Sustainable hydrogen evolution reaction (HER) from water has emerged as a promising pathway for the storage and conversion of solar energy in chemical bonds. Hydrogen is a valuable energy carrier that can be transformed into electricity using fuel cell technology or used in the production of industrially relevant chemicals such as ammonia and methanol. Heterogenization of molecular catalysts is an attractive strategy to combine the advantageous properties of homogeneous and heterogeneous catalysis. Metal-organic frameworks (MOFs) have emerged as a promising class of materials; however, their insulating nature has limited their application as electrocatalysts. We have demonstrated the successful integration of metal dithiolene units into one and two-dimensional frameworks by using dinucleating and trinucleating thiolate-based ligand scaffolds. The developed metal dithiolene frameworks display high activity for the electrocatalytic HER in acidic aqueous media. The HER performance of the MOF-based electrocatalysts is investigated, to understand the charge transfer properties of the constructed MOF/electrode architecture. Additionally, the electronic conductivity values of the developed MOFs are among that of the best organic conductors, and are switchable from semiconducting to metallic. We expect the design principles discovered in these studies to have a profound impact towards the development of advanced materials and sustainable technologies.

Conductive metal-organic frameworks for electrocatalytic H<sub>2</sub> evolution

2019 Fall National Meeting

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Conductive metal-organic frameworks for electrocatalytic H2 evolution

Conductive metal-organic frameworks for electrocatalytic H₂ evolution