Abstract

Semiconductor photocatalysis holds promising keys to address various energy and environmental challenges. Most studies to date are based on ensemble analysis, which may mask critical photocatalytic kinetics in single nanocatalysts. Here we report a study of imaging photocatalytic hydrogen production of single CdS nanoparticles with a plasmonic microscopy in an in operando manner. Surprisingly, we find that the photocatalytic reaction switches on and off stochastically despite the fact that the illumination is kept constant. The on and off states follow truncated and full-scale power-law distributions in broad time scales spanning 3–4 orders of magnitude, respectively, which can be described with a statistical model involving stochastic reactions rates at multiple active sites. This phenomenon is analogous to fluorescence photoblinking, but the underlying mechanism is different. As individual nanocatalyst represents the elementary photocatalytic platform, the discovery of the intermittent nature of the photocatalysis provides insights into the fundamental photochemistry and photophysics of semiconductor nanomaterials, which is anticipated to substantially benefit broad application fields such as clean energy, pollution treatment, and chemical synthesis.

Original languageEnglish (US)
Pages (from-to)10566-10571
Number of pages6
JournalProceedings of the National Academy of Sciences of the United States of America
Volume114
Issue number40
DOIs
Publication statusPublished - Oct 3 2017

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Keywords

  • Intermittent activity
  • Semiconductor photochemistry
  • Semiconductor photophysics
  • Single-nanoparticle catalysis
  • Surface plasmon resonance microscopy

ASJC Scopus subject areas

  • General

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