Highly active iron-containing silicotungstate catalyst for heterogeneous Fenton oxidation of 4-chlorophenol

• An iron-containing silicotungstate was synthesized as the Fenton-like catalyst.
• Fenton oxidation of 4-chlorophenol was studied both in dark and irradiated systems.
• The catalyst shows superior activity ranging from acidic to neutral pHs.
• The degradation of 4-chlorophenol was greatly enhanced under irradiation.
• We proposed a catalytic mechanism based on synergy of iron and heteropolyanion.

Polyoxometalates (POMs) have been a class of attractive redox catalysts and photocatalysts, but so far, there have been few reports on application of POMs in Fenton (or Fenton-like) oxidation processes. In this context, an iron-containing silicotungstate (FeIIIAspSiW) was synthesized using ferric chloride (FeCl3, FeIII), aspartic acid (C4H7NO4, Asp) and silicotungstic acid (H4SiW12O40·xH2O, SiW) as raw materials and employed as a heterogeneous catalyst for Fenton oxidizing 4-chlorophenol (4-CP). The chemical formula of FeIIIAspSiW is speculated as [Fe(C4H5NO4)]3.5H0.5SiW12O40·14H2O with Keggin-structured SiW12O404− anion. The FeIIIAspSiW catalyst showed high activity for oxidation of 4-CP by H2O2 ranging from acidic to circumneutral pHs under both the dark and irradiated conditions. Besides, the catalyst also exhibited good regenerability without significant performance drop. The catalytic mechanism in non-irradiated system was related to the Fenton-like catalysis of ferric iron in FeIIIAspSiW. Moreover, the enhanced degradation of 4-CP under irradiation was attributed to the synergistic effect of Fenton-like catalysis of ferric iron and photocatalysis of SiW12O404− anions in FeIIIAspSiW.

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