Catalyzing water splitting is a promising way to meet increasing global clean energy demand. Water reduction is already well-catalyzed by Pt and its analogues; however, the water oxidation (WO) half-reaction lags behind its counterpart. Rational design of new catalysts requires a clear understanding of the WO mechanism, but mechanistic studies on Ir-based catalysts can be particularly challenging due to the short lifetimes of associated intermediates. In this work, we use surface-enhanced infrared absorption spectroscopy (SEIRAS) to build on recent reports that active site structure can fundamentally change the WO mechanism on metal oxide catalysts. By comparing WO on atomically-defined Ir dinuclear heterogeneous catalysts (Ir-DHCs) and ill-defined IrO<sub>x</sub>, we further elucidate the effect of extended active site structure on WO mechanisms.

Probing water oxidation pathways on atomically-defined Ir catalysts through SEIRAS

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ACS Fall 2022

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