Ammonia is one of the widely produced chemicals in the world, with broad applications in producing agricultural fertilizer, energy, and in the pharmaceutical industry. Photocatalytic nitrogen fixation for “green ammonia” synthesis, using water as a reducing reagent and sunlight under ambient conditions, provides an attractive route for clean, sustainable, and distributed ammonia synthesis. This approach might serve as an alternative to the thermochemical (Haber-Bosch process), particularly in remote areas where access to the centralized infrastructure or pipelines is limited. To date, almost all photocatalysts for nitrogen reduction reaction (NRR) suffer from poor selectivity, low activity due to the difficulty in breaking strong N[endif]--&gt;N bond, competition with the more favorable hydrogen evolution reaction (HER), and inefficient utilization of the solar spectrum. In this talk, a photo-electrochemical setup is demonstrated using a hybrid plasmonic-semiconductor as an active photocatalyst under visible light excitation. 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.

Plasmon-enhanced photochemical ammonia synthesis from nitrogen and water using visible-light responsive Au-Ag2O nanocages

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.