The electrochemical polymerisation of 1,2 dihydroxybenzene (catechol) and 2-hydroxybenzyl alcohol (2HBA) from aqueous neutral, acidic and basic solutions was investigated. The development of polymer films on gold working electrodes was observed by the rapid decrease in current seen in the cyclic voltammograms (CV). The currents pertaining to the oxidation and polymerisation of catechol are far higher (by some two orders of magnitude) than for the 2HBA in all tested media. The presence of polymer films was confirmed by the decrease in current in the CV scans subsequent to the first. Molecular structures, electron density distribution and the eigenvalues of the Highest Occupied Molecular Orbital (HOMO) and the Lowest Unoccupied Molecular Orbital (LUMO) of each compound and their ionised forms were calculated using Spartan 14 V1.1.4 molecular modelling suite package. All values have been carried out by restricted Hartree-Fock (RHF) level using 6-311G* basis set. The calculated energy levels were used to evaluate the electrochemical event. (C) 2014 Elsevier Ltd. All rights reserved.