Research in the Marinescu group focuses on fundamental research to understand, design, and synthesize novel catalytic systems essential to the development of efficient solar-to-fuel technologies. Inspired by biological systems, we innovate molecular catalysts that involve hydrogen bonding networks capable of small molecule activation, and multiple proton and electron transfers. We have shown that cobalt complexes with pendant proton relays (NH groups) act as highly efficient catalysts for the reduction of CO2 to CO, and that the presence of the pendant NH moiety is crucial for catalysis.
We also explore the immobilization of metal complexes to electrodes as a method to combine homogeneous and heterogeneous catalysis. Metal-organic frameworks (MOFs) have emerged as a promising class of materials; however, the insulating nature of MOFs has limited their application as electrocatalysts. We have shown that metal dithiolene units can be successfully integrated into one- and two-dimensional (1D/2D) frameworks. The generated coordination polymers display unique electronic properties ‚Ä" they catalyze with remarkable activity the electrocatalytic conversion of water into hydrogen, and their electrical conductivity is among that of the best coordination polymers. We expect the design principles discovered in these studies to have a profound impact towards the development of advanced materials and sustainable technologies.
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