Report
Teaser, summary, work performed and final results
Periodic Reporting for period 1 - GREENLIGHT_REDCAT (Towards a Greener Reduction Chemistry by Using Cobalt Coordination Complexes as Catalysts and Light-driven Water Reduction as a Source of Reductive Equivalents)
Teaser
A prerequisite for a future sustainable society is the development of alternative greener synthetic methods for the efficient production of chemicals without environmental harm. Among the different opportunities to this end, the use of freely accessible and widespread sunlight...
Summary
A prerequisite for a future sustainable society is the development of alternative greener synthetic methods for the efficient production of chemicals without environmental harm. Among the different opportunities to this end, the use of freely accessible and widespread sunlight to drive reactions has become an ambitious but challenging approach. In this regard, the project aims to merge concepts at the edge of the emerging fields of water splitting, solar fuels and photo-redox catalysis by exploring the capacity of coordination complexes initially developed for water reduction to perform light-driven catalytic transformations of organic substrates. To this end, we will develop bio-inspired catalytic systems by some means mimic natural photosynthesis. The development of these effective catalysts requires a detailed understanding of the reaction mechanisms involved.
The ultimate objective of the project is the development of new sustainable synthetic methods for greener selective catalytic reductions of organic substrates, without causing damage to the environment by chasing the use of visible light and water as sources of electrons and protons as reducing equivalents. We also aim for expanding the reactivity to a new methodology for electrophile-electrophile umpolung couplings by rational modification of the catalytic system from basic understating of the reactions. In addition, we will explore new strategies to control regioselectivity and/or enantioselectivity in photosynthetic transformations.
Work performed
We have developed new coordination complexes based on earth abundant elements and obtained artificial metalloenzymes. These new coordination complexes have been found high efficient catalysts that operates at fast reaction rates in several photocatalytic chemical transformations. For instance, our catalysts are highly active in the reduction of water to hydrogen and reduction of CO2 to fuels by using light as a source of energy. Moreover, we have also found that some of the developed catalysts are extraordinarily active in the photocatalytic reduction of ketones, aldehydes and olefins, obtaining extraordinary selectivities. In addition, we have also extended the reactivity to the activation of inert bonds in order to develop new methodologies for the synthesis of molecules with biological activity.
Fundamental understanding of the reactions Mechanistic studies on those complexes bring us to discover the non-innocent nature of the ligands used, as well as key intermediates of the catalytic cycle.
Final results
\"The chemical reactivity to be developed based on artificial photosynthetic schemes is presented in the long term as the \"\"dreamed technology\"\". This technology have the potential to be disruptive and open up newer and greener reductive chemical processes that only use water and light. In the long term and beyond the project, it is envisioned that the incorporation of artificial photosynthetic schemes for the synthesis of chemicals and fuels will incite a change of the current industrial, society and energy paradigm.\"