Abstract

To clarify the evolution mechanism of environmentally-persistent free radicals (EPFRs) in biochar as a function of pyrolysis temperature, three-component pyrolytic carbon was characterized by electron paramagnetic resonance (EPR) spectroscopy. Four types of EPFRs were distinguished by using the peak splitting method. The EPFRs in three-component pyrolytic carbon obtained at a pyrolysis temperature of 300 °C were mainly oxygen-containing free radicals (57.31–83.63 %). Upon increasing the pyrolysis temperature, simple aromatic ring radicals were formed by the dehydrogenation of biomass, and then the polymeric aromatic radicals formed, accompanied by π-electron delocalization to form phenyl-π radicals. Biomass pyrolysis was simulated by mechanically mixing the three components in different proportions. A comparison of the experimental and theoretical values indicated that interactions between the three components did not obviously affect the EPFR concentration in the range of 450–550 °C, with a maximum relative error of 12.78 %. A prediction model for the EPFRs concentration in multi-component pyrolytic carbon was proposed. This study also clarified the generation and transformation mechanisms of EPFRs in three-component pyrolytic carbon, thus providing guidance for generating and regulating biochar EPFRs.

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