Biochar-goethite composites inhibited/enhanced degradation of triphenyl phosphate by activating persulfate: Insights on the mechanism

Sci Total Environ. 2023 Feb 1;858(Pt 2):159940. doi: 10.1016/j.scitotenv.2022.159940. Epub 2022 Nov 3.

Abstract

In this study, the biochar-goethite composites (MBC@FH) were synthesized through co-ball milling and the degradation of triphenyl phosphate (TPhP) was compared in persulfate (PDS) alone system and MBC@FH&PDS systems. The results showed that TPhP can be effectively degraded in PDS alone system and degradation efficiency reached up to 90 % within reaction of 8 h, at a PDS concentration of 10 mM, a reaction temperature of 30 °C and a system pH of 6.12. The obvious degradation can be ascribed to the reactive oxygen species (ROS) generated by self-decompose of PDS, among which 1O2, ∙OH and O2- play a major role in the degradation process. Although 350 °C biochar-goethite composites (MBC35@FH) and 800 °C biochar-goethite composites (MBC80@FH) facilitated PDS activation to produce more ROS, the catalytic degradation of TPhP was different in their systems. The degradation of TPhP was inhibited by MBC35@FH due to its stronger adsorption for TPhP, while MBC80@FH promoted TPhP degradation and degradation efficiency was up to 100 % within 6 h. 1O2 and SO4- played a stronger degradation role than ∙OH and O2- in above systems. The transformation of Fe species, functional groups (oxygen-containing functional groups, pyrrolic nitrogen) and persistent free radicals (PFRs) on the MBC@FH were involved in the PDS activation to produce ROS. Furthermore, MBC80@FH was more capable of activating PDS than MBC35@FH due to its abundant defect sites, larger specific surface area, more PFRs, higher Fe content and stronger electron transfer capability. In addition, seven possible TPhP intermediates were identified and possible degradation pathways of TPhP were proposed accordingly. This study illustrated that not all metallic carbon catalysts are necessarily beneficial for organic contaminants degradation.

Keywords: Activating mechanism; Catalytic degradation; MBC@FH; Organophosphates; Reactive oxygen species.

MeSH terms

  • Charcoal* / chemistry
  • Free Radicals / chemistry
  • Reactive Oxygen Species

Substances

  • biochar
  • triphenyl phosphate
  • goethite
  • Reactive Oxygen Species
  • Charcoal
  • Free Radicals