Boong, S. K., Chong, C., Lee, J., Ang, Z. Z., Li, H., & Lee, H. K. (2023). Superlattice‐based Plasmonic Catalysis: Concentrating Light at the Nanoscale to Drive Efficient Nitrogen‐to‐Ammonia Fixation at Ambient Conditions. Angewandte Chemie International Edition, 62(7). Portico. https://doi.org/10.1002/anie.202216562
Abstract:
Plasmonic catalysis promises green ammonia synthesis but is limited by the need for co‐catalysts and poor performances due to weak electromagnetic field enhancement. Here, we use two‐dimensional plasmonic superlattices with dense electromagnetic hotspots to boost ambient nitrogen‐to‐ammonia photoconversion without needing co‐catalyst. By organizing Ag octahedra into a square superlattice to concentrate light, the ammonia formation is enhanced by ≈15‐fold and 4‐fold over hexagonal superlattice and disorganized array, respectively. Our unique catalyst achieves superior ammonia formation rate and apparent quantum yield up to ≈15‐fold and ≈103‐fold, respectively, better than traditional designs. Mechanistic investigations reveal the abundance of intense plasmonic hotspots is crucial to promote hot electron generation and transfer for nitrogen reduction. Our work offers valuable insights to design electromagnetically hot plasmonic catalysts for diverse chemical and energy applications.
License type:
Publisher Copyright
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 - Start-Up Grants
Grant Reference no. : NA
Description:
This is the peer reviewed version of the following article: Boong, S. K., Chong, C., Lee, J., Ang, Z. Z., Li, H., & Lee, H. K. (2023). Superlattice‐based Plasmonic Catalysis: Concentrating Light at the Nanoscale to Drive Efficient Nitrogen‐to‐Ammonia Fixation at Ambient Conditions. Angewandte Chemie International Edition, 62(7). Portico. https://doi.org/10.1002/anie.202216562 , which has been published in final form at doi.org/10.1002/anie.202216562. 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.