The development of efficient and inexpensive catalysts capable of solar-to-fuel energy conversion is vital for mitigating the adverse effects of carbon-based fuels on the environment and meeting the rising global energy demand. Immobilization of molecular catalytic units is an attractive strategy to combine homogeneous and heterogeneous catalysis for electrolysis applications. Metal-organic frameworks have received huge attention in the last years as promising porous materials for a wide range of applications, including electrocatalysis. We demonstrate here the successful integration of metal dithiolene units into two-dimensional extended frameworks by using 2,3,6,7,10,11-triphenylenehexathiolate as the supporting ligand. The developed metal dithiolene frameworks display remarkable activity for the electrocatalytic conversion of water into hydrogen and their physical properties have been explored. The ligand framework allows for excellent control of electronic effects, which will facilitate structure-activity studies. Our innovative synthetic strategy offers an unprecedented control over the physical and chemical properties of these systems, which will ultimately allow us to rationally design and dial-in their desired electronic and catalytic properties. We expect the design principles discovered in these studies to have a profound impact towards the development of advanced materials and sustainable technologies.<br/>

Metal dithiolene frameworks with tunable physical and chemical properties

254th National Meeting (2017)

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