Synthesis and Properties of Multiredox Molecular Systems of Transition Metals

CATTANEO, MAURICIO

Buenos Aires

Conferencia; Shaping the Future of German-Argentinian Scientific Cooperation ? The Role of Curiosity-Driven Research; 2018

Alexander von Humboldt Foundation

Multiple proton-coupled electron transfer (PCET) processes are key steps in natural processes such as photosynthesis, cell respiration and nitrogen fixation. Understanding their relevant parameters is necessary to design systems with long-lived charge separated states that may lead to artificial molecular devices for efficient conversion of solar into electrical or chemical energy or design of novel multiredox catalyst.Accumulation of several redox equivalents in one molecular unit allows concentration of chemical energy that can be further interconverted with other molecules with perspectives in new catalytic processes, as for example water oxidation by ruthenium molecular catalysts. Also, using light to produce with its energy a movement of more than a redox equivalent will endeavor accumulation of energy.Transition metal complexes can be modified to have access to several oxidation states, which can include ligands with also redox properties. This allows to these systems a broad spectrum of multiderox processes that can be accessed. Polypyridine Rhenium and Ruthenium complexes, moreover its rich ground state chemistry, can perform a diverse reactivity from their excited states. Some new compounds of ruthenium with primary amines where the a-carbon is fully protected allow complexes to reach higher oxidation coupled with loss of protons that stabilize the electronic charge of the molecule. Combining ground state and excited state chemistry of these molecular systems and combining them with PCET processes envision an advance in the understanding of multiredox fundamental parameters and develop of novel light induced chemistry processes, catalysis and energy storage.