Ir-based perovskite oxides show great
promise for next-generation
oxygen evolution reaction (OER) electrocatalysts in an acidic medium,
but they are generally stuck with their uncontrollable surface amorphization
and thus structural instability (e.g., serious Ir
leaching) during OER. Herein, we report the high-yield chemical exfoliation
of Ruddlesden–Popper layered perovskite Sr2IrO4 into protonated colloidal nanosheets with an undamaged perovskite
framework. We further demonstrate the potential of protonated perovskite
nanosheets to evade the trade-off between OER activity and structural
stability. The 2D morphological benefit and nice monodispersity of
these protonated perovskite nanosheets enable the facile fabrication
of an ultralow-Ir-loading catalyst film (30 μg cm–2), which exhibits about 10 times higher activity than the IrO2 catalyst film and undergoes almost as much Ir leaching during
OER. Our joint experimental and theoretical results also reveal that
structural hydroxyl groups on the surface of protonated nanosheets
participate in the catalytic cycle of OER, and the protonated layered
perovskite framework represents an example of OER electrocatalyst
that works with a non-traditional adsorbate evolution mechanism.