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Oriented External Electric Fields: Tweezers and Catalysts for Reactivity in Halogen-Bond Complexes
Chao Wang1,2, David Danovich1, Hui Chen2
1Institute of Chemistry , The Hebrew University of Jerusalem , Jerusalem 9190407 , Israel.
Journal of the American Chemical Society
|April 5, 2019
Summary
Oriented-external electric fields (OEEFs) catalyze uncommon halogen bond (XB) displacement reactions. These electric fields control reactivity, enabling spontaneous, barrier-free reactions at critical strengths.
Area of Science:
- Theoretical Chemistry
- Chemical Physics
Background:
- Halogen bonds (XB) are crucial in molecular interactions.
- Displacement reactions involving XBs typically have high energy barriers.
- Controlling XB reactivity is essential for chemical synthesis.
Purpose of the Study:
- To investigate methods for controlling and enabling XB displacement reactions.
- To explore the catalytic effect of oriented-external electric fields (OEEFs) on XB reactivity.
- To understand the mechanism of OEEF-induced catalysis.
Main Methods:
- Theoretical study of 14 XB systems.
- Analysis of reaction barriers in gas and solvent phases.
- Application of valence bond modeling.
- Simulations using oriented-external electric fields (OEEFs).
Main Results:
- OEEFs act as 'electric tweezers,' catalyzing XB displacement reactions by tens of kcal/mol.
- Reversed OEEF direction inhibits reactions and weakens XB interactions.
- At critical OEEF strengths, reactions become spontaneous and barrier-free.
- OEEFs provide precise control over XB structure and reactivity.
Conclusions:
- OEEFs offer a powerful method for controlling and enabling challenging chemical reactions.
- This catalytic approach opens new avenues for manipulating molecular reactivity.
- Valence bond modeling elucidates the mechanism of electric field control.
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