Annual Scientific Report 2017

Abstract

Nature inspire us, we would like to mimic the transformations that sustain life. However, although these are fundamental processes, they have a huge technological potential that remains unharnessed. We aim to transfer concepts from artificial photosynthesis to the organic synthesis, to carry out endergonic transformations using sun-light as a driving force. These studies will trigger the development of new and greener and sustainable methodologies for the synthesis of fuels and transformation of organic molecules.

To this end, we are currently investigating transformations catalysed by the reactivity of first row transition metals (1RTM) Such as i) multi-proton/-electron reactions such as water oxidation, water and CO₂ reduction and reductions of organic compounds as well as ii) electro- and photocatalytic C-X (X = H, F, Cl or Br) activations mediated by biomimetic complexes based on earth abundant elements. Special emphasis is done on unravel the operative mechanisms by combination physical inorganic and organic chemistry, and theoretical methods. We are also rationally designing catalytic systems, with the aid of high-throughput screening techniques (HST), for the development of synthetic applications of interest.

Topics addressed

• Water Oxidation and high oxidation states
• Water and CO₂ Reduction
• High-throughput experimental techniques

Articles

“Making and Breaking of the O-O Bond at Iron Complexes” Coord. Chem. Rev. 2017, 334, 2-24.
Ilaria Gamba, Zoel Codolà, Julio Lloret-Fillol, Miquel Costas

“Generation, spectroscopic and chemical characterization of an octahedral iron (V) – nitrido species with a neutral TACN-based pentadentate ligand platform” J. Am. Chem. Soc., 2017, 139, 9168–9177.
Gerard Sabenya, Laura Lázaro, Ilaria Gamba, Vlad Martin-Diaconescu, Erik Andris, Thomas Weyhermüller, Frank Neese, Jana Roithova, Eckhard Bill, Julio Lloret-Fillol, Miquel Costas

“Cobalt-Copper Dual Light-Driven Catalytic Reduction of Aldehydes and Aromatic Ketones in Aqueous Media” Chem. Sci., 2017, 8, 4739-4749.
Arnau Call, Carla Casadevall, Ferran Acuña-Parés, Alicia Casitas, and Julio Lloret-Fillol