Prospects in light-driven water activation have prompted rapid progress in hydrogenation reactions. We describe a Ni -N site built on carbon nitride for catalyzed semihydrogenation of alkynes, with water supplying protons, powered by visible-light irradiation. Importantly, the photocatalytic approach developed here enabled access to diverse deuterated alkenes in D O with excellent deuterium incorporation. Under visible-light irradiation, evolution of a four-coordinate Ni species into a three-coordinate Ni species was spectroscopically identified. In combination with theoretical calculations, the photo-evolved Ni is posited as HO-Ni -N with an uncoordinated, protonated pyridinic nitrogen, formed by coupled Ni reduction and water dissociation. The paired Ni-N prompts hydrogen liberation from water, and it renders desorption of alkene preferred over further hydrogenation to alkane, ensuring excellent semihydrogenation selectivity.
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