Molecular engineering of a cobalt-based electrocatalytic nanomaterial for H2 evolution under fully a

Abstract

The viability of a hydrogen economy depends on the design of efficient catalytic systems based on earth-abundant elements. Innovative breakthroughs for hydrogen evolution based on molecular tetraimine cobalt compounds have appeared in the past decade. Here we show that such a diimine–dioxime cobalt catalyst can be grafted to the surface of a carbon nanotube electrode. The resulting electrocatalytic cathode material mediates H2 generation (55,000 turnovers in seven hours) from fully aqueous solutions at low-to-medium overpotentials. This material is remarkably stable, which allows extensive cycling with preservation of the grafted molecular complex, as shown by electrochemical studies, X-ray photoelectron spectroscopy and scanning electron microscopy. This clearly indicates that grafting provides an increased stability to these cobalt catalysts, and suggests the possible application of these materials in the development of technological devices. Efficient hydrogen-evolving catalysts comprising readily available elements are needed if hydrogen is to be adopted as a clean alternative to fossil fuels. Now, a diimine–dioxime cobalt complex has been covalently attached to a carbon nanotube electrode to yield an active and robust electrocatalyst for hydrogen generation (55,000 turnovers in seven hours) from aqueous solutions.

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Andreiadis, E., Jacques, PA., Tran, P. et al. Molecular engineering of a cobalt-based electrocatalytic nanomaterial for H₂ evolution under fully aqueous conditions. Nature Chem 5, 48–53 (2013). https://doi.org/10.1038/nchem.1481

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