A visible-light-photocatalytic water-splitting strategy for sustainable hydrogenation/deuteration of aryl chlorides
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摘要:
Hydrogenation/deuteration of carbon chloride (C-Cl) bonds is of high significance but remains a remarkable challenge in synthetic chemistry,especially using safe and inexpensive hydrogen donors.In this article,a visible-light-photocatalytic watersplitting hydrogenation technology (WSHT) is proposed to in-situ generate active H-species (i.e.,Had) for controllable hydrogenation of aryl chlorides instead of using flammable H2.When applying heavy water-splitting systems,we could selectively install deuterium at the C-Cl position ofaryl chlorides under mild conditions for the sustainable synthesis of high-valued added deuterated chemicals.Sub-micrometer Pd nanosheets (Pd NSs) decorated crystallined polymeric carbon nitrides (CPCN) is developed as the bifunctional photocatalyst,whereas Pd NSs not only serve as a cocatalyst of CPCN to generate and stabilize H (D)-species but also play a significant role in the sequential activation and hydrogenation/deuteration of C-Cl bonds.This article highlights a photocatalytic-WSHT for controllable hydrogenation/deuteration of low-cost aryl chlorides,providing a promising way for the photosynthesis of high-valued added chemicals instead of the hydrogen evolution.