Spin labeling ESR investigation of the molecular environment of soil interacting with chemical organic contaminants

摘要

This manuscript elucidates the influence of special functional groups of organic xenobiotic chemicals on partly simultaneous molecular binding mechanisms. organic xenobiotics are released as contaminants into the environment and are partially bound to soil constituents, such as humic substances (HS) and the mineral phase. The interaction of chemical contaminants with HS of soil was investigated using a labeling technique of soil samples with stable nitroxide radicals as model contaminants. These nitroxide radicals only differed in one functionality, a hydroxy or an amino functional group. Electron spin resonance (ESR) analyses of contaminated soil samples showed that the interaction was a multistage process that comprised an initial increase in the concentration of free organic radicals of soil influenced by contaminants with hydroxy or amino functionality, a decrease in the polarity of the molecular environment of soil, and a change in mobility of contaminant molecules. Towards the end of interaction, the concentration of free organic radicals usually decreased. Binding of contaminants to soil constituents via specific functionality was revealed detecting a change in their ESR spectra. Basing on the ESR analyses, a two-way exchange of protons' electron pairs between contaminants and HS was hypothesized to interpret the beginning of interaction.