Heterobinuclear Light Absorber Coupled to Molecular Wire for Charge Transport across Ultrathin Silica Membrane for Artificial Photosynthesis

ACS Applied Materials & Interfaces
Georgios Katsoukis, Heinz Frei

Abstract

Coupling of robust, all-inorganic heterobinuclear light absorbers to metal oxide catalysts for water oxidation across an ultrathin product-separating silica membrane requires charge transfer through organic molecular wires embedded in the silica. A synthetic approach for assembling the bimetallic units on the silica surface is introduced that is compatible with the presence of encapsulated organic molecules. Accurate selection and fine tuning of the concentration of embedded conducting wires are enabled by a two-step method consisting of surface attachment of a tripodal anchor, trimethoxysilyl aniline, followed by attachment of p-oligo(phenylene vinylene) through amide linkage. Each step of the assembly process was monitored and characterized by a combination of Fourier transform infrared, Fourier transform-Raman, and UV-vis spectroscopy techniques. Hole transfer was observed from transient CoIII, formed by TiIVOCoII → TiIIIOCoIII charge transfer excitation of the chromophore, to p-oligo(phenylene vinylene) molecule within the 8 ns width of the photolysis laser pulse by transient optical absorption spectroscopy of the wire radical cation. The rectifying property of the light absorber-wire assembly enabled by appropriate selecti...Continue Reading

References

May 28, 2008·Langmuir : the ACS Journal of Surfaces and Colloids·Akihiro OkamotoKazuhito Hashimoto
Jul 12, 2008·Langmuir : the ACS Journal of Surfaces and Colloids·Philippe BanetDaniel Brunel
May 1, 2009·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Manuel PiacenzaFabio Della Sala
Sep 1, 2012·Journal of the American Chemical Society·Han Sen SooHeinz Frei
Nov 28, 2013·Proceedings of the National Academy of Sciences of the United States of America·Aaron K VannucciThomas J Meyer
Nov 29, 2014·Faraday Discussions·Guangbi YuanHeinz Frei
Aug 31, 2016·Accounts of Chemical Research·Wooyul KimHeinz Frei

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