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Assessment of quantum chemical methods for the calculation of homolytic N–F bond dissociation energies

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Date
2016
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Elsevier BV
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<p>In this article, the performance of a wide range of conventional and double-hybrid DFT methods (in conjunction with Dunning basis sets of double-, triple- and quadruple-zeta quality), as well as a number of Gaussian-n thermochemical protocols are assessed for their ability to compute accurate homolytic N–F bond dissociation energies (BDEs). Their performance is evaluated against a previously reported set of 31 highly accurate gas-phase N–F BDEs obtained using the benchmark-quality W2w thermochemical protocol (See: R.J. O'Reilly, A. Karton, L. Radom, <i>J. Phys. Chem. A</i> <b>2011</b>, 115, 5496.). Out of all of the DFT/basis set combinations investigated, ωB97 and M06-2X (in conjunction with the aug'-cc-pVDZ basis set) offer the lowest mean absolute deviations (MADs =2.4 and 2.7 kJ mol<sup>–1</sup>, respectively). Of the Gaussian-n procedures, G3X offers the best performance (MAD =1.4 kJ mol<sup>–1</sup>), whilst the significantly more economical G3X(MP2)-RAD method also offers excellent performance (MAD =1.8 kJ mol<sup>–1</sup>).</p>
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Chemical Data Collections, v.5-6, p. 28-35