Journal of the American Chemical Society p. 12544 - 12545 (2020)
Update date:2022-08-17
Topics:
Wise, Catherine F.
Mayer, James M.
The aqueous CG value used to calculate the bond dissociation free energy (BDFE) values reported in the published Communication was incorrect due to a sign error in its derivation. This systematic error does not affect the conclusions of the study, as all of the aqueous BDFE values shift together. The correct aqueous CG,H2O value is 52.8 kcal mol?1, as reported by Connelly, Wiedner, and Appel.1 We thank Drs. Wiedner and Appel for helpful discussions regarding this correction. We report here revised equations, tables, and schemes with BDFE values adjusted for the correct aqueous CG,H2O term. Pages 14971 and 14972. Equation 1 has been modified to report the correct aqueous CG term, and eqs 4 and 5, which give BDFE values for NiII(OH)2 and NiIIIO(OH), have also been adjusted accordingly. The revised equations are shown below: BDFE(X?H) = 23.06E(pH 0) + 52.8 kcal mol?1 (1) = } =} ? ? Ni O(OH)/Ni (OH) E 0.99 0.03 V BDFE 75.6 1.0 kcal mol III II 2 1 (4) = } = } ? ? Ni O /Ni O(OH) E 1.36 0.02 V BDFE 84.2 1.0 kcal mol IV 2 III 1 (5) Revised BDFE values for the PCET substrates discussed in the original text are given in Table 1. Page 14973. The BDFE ranges discussed in the original publication were adjusted in a similar manner. Thermodynamically favorable reactions at NiIIIO(OH) are predicted for substrates with X?H BDFE less than 75 kcal mol?1 (and were observed for substrates with X?H BDFE ranging from 61 to 73 kcal mol?1). Thermodynamically unfavorable reactivity is predicted (and was observed) for substrates with X?H BDFE greater than 76 kcal mol?1. The observed equilibrium reactivity with 2,4,6-tBu3PhOH is consistent with both the substrate and NiII(OH)2 having an O?H BDFE of ?75.5 kcal mol?1. The number line in Scheme 1 has been adjusted to reflect the corrected BDFE values, and the revised scheme is shown below. [Formula presented] Supporting Information. The BDFE values reported in Tables S1 and S5 were also adjusted for the correct aqueous CG value. The corrected tables are provided in the complete, revised Supporting Information file.
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