Chong, C., Boong, S. K., Raja Mogan, T., Lee, J., Ang, Z. Z., Li, H., & Lee, H. K. (2024). Catalyst‐On‐Hotspot Nanoarchitecture: Plasmonic Focusing of Light onto Co‐Photocatalyst for Efficient Light‐To‐Chemical Transformation. Small. Portico. https://doi.org/10.1002/smll.202309983
Abstract:
AbstractPlasmon‐mediated catalysis utilizing hybrid photocatalytic ensembles promises effective light‐to‐chemical transformation, but current approaches suffer from weak electromagnetic field enhancements from polycrystalline and isotropic plasmonic nanoparticles as well as poor utilization of precious co‐catalyst. Here, efficient plasmon‐mediated catalysis is achieved by introducing a unique catalyst‐on‐hotspot nanoarchitecture obtained through the strategic positioning of co‐photocatalyst onto plasmonic hotspots to concentrate light energy directly at the point‐of‐reaction. Using environmental remediation as a proof‐of‐concept application, the catalyst‐on‐hotspot design (edge‐AgOcta@Cu2O) enhances photocatalytic advanced oxidation processes to achieve superior organic‐pollutant degradation at ≈81% albeit having lesser Cu2O co‐photocatalyst than the fully deposited design (full‐AgOcta@Cu2O). Mass‐normalized rate constants of edge‐AgOcta@Cu2O reveal up to 20‐fold and 3‐fold more efficient utilization of Cu2O and Ag nanoparticles, respectively, compared to full‐AgOcta@Cu2O and standalone catalysts. Moreover, this design also exhibits catalytic performance >4‐fold better than emerging hybrid photocatalytic platforms. Mechanistic studies unveil that the light‐concentrating effect facilitated by the dense electromagnetic hotspots is crucial to promote the generation and utilization of energetic photocarriers for enhanced catalysis. By enabling the plasmonic focusing of light onto co‐photocatalyst at the single‐particle level, the unprecedented design offers valuable insights in enhancing light‐driven chemical reactions and realizing efficient energy/catalyst utilizations for diverse chemical, environmental, and energy applications.
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Funding Info:
This research / project is supported by the Agency of Science, Technology and Research, Singapore - AME YIRG
Grant Reference no. : A2084c0158
This research / project is supported by the Ministry of Education, Singapore - AcRF Tier 1
Grant Reference no. : RS13/20
This research / project is supported by the Ministry of Education, Singapore - AcRF Tier 1
Grant Reference no. : RG4/21
This research / project is supported by the National University of Singapore - Center of Hydrogen Innovation
Grant Reference no. : CHI-P2022-05
This research / project is supported by the Nanyang Technological University - NA
Grant Reference no. : Start-Up Grants
Description:
This is the peer reviewed version of the following article: Chong, C., Boong, S. K., Raja Mogan, T., Lee, J., Ang, Z. Z., Li, H., & Lee, H. K. (2024). Catalyst‐On‐Hotspot Nanoarchitecture: Plasmonic Focusing of Light onto Co‐Photocatalyst for Efficient Light‐To‐Chemical Transformation. Small. Portico. https://doi.org/10.1002/smll.202309983 , which has been published in final form at doi.org/10.1002/smll.202309983. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions. This article may not be enhanced, enriched or otherwise transformed into a derivative work, without express permission from Wiley or by statutory rights under applicable legislation. Copyright notices must not be removed, obscured or modified. The article must be linked to Wiley’s version of record on Wiley Online Library and any embedding, framing or otherwise making available the article or pages thereof by third parties from platforms, services and websites other than Wiley Online Library must be prohibited.