Enhanced hydrodechlorination of 4-chlorophenol through carboxymethylcellulose-modified Pd/Fe nanosuspension synthesized by one-step methods

Chemosphere. 2024 May:356:141857. doi: 10.1016/j.chemosphere.2024.141857. Epub 2024 Apr 1.

Abstract

Palladized iron (Pd/Fe) represents one of the most common modification strategies for nanoscale zero-valent iron (nZVI). Most studies prepared Pd/Fe by reducing iron salts and depositing Pd species on the surface of pre-synthesized nZVI, which can be called the two-step method. In this study, we proposed a one-step method to obtain Pd/Fe by the concurrent formation of Fe0 and Pd0 and investigated the effects of these two methods on 4-chlorophenol (4-CP) removal, with carboxymethylcellulose (CMC) coated as a surface modifier. Results indicated that the one-step method, not only streamlined the synthesis process, but also Pd/Fe-CMCone-step, synthesized by it, exhibited a higher 4-CP removal rate (97.9%) compared to the two-step method material Pd/Fe-CMCtwo-step (82.4%). Electrochemical analyses revealed that the enhanced activity of Pd/Fe-CMCone-step was attributed to its higher electron transfer efficiency and more available reactive species, active adsorbed hydrogen species (Hads*). Detection of intermediate products demonstrated that, under the influence of Pd/Fe-CMCone-step, the main route of 4-CP was through hydrodechlorination (HDC) to form phenol and H* was the main active specie, supported by EPR tests, quenching experiments and product analysis. Additionally, the effects of initial 4-CP concentration, initial pH, O2 concentration, anions such as Cl-, SO42-, HCO3-, and humic acid (HA) were also investigated. In conclusion, the results of this study suggest that Pd/Fe-CMCone-step, synthesized through the one-step method, is a convenient and efficient nZVI-modifying material suitable for the HDC of chlorinated organic compounds.

Keywords: Catalytic mechanism; Hydrodechlorination; Palladium; Synthetic methods; Zero-valent iron.

MeSH terms

  • Adsorption
  • Carboxymethylcellulose Sodium* / chemistry
  • Chlorophenols* / chemistry
  • Halogenation
  • Iron* / chemistry
  • Metal Nanoparticles / chemistry
  • Palladium* / chemistry
  • Suspensions
  • Water Pollutants, Chemical / chemistry

Substances

  • Chlorophenols
  • Carboxymethylcellulose Sodium
  • Iron
  • 4-chlorophenol
  • Palladium
  • Water Pollutants, Chemical
  • Suspensions