Highly active and stable surface structure for oxygen evolution reaction originating from balanced dissolution and strong connectivity in BaIrO3 solid solutions

Abstract

Catalysts for the oxygen evolution reaction (OER) are receiving great interest since OER remains the bottleneck of water electrolyzers for hydrogen production. Especially, OER in acidic solutions is crucial since it produces high current densities and avoids precipitation of carbonates. However, even the acid stable iridates undergo severe dissolution during the OER. BaIrO₃ has the strongest IrO₆ connectivity and stable surface structure, yet it suffers from lattice collapse after OER cycling, making it difficult to improve the OER durability. In the present study, we have successfully developed an OER catalyst with both high intrinsic activity and stability under acidic conditions by preventing the lattice collapse after repeated OER cycling. Specifically, we find that the substitution of Ir-site with Mn for BaIrO₃ in combination with OER cycling leads to a remarkable activity enhancement by a factor of 28 and an overall improvement in stability. This dual enhancement of OER performance was accomplished by the novel strategy of slightly increasing the Ir-dissolution and balancing the elemental dissolution in BaIr_1−xMn_xO₃ to reconstruct a rigid surface with BaIrO₃-type structure. More importantly, the mass activity for BaIr_0.8Mn_0.2O₃ reached ∼73 times of that for IrO₂, making it a sustainable and promising OER catalyst for energy conversion technologies.