Author:
Swearer Dayne F.,Zhao Hangqi,Zhou Linan,Zhang Chao,Robatjazi Hossein,Martirez John Mark P.,Krauter Caroline M.,Yazdi Sadegh,McClain Michael J.,Ringe Emilie,Carter Emily A.,Nordlander Peter,Halas Naomi J.
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.
Funder
Welch Foundation
DOD | Air Force Office of Scientific Research
Publisher
Proceedings of the National Academy of Sciences
Cited by
368 articles.
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