Plasmonic Photocatalysis of Nitrous Oxide into N2 and O2 Using Aluminum–Iridium Antenna–Reactor Nanoparticles

Abstract
Photocatalysis with optically active “plasmonic” nanoparticles is a growing field in heterogeneous catalysis, with the potential for substantially increasing efficiencies and selectivities of chemical reactions. Here the decomposition of nitrous oxide (N2O), a potent anthropogenic greenhouse gas, on illuminated aluminum-iridium (Al-Ir) antenna-reactor plasmonic photocatalysts, is reported. Under resonant illumination conditions, N2 and O2 are the only observable decomposition products, avoiding the problematic generation of NOx species observed using other approaches. Because no appreciable change to the apparent activation energy was observed under illumination, the primary reaction enhancement mechanism for Al-Ir is likely due to photothermal heating, rather than plasmon-induced hot-carrier contributions. This light-based approach can induce autocatalysis for rapid N2O conversion, a process with highly promising potential for applications in N2O abatement technologies, satellite propulsion, or emergency life-support systems in space stations and submarines.
Funding Information
  • Welch Foundation (C-1220, C-1222)
  • Division of Graduate Education (1450681)
  • Air Force Office of Scientific Research (MURI FA9550-15-1-0022)