Heterometallic antenna-reactor complexes for photocatalysis.
Proc Natl Acad Sci U S A
; 113(32): 8916-20, 2016 08 09.
Article
en En
| MEDLINE
| ID: mdl-27444015
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 401. These observations indicate that antenna-reactor complexes may greatly expand possibilities for developing designer photocatalytic substrates.
Texto completo:
1
Banco de datos:
MEDLINE
Idioma:
En
Año:
2016
Tipo del documento:
Article