Modelling Photosynthesis with ZnII-Protoporphyrin All-DNA G-Quadruplex/Aptamer Scaffolds |
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Authors: | Dr Guo-Feng Luo Yonatan Biniuri Dr Wei-Hai Chen Dr Jianbang Wang Ehud Neumann Henri-Baptiste Marjault Prof Rachel Nechushtai Dr Martin Winkler Prof Thomas Happe Prof Itamar Willner |
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Institution: | 1. Institute of Chemistry and Center for Nanoscience and Nanotechnology, The Hebrew University of Jerusalem, Jerusalem, 91904 Israel;2. Institute of Life Science, The Hebrew University of Jerusalem, Jerusalem, 91904 Israel;3. Department of Biochemistry of Plants, Ruhr-University Bochum, Germany |
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Abstract: | All-DNA scaffolds act as templates for the organization of photosystem I model systems. A series of DNA templates composed of ZnII-protoporphyrin IX (ZnIIPPIX)-functionalized G-quadruplex conjugated to the 3′- or 5′-end of the tyrosinamide (TA) aptamer and ZnIIPPIX/G-quadruplex linked to the 3′- and 5′-ends of the TA aptamer through a four-thymidine bridge. Effective photoinduced electron transfer (ET) from ZnIIPPIX/G-quadruplex to bipyridinium-functionalized tyrosinamide, TA-MV2+, bound to the TA aptamer units is demonstrated. The effectiveness of the primary ET quenching of ZnIIPPIX/G-quadruplex by TA-MV2+ controls the efficiency of the generation of TA-MV+.. The photosystem-controlled formation of TA-MV+. by the different photosystems dictates the secondary activation of the ET cascade corresponding to the ferredoxin-NADP+ reductase (FNR)-catalysed reduction of NADP+ to NADPH by TA-MV+., and the sequestered alcohol dehydrogenase catalysed reduction of acetophenone to 1-phenylethanol by NADPH. |
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Keywords: | artificial photosynthesis electron transfer energy conversion ferredoxin-NADP+ reductase nanobiotechnology |
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