4.8 Article

Near Unity Quantum Yield of Light-Driven Redox Mediator Reduction and Efficient H2 Generation Using Colloidal Nanorod Heterostructures

Journal

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 134, Issue 28, Pages 11701-11708

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/ja303698e

Keywords

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Funding

  1. Lonza Ltd. (Switzerland) as part of Lonza's LIFT program of long term innovation
  2. U.S. Department of Energy Office of Basic Energy Sciences, Solar Photochemistry Program [DE-FG02-07ER-15906]

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The advancement of direct solar-to-fuel conversion technologies requires the development of efficient catalysts as well as efficient materials and novel approaches for light harvesting and charge separation. We report a novel system for unprecedentedly efficient (with near-unity quantum yield) light-driven reduction of methylviologen (MV2+), a common redox mediator, using colloidal quasi-type II CdSe/CdS dot-in-rod nanorods as a light absorber and charge separator and mercaptopropionic acid as a sacrificial electron donor. In the presence of Pt nanoparticles, this system can efficiently convert sunlight into H-2, providing a versatile redox mediator-based approach for solar-to-fuel conversion. Compared to related CdSe seed and CdSe/CdS core/shell quantum dots and CdS nanorods, the quantum yields are significantly higher in the CdSe/CdS dot-in-rod structures. Comparison of charge separation, recombination and hole filling rates in these complexes showed that the dot-in-rod structure enables ultrafast electron transfer to methylviologen, fast hole removal by sacrificial electron donor and slow charge recombination, leading to the high quantum yield for MV2+ photoreduction. Our finding demonstrates that by controlling the composition, size and shape of quantum-confined nanoheterostructures, the electron and hole wave functions can be tailored to produce efficient light harvesting and charge separation materials.

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