Efficient Alkaline Water Oxidation with a Regenerable Nickel Pseudo-Complex

Efficient and robust electrocatalysts are required for the oxygen evolution reaction (OER). Photosystem II-inspired synthetic transition metal complexes have shown promising OER activity in water-poor or mild conditions, yet challenges remain in the improvement of current density and performance stability for practical applications in alkaline electrolytes in contrast to solid-state oxide catalysts. Here, we report that a nickel pseudo-complex (bpy)(z)NiOxHy (bpy = 2,2'-bipyridine) catalyst, which bridges solid oxide and molecular catalysts, exhibits the highest OER activity among nickel-based catalysts with a turnover frequency of 1.1 s(-1) at an overpotential of 0.30 volts, even outperforming iron-incorporated nickel (oxy)hydroxide under an identical nickel mass load. Benefiting from the strong coordination between bpy and nickel, this (bpy)(z)NiOxHy catalyst exhibits long-term stability in highly alkaline media at 1.0 mA cm(-2) for over 200 h and at 20 mA cm(-2) for over 60 h. Our findings indicate that dynamically coordinating a small amount of bpy in the catalyst layer efficiently sustains highly active nickel sites for water oxidation, demonstrating a general strategy for improving the activity of transition metal sites with active ligands beyond the incorporation of metal cations to form double-layered hydroxides.

Automated summary

A nickel pseudo-complex catalyst exhibited high OER activity and long-term stability in alkaline electrolytes, outperforming other nickel-based catalysts. Coordination of active ligands was found to sustain highly active nickel sites for water oxidation, offering a novel strategy for improving the efficiency of transition metal sites.