Document Type

Article

Journal/Book Title

The Journal of Physical Chemistry A

Publication Date

8-7-2015

Publisher

American Chemical Society

Volume

119

Issue

34

First Page

1

Last Page

27

Abstract

The ability of neutral and charged S-compounds to form different sorts of noncovalent bonds is examined by ab initio calculations. Neutrals are represented by CH3SH and fluoro substituted FSCH3; cations are (CH3)3S+, CH3SH2+, and FHSCH3+. Each is paired with N-methylacetamide (NMA) whose O atom serves as common electron donor. Charged species engage in much stronger noncovalent bonds than do the neutral molecules, by as much as an order of magnitude. The strongest noncovalent bond for any system is a O∙∙SF chalcogen bond wherein the O lies directly opposite a S-F covalent bond, amounting to as much as 39 kcal/mol. Second in binding energy is the SH∙∙O H-bond which can be as large as 34 kcal/mol. Somewhat weaker is the O∙∙SC chalcogen bond, followed by the CH∙∙O H-bond and finally the O∙∙C tetrel bond, which has the appearance of a trifurcated H-bond. Any CH group which participates in a CH∙∙O H-bond shifts its NMR signal downfield by an amount which is roughly proportional to the strength of the H-bond. This situation is clearly distinguishable from that in a O∙∙S chalcogen or SH∙∙O H-bond wherein the methyl protons are shifted upfield.

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.5b06831.

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