How changes in interfacial pH lead to new voltammetric features: the case of the electrochemical oxidation of hydrazine

Phys Chem Chem Phys. 2018 May 3;20(17):11787-11793. doi: 10.1039/c8cp01835a.

Abstract

The electrochemical oxidation of hydrazine was investigated in strongly and weakly pH buffered solutions to reveal the role of buffer capacity in proton-electron transfer redox reactions. In sufficiently buffered solutions, a single voltammetric feature was observed. However, increasing the hydrazine concentration (or, equivalently, moving to an insufficiently buffered solution) gave rise to a second voltammetric feature. These results are rationalised with a conceptually simple model and finite element simulations. We demonstrate that the new voltammetric feature is caused by a large change in the pH at the electrode surface as the reaction proceeds. Importantly, we show that the occurrence of additional voltammetric features are general for proton-electron transfer reactions in insufficiently buffered solutions, and should not be confused with changes in the reaction mechanism.