Journal
SCIENCE
Volume 362, Issue 6410, Pages 69-+Publisher
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.aat6967
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Funding
- Air Force Office of Scientific Research Multidisciplinary Research Program of the University Research Initiative [MURI FA9550-15-1-0022]
- Welch Foundation [C-1220, C-1222]
- National Science Foundation [1450681]
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Photocatalysis based on optically active, plasmonic metal nanoparticles has emerged as a promising approach to facilitate light-driven chemical conversions under far milder conditions than thermal catalysis. However, an understanding of the relation between thermal and electronic excitations has been lacking. We report the substantial light-induced reduction of the thermal activation barrier for ammonia decomposition on a plasmonic photocatalyst. We introduce the concept of a light-dependent activation barrier to account for the effect of light illumination on electronic and thermal excitations in a single unified picture. This framework provides insight into the specific role of hot carriers in plasmon-mediated photochemistry, which is critically important for designing energy-efficient plasmonic photocatalysts.
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