The dataset contains all computational results, including validation of the level of theory, molecular structures, and analysis spreadsheets that are in support of our experimental observations of spontaneous reactivity of anthralin/dithranol molecule with molecular oxygen without any catalyst or co-substrate.

The publication is current under review at Journal of Organic Chemistry.

****Free volume correction:
We employed a correction to translational entropy as suggested by Whitesides et al. in their paper entitled "Estimating the Entropic Cost of Self-Assembly of Multi-particle Hydrogen-Bonded Aggregates", JOC 1998, 64, 3821-3830.
In addition to the worked out example in the publication (for chloroform) we provided parameters for all the considered solvents and beyond.

****Theory validation:
We used the computational work of Korth and Mulder (JOC 2013, 78, 7674) for a high level wave function reference calculations, in order to validate the various level of density functional for carrying out the large scale computational mapping of tautomerism in anthralin/dithranol. All computational results and the detailed analysis are provided in the archive.
In addition to the relative stability of the gas phase structures, a brief inquiry was completed for critically assessing the various polarizable continuum model.

Remarkably, the most accurate functional and the most adequate polarizable continuum model were found to come from the same theoretical and computational chemistry school at University of Minneapolis (Truhlar/Cramer).

****Molecular structures
We provide the atomic positional coordinates of all the tautomers in their equilibrium structures along with their ground state energies (list of energies.txt file) that are mentioned in the manuscript or the JOC supporting information.