Two-dimensional metal dithiolene metal-organic frameworks as conductive materials for solar energy conversion

Abstract

Electrocatalytic hydrogen evolution from water using solar energy is one potential pathway towards a clean energy economy. The work in this dissertation attempted to improve upon the stability and activity of a well-studied hydrogen-evolving cobalt dithiolene electrocatalyst by incorporating it into a metal-organic framework (MOF). This work shows that metal dithiolene units can be successfully integrated into two-dimensional frameworks, and that the generated coordination polymers function as efficient electrocatalysts for the hydrogen evolving reaction under fully aqueous conditions. Their electrical conductivity was also investigated and shown to be among that of the best coordination polymers. The design principles demonstrated in these studies have had a significant impact on the development of other catalytically-active frameworks in the field and will hopefully lead to more efficient devices for solar energy conversion and storage.