Preparation, Isolation, and Structural Characterization of Lewis Base Iminium Salts of 1,8-Diazabicyclo[5.4.0]undec-7-ene and Their Application as Green Reagents in an Aqueous Medium
Приготовление, выделение и структурная характеристика иминовых солей оснований Льюиса 1,8-диазабицикло[5.4.0]ундец-7-ена и их применение в качестве «зелёных» реагентов в водной среде
2024-11-21
SCID: 54.1/6enue9d7
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1,8-diazabicyclo[5.4.0]undec-7-eneDBULewis base iminium saltsN-substituent chemical shiftN-sulfonyl iminium saltsaqueous mediumbase-free functionalizationdensity functional theoryrecoverable reusable Lewis base
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Abstract (AI)
We report a state-of-the-art synthesis and isolation procedure for 13 Lewis base iminium salts (LBI) of 1,8-diazabicyclo[5.4.0]undec-7-ene (DBU), confirming their structures meticulously by different spectral data. The LBIs are distinct from their parent compound (DBU), which provides emphatic support in favor of LBI formation in various DBU-catalyzed reactions. Density functional theory studies of N-sulfonyl LBI of DBU have given new insight into alternate iminium salts, offering a new opportunity for further investigation. We describe the applications of three LBIs as direct reagents for base-free functionalization, broadening their scope as eco-friendly reagents in aquatic media. The Lewis base is recoverable and reusable to prepare the LBI after the reaction. We also document the influence of the N substituent on the chemical shift of these iminium salts.
Key Findings
1
DFT studies on N-sulfonyl DBU LBIs reveal alternative iminium salt structures, providing new mechanistic insight and avenues for further study.
2
LBIs are structurally distinct from parent DBU, supporting that iminium formation occurs in various DBU-catalyzed reactions.
3
Synthesized and isolated 13 distinct Lewis base iminium (LBI) salts derived from DBU with structures confirmed by multiple spectroscopic methods.
4
The Lewis base (DBU) can be recovered and reused to regenerate LBIs after reactions, enhancing reagent sustainability.
5
The N-substituent of the iminium salts affects their NMR chemical shifts, demonstrating substituent-dependent spectroscopic properties.
6
Three LBIs function as direct, base-free reagents for substrate functionalization in aqueous (green) media.
Research Object
Lewis base iminium salts (LBIs) of 1,8-diazabicyclo[5.4.0]undec-7-ene (DBU)
Research Subject
Their preparation, isolation, structural characterization (spectroscopic and DFT analysis), influence of N‑substituents on chemical shifts, and application as green, recoverable/reusable reagents for base-free functionalization in aqueous media
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2024-11-21
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