Heterometallic antenna−reactor complexes for photocatalysis
Top Cited Papers
- 21 July 2016
- journal article
- research article
- Published by Proceedings of the National Academy of Sciences in Proceedings of the National Academy of Sciences of the United States of America
- Vol. 113 (32), 8916-8920
- https://doi.org/10.1073/pnas.1609769113
Abstract
Metallic nanoparticles with strong optically resonant properties behave as nanoscale optical antennas, and have recently shown extraordinary promise as light-driven catalysts. Traditionally, however, heterogeneous catalysis has relied upon weakly light-absorbing metals such as Pd, Pt, Ru, or Rh to lower the activation energy for chemical reactions. Here we show that coupling a plasmonic nanoantenna directly to catalytic nanoparticles enables the light-induced generation of hot carriers within the catalyst nanoparticles, transforming the entire complex into an efficient light-controlled reactive catalyst. In Pd-decorated Al nanocrystals, photocatalytic hydrogen desorption closely follows the antenna-induced local absorption cross-section of the Pd islands, and a supralinear power dependence strongly suggests that hot-carrier-induced desorption occurs at the Pd island surface. When acetylene is present along with hydrogen, the selectivity for photocatalytic ethylene production relative to ethane is strongly enhanced, approaching 40:1. These observations indicate that antenna−reactor complexes may greatly expand possibilities for developing designer photocatalytic substrates.Keywords
Funding Information
- Welch Foundation (C-1220)
- Welch Foundation (C-1222)
- DOD | Air Force Office of Scientific Research (FA9550-15-1-0022)
- DOD | Air Force Office of Scientific Research (FA9550-15-1-0022)
- DOD | Air Force Office of Scientific Research (FA9550-15-1-0022)
- DOD | Air Force Office of Scientific Research (FA9550-15-1-0022)
- DOD | Air Force Office of Scientific Research (FA9550-15-1-0022)
- DOD | Air Force Office of Scientific Research (FA9550-15-1-0022)
- DOD | Air Force Office of Scientific Research (FA9550-15-1-0022)
- DOD | Air Force Office of Scientific Research (FA9550-15-1-0022)
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