In situ synthesis of Fe-N co-doped carbonaceous nanocomposites using biogas residue as an effective persulfate activator for remediation of aged petroleum contaminated soils

Abstract

Persulfate (PS)-based chemical oxidation is an effective method for the remediation of petroleum-contaminated soils, but higher concentrations of PS (3–40%) may lead to soil acidification (pH decreased by 1.8–6.2 units) and affect the microbial communities. In this study, Fe/N co-doped carbonaceous nanocomposites (Fe-N @ CN) that can efficiently activate PS were developed from biogas residue for the remediation of petroleum-contaminated soil. The as-obtained Fe-N@CN displayed that the Fe-based nanoparticles were encapsulated in graphitic nanosheets, with Fe3C and FeN0.0760 as the main bonding modes. The removal efficiency of total petroleum hydrocarbons (TPHs) reached 73.14% in 3 days with a PS dose of 2% and catalyst dose of 0.4%, and increased by 15.8% on adding 30 mmol/kg of β-cyclodextrin. The free-radical quenching experiment and electron paramagnetic resonance revealed that SO4·-,·OH, O2·-, and 1O2 were involved in the removal of TPHs. Because of the low PS dosage, the remediation process had no significant effect on the soil pH. During the remediation process, soil catalase activity was enhanced and then recovered, whereas the soil bacterial community, reflected by the operational taxonomic unit values, decreased and then recovered. TPH-degrading bacteria were produced in the Fe-N@CN/PS/soil system after chemical oxidation, further contributing to soil remediation.