研究领域

Organic Chemistry

One approach that we had taken to artificial photosynthesis is mimicry of the steps used by photosynthetic organisms to convert solar energy into chemical potential. Analogs of photosynthetic reaction centers consisting of tetrapyrrole chromophores covalently linked to electron acceptors and donors are designed and synthesized in our laboratory. Excitation of these artificial reaction centers results in a cascade of energy transfer/electron transfer processes which, in selected cases, forms a final charge separated state characterized by a giant dipole moment (>150 D), a quantum yield approaching unity, a significant fraction of the photon energy stored as chemical potential, and a lifetime sufficient for reaction with secondary electron donors and acceptors. Reaction with secondary electron/hole transfer species, in some cases, occurs in solution, in membranes, or through interactions with conductive surfaces. Recent examples of artificial constructs include mimicry of light harvesting by carotenoid pigments. Antenna systems are being synthesized based on polymer polyenes covalently attached to tetrapyrroles. Absorption from the blue-green to the red has been observed. Conformational disorder is thought to limit the effective conjugation length of the polymer providing a distribution of shorter effective conjugation lengths. Thus, the spectrum of the polyene polymer covers the entire visible spectrum, making it a nearly ideal antenna for sunlight. New antenna reaction center complexes in which a carotenoid moiety is located in quasi-conjugation to the tetrapyrroles p-system allowing fast energy transfer are being designed.

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"[FeFe]-Hydrogenase Catalyzed H2 Production in a Photoelectrochemical Biofuel Cell," M. Hambourger, M. Gervaldo, D. Svedruzic, P. W. King, D. Gust, M. Ghirardi, A. L. Moore and T. A. Moore, J. Am. Chem. Soc. 130 2015-2022 (2008) "Energy Transfer, Excited-State Deactivation and Exciplex Formation in Artificial Caroteno-Phthalocyanine Light Harvesting Antennas," R. Berera, I. H. M van Stokkum, G. Kodis, A. Keirstead, S. Pillai, C. Herrero, R. E. Palacios, M. Vengris, R. van Grondelle, D. Gust, T. A. Moore, A. L. Moore, and J. T. M. Kennis, J. Phys. Chem. B. 111 6868- 6877 (2007) "Charge Separation and Energy Transfer in a Caroteno-C60 Dyad: Photoinduced Electron Transfer from the Carotenoid Excited States," R. Berera, G. F. Moore, I. van Stokkum, G. Kodis, M. Gervaldo, R. van Grondelle, J. T. M. Kennis, D. Gust, T. A. Moore and A. L. Moore, Photochem. Photobiol. Sci. 5 1142-1149 (2006) "Tetrapyrrole Singlet Excited State Quenching by Carotenoids in an Artificial Photosynthetic Antenna," R. E. Palacios, G.Kodis, C. Herrero, E. M. Ochoa, M. Gervaldo, S. L. Gould, J. T. M. Kennis, D. Gust, T. A. Moore, and A. L. Moore, J. Phys. Chem. B. 110 25411-25420 (2006) "Conductance of a Biomolecular Wire," I. Visoly-Fisher, K. Daie, Y. Terazono, C. Herrero, F. Fungo, L. Otero, E. Durantini, J. J. Silber, L. Sereno, D. Gust, T. A. Moore, A. L. Moore and S. M. Lindsay, Proc. Natl. Acad. Sci. 103 8686-8690 (2006)