The photochemistry of transition metal monohydrides is relatively unexplored, even though such hydrides are common intermediates in solar fuels catalysis. The iridium hydride [Cp*Ir(bpy)(H)]+ has the remarkable ability to generate H2 from aqueous solutions photochemically, which has been harnessed to achieve molecular photoelectrocatalytic water splitting. To understand the photochemistry of monohydride complexes, detailed thermodynamic and kinetic studies have been carried out in water and acetonitrile, leading to the discovery of a new “self-quenching” mechanism for extremely efficient hydrogen evolution from the triplet excited state of [Cp*Ir(bpy)(H)]+. Details of this new mechanism and implications in catalysis will be discussed.

Mechanisms of photochemical H2 evolution from organometallic iridium hydrides

254th National Meeting (2017)

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