A quantum chemical study of the effect of substituents in governing the strength of the S–F bonds of sulfenyl-type fluorides toward homolytic dissociation and fluorine atom transfer

Title
A quantum chemical study of the effect of substituents in governing the strength of the S–F bonds of sulfenyl-type fluorides toward homolytic dissociation and fluorine atom transfer
Publication Date
2019
Author(s)
O'Reilly, Robert
( author )
OrcID: https://orcid.org/0000-0002-5000-1920
Email: roreill6@une.edu.au
UNE Id une-id:roreill6
Balanay, Mannix P
Type of document
Journal Article
Language
en
Entity Type
Publication
Publisher
Elsevier BV
Place of publication
The Netherlands
DOI
10.1016/j.cdc.2019.100186
UNE publication id
une:1959.11/58182
Abstract

The gas-phase homolytic S–F bond dissociation energies (BDEs) of 21 sulfenyl-type fluorides (RSF) have been obtained using the W1w thermochemical protocol. The BDEs (at 298K) for the species in this set range from 316.2 (HCCSF) to 368.1 (H2CCHSF) kJ mol–1. We additionally report fluorine-transfer energies (FTEs), corresponding to the energetics of fluorine transfer from RSF to H2S. At 298K, the FTEs range from –10.7 (H2AlSF) to 90.7 (MeHNSF) kJ mol–1. We have also assessed the performance of a wide range of density functional theory (DFT) and double-hybrid DFT methods (in conjunction with the A'VQZ basis set) for the calculation of these quantities. For the calculation of S–F BDEs, the M06-2X procedure offers the best performance, with a mean absolute deviation (MAD) of 1.6kJ mol–1, whilst for the FTEs, B2K-PLYP and DSD-PBEP86 offer the best performance with MADs of 0.5kJ mol–1.

Link
Citation
Chemical Data Collections, v.20
ISSN
2405-8300

Files:

NameSizeformatDescriptionLink