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Self-assembled molecular p/n junctions for applications in dye-sensitized solar energy conversion

Nature Chemistry volume 8, pages 845–852 (2016)Cite this article

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A Corrigendum to this article was published on 22 September 2016

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Abstract

The achievement of long-lived photoinduced redox separation lifetimes has long been a central goal of molecular-based solar energy conversion strategies. The longer the redox-separation lifetime, the more time available for useful work to be extracted from the absorbed photon energy. Here we describe a novel strategy for dye-sensitized solar energy applications in which redox-separated lifetimes on the order of milliseconds to seconds can be achieved based on a simple toolkit of molecular components. Specifically, molecular chromophores (C), electron acceptors (A) and electron donors (D) were self-assembled on the surfaces of mesoporous, transparent conducting indium tin oxide nanoparticle (nanoITO) electrodes to prepare both photoanode (nanoITO|–A–C–D) and photocathode (nanoITO|–D–C–A) assemblies. Nanosecond transient-absorption and steady-state photolysis measurements show that the electrodes function microscopically as molecular analogues of semiconductor p/n junctions. These results point to a new chemical strategy for dye-sensitized solar energy conversion based on molecular excited states and electron acceptors/donors on the surfaces of transparent conducting oxide nanoparticle electrodes.

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Figure 1: Layer-by-layer molecular p/n junction assemblies on mesoporous nanoITO electrodes.
Figure 2: UV-vis absorptivity and absorbance spectra for individual molecular components and assembled photoanodes, respectively.
Figure 3: Summary of bias-dependent transient-absorption measurements on the photoanode assembly nanoITO|–MV2+–RuP22+–DA.
Figure 4: Summary of bias-dependent transient-absorption measurements on the photocathode assembly nanoITO|–DA–RuP22+–MV2+.
Figure 5: Steady-state photolysis of photoanode and photocathode assemblies.

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Change history

  • 24 August 2016

    In the version of this Article originally published, the affiliation details for Kyung-Ryang Wee were not correct, these have been updated in the online versions of this paper.

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Acknowledgements

This material is based on work supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, under Award No. DE-FG02-06ER15788.

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Authors and Affiliations

  1. Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, 27599-3290, North Carolina, USA

    Byron H. Farnum & Thomas J. Meyer

  2. Department of Chemistry, Daegu University, Gyeongsan, 712-714, Republic of Korea

    Kyung-Ryang Wee

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Contributions

B.H.F. and T.J.M. conceived and designed the experiments. K.R.W. synthesized the molecular species. B.H.F. assembled the electrodes and performed the transient-absorption and photolysis experiments. B.H.F. and T.J.M. wrote the paper.

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Correspondence to Thomas J. Meyer.

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Farnum, B., Wee, KR. & Meyer, T. Self-assembled molecular p/n junctions for applications in dye-sensitized solar energy conversion. Nature Chem 8, 845–852 (2016). https://doi.org/10.1038/nchem.2536

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