Heterometallic antenna-reactor complexes for photocatalysis

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

Research output: Contribution to journalArticle

162 Scopus citations

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.

Original languageEnglish (US)
Pages (from-to)8916-8920
Number of pages5
JournalProceedings of the National Academy of Sciences of the United States of America
Volume113
Issue number32
DOIs
StatePublished - Aug 9 2016

All Science Journal Classification (ASJC) codes

  • General

Keywords

  • Catalysis|aluminum
  • Nanoparticle
  • Photocatalysis
  • Plasmon

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  • Cite this

    Swearer, D. F., Zhao, H., Zhou, L., Zhang, C., Robatjazi, H., Martirez, J. M. P., Krauter, C. M., Yazdi, S., McClain, M. J., Ringe, E., Carter, E. A., Nordlander, P., & Halas, N. J. (2016). Heterometallic antenna-reactor complexes for photocatalysis. Proceedings of the National Academy of Sciences of the United States of America, 113(32), 8916-8920. https://doi.org/10.1073/pnas.1609769113