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高橋開人 博士 (化學動態學與光譜組)

高橋開人 博士
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最新研究成果
Mei-Tsan Kuo, Kaito Takahashi,* and Jim Jr-Min Lin*
ChemPhysChem
Reactions of Criegee Intermediates are Enhanced by Hydrogen-atom Relay Through Molecular Design
We report a type of highly efficient double hydrogen atom transfer (DHAT) reaction. The reactivities of 3-aminopropanol and 2-aminoethanol towards Criegee intermediates (syn- and anti-CH3CHOO) were found to be much higher than those of npropanol and propylamine. Quantum chemistry calculation has confirmed that the main mechanism of these very rapid reactions is DHAT, in which the nucleophilic attack of the NHgroup is catalyzed by the OH group which acts as a bridge of HAT. Typical gas-phase DHAT reactions are termolecular reactions involving two hydrogen bonding molecules; these reactions are typically slow due to the substantial entropy reduction of bringing three molecules together. Putting the reactive and catalytic groups in one molecule circumvents the problem of entropy reduction and allows us to observe the DHAT reactions even at low reactant concentrations. This idea can be applied to improve theoretical predictions for atmospherically relevant DHAT reactions.
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