期刊
NATURE COMMUNICATIONS
卷 10, 期 -, 页码 -出版社
NATURE PORTFOLIO
DOI: 10.1038/s41467-019-12018-7
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资金
- JST-PRESTO [JPMJPR1544]
- Japan Society for the Promotion of Science (JSPS) [26220911, A18H020740]
- MEXT
- MEXT program Elements Strategy Initiative to Form Core Research Center
The hydrogen isotope deuterium is widely used in the synthesis of isotopically-labeled compounds and in the fabrication of semiconductors and optical fibers. However, the facile production of deuterium gas (D-2) and hydrogen deuteride (HD) in a controlled manner is a challenging task, and rational heterogeneously-catalyzed protocols are still lacking. Herein, we demonstrate the selective production of hydrogen isotope compounds from a combination of formic acid and D2O, through cooperative action by a PdAg nanocatalyst on a silica substrate whose surface is modified with amine groups. In this process, D-2 is predominantly evolved by the assist of weakly basic amine moieties, while nanocatalyst particles in the vicinity of strongly basic amine groups promote the preferential formation of HD. Kinetic data and calculations based on semi-classically corrected transition state theory coupled with density functional theory suggest that quantum tunneling dominates the hydrogen/deuterium exchange reaction over the metallic PdAg surfaces.
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