Wednesday, 16 October 2019: 08:10
Room 215 (The Hilton Atlanta)
Photo(electro)catalytic N2 fixation with water under ambient conditions offers an ideal pathway for clean, sustainable, and decentralized ammonia production and might serve as a potential alternative to the capital and energy intensive Haber-Bosch process. To date, almost all photocatalysts for nitrogen reduction reaction (NRR) suffer from poor selectivity, low activity due to the difficulty in breaking the strong N2 triple bond, competition with the more favorable hydrogen evolution reaction (HER), and inefficient utilization of the solar spectrum. Here, a photo(electro)chemical setup is demonstrated using a hybrid plasmonic-semiconductor as an active photocatalyst under visible light. Hybrid hollow Au-Ag2O nanocages are utilized to convert atmospheric N2 to NH3 in a pure water system without using sacrificial reagents. The average NH3 production rate of 28.2 mg m-2 h-1 and the solar-to-ammonia (STA) conversion efficiency of 0.017% are achieved under one sun illumination. The apparent quantum efficiency of 1.2% for NH3 production is obtained with the monochromatic light source at 685 nm, which is among the highest ever-reported values for the photocatalytic NRR. The isotopic labeling experiments using 15N2 confirms that supplied N2 gas is the only source of NH3 formation in the system. This work showcases the application of plasmonic photocatalysis in the challenging multi-electron nitrogen fixation.
