Journal
ADVANCED SCIENCE
Volume 9, Issue 3, Pages -Publisher
WILEY
DOI: 10.1002/advs.202103408
Keywords
carbonyls; deuteration; heavy water; noble metal-free; photocatalysis
Categories
Funding
- National Science Foundation [CHE-1955358, CHE-1955336]
- Herman Frasch Foundation [820-HF17]
- University of Cincinnati
- Purdue University
- NSF-MRI grant [CHE-1726092]
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This study introduces a noble metal-free and ultrathin ZnIn2S4 photocatalyst for deuteration reactions using heavy water as the sole deuterium source. By synthesizing defective two-dimensional ZIS nanosheets with surfactant assistance, the performance is significantly enhanced.
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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