Chuang Han, Guanqun Han, Shukai Yao, Lan Yuan, Xingwu Liu, Zhi Cao, Arun Mannodi‐Kanakkithodi, Yujie Sun

Nov 19, 2021
Advanced Science

Surfactant‐assisted synthesis enables to obtain defective ultrathin ZnIn2S4 nanosheets which can act as noble metal‐free photocatalysts for effective photoreductive deuteration of carbonyls and imines to produce deuterated alcohols and amines using D2O as the sole deuterium source under ambient conditions. Deuterium (D) labeling is of great value in organic synthesis, pharmaceutical industry, and materials science. However, the state‐of‐the‐art deuteration methods generally require noble metal catalysts, expensive deuterium sources, or harsh reaction conditions. Herein, noble metal‐free and ultrathin ZnIn2S4 (ZIS) is reported as an effective photocatalyst for visible light‐driven reductive deuteration of carbonyls to produce deuterated alcohols using heavy water (D2O) as the sole deuterium source. Defective two‐dimensional ZIS nanosheets (D‐ZIS) are prepared in a surfactant assisted bottom‐up route exhibited much enhanced performance than the pristine ZIS counterpart. A systematic study is carried out to elucidate the contributing factors and it is found that the in situ surfactant modification enabled D‐ZIS to expose more defect sites for charge carrier separation and active D‐species generation, as well as high specific surface area, all of which are beneficial for the desirable deuteration reaction. This work highlights the great potential in developing low‐cost semiconductor‐based photocatalysts for organic deuteration in D2O, circumventing expensive deuterium reagents and harsh conditions.

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