Document Type

Article

Journal/Book Title

The Journal of Physical Chemistry A

Publication Date

4-26-2017

Publisher

American Chemical Society

Volume

121

Issue

18

First Page

1

Last Page

23

Abstract

Receptors for halide anions are constructed based on the imidazolium unit, and then replacing the H-bonding C-H group firstby halogen-bonding C-I and then by tetrel-bonding C-SnH3 and C-SiF3.Attaching a phenyl ring to any of these species has little effect on its ability to bind a halide, but incorporation of a second imidazolium to the benzene connector, forming a bidentate dicationic receptor, greatly enhances the binding. Addition of electron-withdrawing F atoms to each imidazolium adds a further increment. F- consistently binds more strongly to the various receptor models than does Cl-. Whereas replacement of the H atom on the imidazolium groups with the halogen-bonding I has an inconsistent perturbing effect, tetrel-bonding SnH3 significantly enhances the binding with either halide, and SiF3 even more so. Placement of the various complexes into aqueous solution reduces binding energies, but the trends that occur in the gas phase are largely reproduced in water. The tetrel-bonding receptors are the most selective for F- over Cl-, with an equilibrium ratio on the order of 1014 for SnH3 and1028 for SiF3. When combined with their strong halide binding, SiF3-ImF3-Bz-ImF3-SiF3+2 bipodal receptors represent an optimal choice in terms of both binding strength and selectivity.

Comments

This document is the Accepted Manuscript version of a Published Work that appeared in final form in The Journal of Physical Chemistry A, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acs.jpca.7b02305.

Included in

Chemistry Commons

Share

COinS
 
 

To view the content in your browser, please download Adobe Reader or, alternately,
you may Download the file to your hard drive.

NOTE: The latest versions of Adobe Reader do not support viewing PDF files within Firefox on Mac OS and if you are using a modern (Intel) Mac, there is no official plugin for viewing PDF files within the browser window.