Picosecond optical and X-ray absorption spectroscopies with time-dependent density functional theory revealed the reaction pathways, electronic and structural conformations of Ir-Co hydrogen evolution photocatalysts. The dyad bearing 2-phenylpyridine ancillary ligands produced more photoreduced Co(II) than its 2-phenylisoquinoline analogue. These findings are important for designs of earth-abundant photosensitizers for photocatalytic applications.
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