光催化
化学
光化学
材料科学
催化作用
生物化学
作者
Dayne F. Swearer,Hangqi Zhao,Linan Zhou,Chao Zhang,Hossein Robatjazi,John Mark P. Martirez,Caroline M. Krauter,Sadegh Yazdi,Michael J. McClain,Emilie Ringe,Emily A. Carter,Peter Nordlander,Naomi J. Halas
标识
DOI:10.1073/pnas.1609769113
摘要
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.
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