Ionic Recognition Controlled by Conformational Change: A DFT Investigation

构象变化控制的离子识别:DFT研究

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Abstract

Ions play a crucial role in the production of important materials and are associated with various health and environmental issues. Noncovalent interactions serve as fundamental tools for controlling the availability of cations and/or anions. Herein, we investigate the ability of two conformations of the 2,6-bis(1,2,3-triazol-4-yl)pyridine molecule to recognize cations (1), such as Li(+), Na(+), or K(+), and anions (2), including F(-), Cl(-), or Br(-). EDA-NOCV analysis demonstrates that the conformers preferentially recognize ions based on the size of the cations (K(+) → Na(+) → Li(+)) and anions (Br(-) → Cl(-) → F(-)). The preferential interaction with smaller cations (and anions) arises from the more attractive electrostatic and orbital interactions (N(···.)cation and C-H(···.)anion bonds). The presence of electron-donor groups (-NH(2)) in the first conformer (1) enhances cation recognition through stronger electrostatic N(···.)cation interactions. Conversely, the presence of electron-acceptor groups (-NO(2)) in the second conformer (2) facilitates anion recognition via more favorable electrostatic, orbital, and dispersion C-H(···.)anion interactions. Cation recognition is found to be more favorable in the first conformer than anion recognition in the second due to more attractive electrostatic energy and/or less Pauli repulsive energy associated with (O or primarily N)(···.)cation interactions in 1 (···.)cations compared to (N or mainly C)-H(···.)anion bonds in 2 (···.)anions. These findings provide significant insights into the mechanisms of cation and/or anion recognition through different conformations using the same base structure and can inform the design of molecules with enhanced functionalities.

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