Journal
SCIENCE CHINA-CHEMISTRY
Volume 63, Issue 3, Pages 386-392Publisher
SCIENCE PRESS
DOI: 10.1007/s11426-019-9672-8
Keywords
deuteration; water-splitting; aryl chlorides; Pd nanosheets; carbon nitride
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Funding
- National Natural Science Foundation of China [21972094, 51701127, 21401190]
- China Postdoctoral Science Foundation [2017M612709]
- Guangdong Special Support Program, Pengcheng Scholar Program, Shenzhen Peacock Plan [KQJSCX20170727100802505, KQTD2016053112042971]
- Educational Commission of Guangdong Province [2016KTSCX126]
- Foundation for Distinguished Young Talents in Higher Education of Guangdong [2018KQNCX221]
- Shenzhen Innovation Program [JCYJ 20170818142642395]
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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., H-ad) for controllable hydrogenation of aryl chlorides instead of using flammable H-2. When applying heavy water-splitting systems, we could selectively install deuterium at the C-Cl position of aryl 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.
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