN emission band. Our photoanode architecture, which involved AuNPs buried under TiO and a plasmon-induced resonance energy transfer-like interaction between g-CN quantum dots (CNQDs) and AuNPs, solved four major problems associated with plasmonic photoelectrocatalysis─it reduced recombination by limiting eliminating direct electrolyte access to AuNPs, it facilitated electron extraction through single-crystal TiO nanorod percolation pathways, it facilitated hole extraction through a defective TiO seed layer or canopy, and it expanded the range of visible light harvesting by pumping the Au surface plasmons from CNQDs through exciton-to-plasmon resonant energy transfer.
我们报道了一种独特的光阳极结构，它包含TiO、g-CN和AuNP，在AM1.5G 1太阳光照下，光电流密度高达3 mA cm时，实现了光电化学（PEC）性能的协同增强。PEC性能高度稳定且可重复，在低至2.4 eV的光子能量下仍能获得光响应，该能量接近Au的带间阻尼阈值。当Au等离子体激元带与g-CN发射带强烈重叠时，光电流增强达到最大值。我们的光阳极结构，其中AuNP埋在TiO之下，且g-CN量子点（CNQD）与AuNP之间存在类似等离子体激元诱导共振能量转移的相互作用，解决了与等离子体激元光电催化相关的四个主要问题——通过限制电解质直接接触AuNP减少了复合，通过单晶TiO纳米棒渗流途径促进了电子提取，通过有缺陷的TiO种子层或覆盖层促进了空穴提取，以及通过激子到等离子体激元的共振能量转移从CNQD泵浦Au表面等离子体激元扩大了可见光捕获范围。
