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Molecular Photosynthesis: Such Stuff as Dreams are Made On

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The use of solar-activated H2O /CO2 routines as a feed-stock for photosynthetic processes is nowadays a breakthrough concept for sustainable energy, solar fuels, green chemistry and food security. The enormous potential of this vital cycle is far from being adequately exploited. Indeed, Natural Photosynthesis will not be adequate to feed the world and power its energy needs in the next decades. As a result of a population increase up to 9 billion people, the global demand for food and energy will increase more than 60% by 2050. In this time-frame, a spontaneous, evolutionary burst of the Natural Machinery is out of reach.

The game-changer relies on a man-made re-design of photosynthesis to overcome the natural bottlenecks, efficiency losses, and govern land exploitation conflicts for food and energy (bio-fuels) production. The urgency is such that we need to accelerate the equivalent of 100 million years evolution to orders of magnitude less contingency. Research on Artificial Photosynthesis is taking the risk of this revolution, by focussing on the high-gain of a sustainable, clean and secure future “….the guarded secret of the plants, mastered by human industry which will know how to make them bear even more abundant fruit than nature, for Nature is not in a hurry and mankind is” (Giacomo Ciamician “The photochemistry of the future” Science 1912, 36, 385-394). An extraordinary research effort has been dedicated to elucidate the structural and mechanistic prerogatives of the natural oxygen evolving complex embedded within the photosystem II enzyme (PSII-OEC). A recent breakthrough in the field of artificial photosynthesis is the discovery of synthetic multi-redox catalysts, as analogs of the PSII -OEC (Scheme 1), with a common functional-motif, i.e. a redox-active, tetranuclear {M4(-O)4 core boosting H2O oxidation to O2 with unprecedented efficiency. Our vision points to a careful choice/design of the catalytic core, of its ligand set and of the surrounding nano-environment. We report herein a combined synthetic, spectroscopic and mechanistic study on the use multi-metal catalysts for water oxidation and their combined use with visible light sensitizers and carbon nanostructures (CNS). The outcome is a hybrid nanomaterial with unperturbed CNS electrical properties, enabling water splitting with high efficiency at overpotentials as low as the natural protein.

1) Bonchio, M.; Fornasiero, P.; Prato M. et al. Energy Environ. Sci. 2018, 11, 1571-1580 2) Squarcina, A.; Sorarù, A.; Rigodanza, F., Carraro, M.; Bonchio, M. et al. ACS Catal. 2017, 7, 1971-1976. 3) Sartorel, A.; Scandola, F.; Kortz, U.; Bonchio, M. et al. Angew. Chem. Int. Ed., 2014.,126, 11364-11367.; 4) Piccinin, S.; Sartorel, A.; Aquilanti, G.; Goldoni, A.; Bonchio, M.; Fabris, S. PNAS 2013 , 110, 4917-4922 5) Sartorel, A.; Bonchio, M.; Campagna, S.; Scandola, F. Chem. Soc. Rev. 2013, 42, 2262-2280. 6) Paolucci, F.; Prato, M.; Bonchio, M. et al. ACS Nano 2013, 7, 811; Nature Chem. 2010, 2, 826-831.

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