Satisfying the world’s steadily increasing energy demand from sustainable energy sources has become a key challenge for our society, including research on renewable energies and energy storage, such as H2 production from H2O. The low efficiency of conventional H2O electrolysis precludes large scale applications. Thus, catalysts are desired to make this otherwise convenient strategy more applicable. Due to its high reactivity and oxophilicity, as well as the large-scale availability, depleted uranium (238U) is widely discussed as an effective and economic catalyst for stable substrates. In our previous studies of the uranium-monoarene complex [(Ad,MeArO)3Mes)U] (1), unique electrochemical and well defined synthetic behavior were found, rendering the complex a perfect candidate for electrocatalysis. Indeed, already 0.02 mol% of 1 showed remarkable catalytic activity for H2O reduction, lowering the overpotential for H2 evolution by 0.5 V and increasing the steady state electrolysis current by a factor of 10. Synthetic studies of 1 with H2O showed the formation of a U(IV)-hydroxo species [(Ad,MeArO)3Mes)U-OH] (2) and H2 (a, Figure 1). In a second step, the homogeneous catalyst can be regenerated by electro-chemical reduction of 2, forming 1 and OH– to close the catalytic cycle (b, Figure 1).

U-mediated electrocatalytic H2 production from water with a molecular uranium coordination complex

251st National Meeting (2016)

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