Photodriven charge separation dynamics in CdSe/ZnS core/shell quantum dot/cobaloxime hybrid for efficient hydrogen production

Jier Huang, Karen L. Mulfort*, Pingwu Du, Lin X. Chen

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

235 Scopus citations

Abstract

Photodriven charge-transfer dynamics and catalytic properties have been investigated for a hybrid system containing CdSe/ZnS core/shell quantum dots (QDs) and surface-bound molecular cobaloxime catalysts. The electron transfer from light-excited QDs to cobaloxime, revealed by optical transient absorption spectroscopy, takes place with an average time constant of 105 ps, followed a much slower charge recombination process with a time constant of ≫3 ns. More interestingly, we also observed photocatalytic hydrogen generation by this QD/cobaloxime hybrid system, with >10-000 turnovers of H 2 per QD in 10 h, using triethanolamine as a sacrificial electron donor. These results suggest that QD/cobaloxime hybrids succeed in coupling single-photon events with multielectron redox catalytic reactions, and such systems could have potential applications in long-lived artificial photosynthetic devices for fuel generation from sunlight.

Original languageEnglish (US)
Pages (from-to)16472-16475
Number of pages4
JournalJournal of the American Chemical Society
Volume134
Issue number40
DOIs
StatePublished - Oct 10 2012

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

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