<br/>Hydrogen production through the reduction of water has emerged as an important strategy for the storage of renewable energy in chemical bonds. One attractive scenario for the construction of efficient devices for electrochemical splitting of water requires the attachment of stable and active hydrogen evolving catalysts to electrode surfaces, which remains a significant challenge. Molecular catalysts are attractive because the ligand environment allows for tuning of their reduction potentials and chemical properties. However, the reported methods for the immobilization of molecular catalysts onto electrodes are scarce and suffer from low catalyst loadings. 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 cobalt dithiolene catalysts into metal-organic surfaces to generate very active modified cathodes for hydrogen generation from water. These materials display low overpotential and remarkable activity and stability under acidic conditions, much higher than those of the molecular complex, suggesting that immobilization as metal-organic surface provides a significant increase in efficiency and thus paves the way towards development of practical devices. Moreover, these materials can be integrated with planar <i>p</i>-type Si to generate very efficient photocathode materials for solar-driven hydrogen production from water.

One and two dimensional cobalt dithiolene frameworks for artificial photosynthesis

253rd National Meeting (2017)

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