<p>This study investigates the removal of diclofenac from water by adsorption onto a dealuminated Y-type zeolite (DAY), followed by destructive regeneration of the spent adsorbent using homogeneous advanced oxidation processes. Two oxidation systems were evaluated: the Fenton reaction (<InlineEquation ID="IEq1"> <EquationSource Format="TEX">\(\text {HO}^{\bullet }\)</EquationSource> <EquationSource Format="MATHML"><math> <msup> <mtext>HO</mtext> <mo>∙</mo> </msup> </math></EquationSource> </InlineEquation>) and thermally activated peroxodisulfate (SO<InlineEquation ID="IEq2"> <EquationSource Format="TEX">\(_{4}^{\bullet -}\)</EquationSource> <EquationSource Format="MATHML"><math> <mmultiscripts> <mrow /> <mrow> <mn>4</mn> </mrow> <mrow> <mo>∙</mo> <mo>-</mo> </mrow> </mmultiscripts> </math></EquationSource> </InlineEquation>). For the Fenton process, two catalysts were tested: ferrous ion (Fe<InlineEquation ID="IEq3"> <EquationSource Format="TEX">\(^{2+}\)</EquationSource> <EquationSource Format="MATHML"><math> <mmultiscripts> <mrow /> <mrow /> <mrow> <mn>2</mn> <mo>+</mo> </mrow> </mmultiscripts> </math></EquationSource> </InlineEquation>) and the Fe(II)–EDDS complex, using ethylenediamine-N,N′-disuccinic acid as a chelating agent. The influence of the oxidation process and of the localization of radical generation on regeneration efficiency was assessed. Regeneration performance was quantified by the adsorption capacity recovery ratio (<InlineEquation ID="IEq4"> <EquationSource Format="TEX">\(q_0/q_{0,1}\)</EquationSource> <EquationSource Format="MATHML"><math> <mrow> <msub> <mi>q</mi> <mn>0</mn> </msub> <mo stretchy="false">/</mo> <msub> <mi>q</mi> <mrow> <mn>0</mn> <mo>,</mo> <mn>1</mn> </mrow> </msub> </mrow> </math></EquationSource> </InlineEquation>) obtained from Langmuir isotherm modelling. The results show that adsorbent regeneration is feasible over several adsorption-regeneration cycles, but that the recovered adsorption capacity decreases with cycle number. For Fenton regeneration with Fe<InlineEquation ID="IEq5"> <EquationSource Format="TEX">\(^{2+}\)</EquationSource> <EquationSource Format="MATHML"><math> <mmultiscripts> <mrow /> <mrow /> <mrow> <mn>2</mn> <mo>+</mo> </mrow> </mmultiscripts> </math></EquationSource> </InlineEquation>, the adsorption capacity recovery was 71.9% after the second cycle and decreased to 19.8% after the third. In contrast, thermally activated peroxodisulfate yielded higher regeneration efficiencies, with 91.1% and 50.5% recovery after the second and third cycles, respectively, which is attributed to the greater persistence of SO<InlineEquation ID="IEq6"> <EquationSource Format="TEX">\(_{4}^{\bullet -}\)</EquationSource> <EquationSource Format="MATHML"><math> <mmultiscripts> <mrow /> <mrow> <mn>4</mn> </mrow> <mrow> <mo>∙</mo> <mo>-</mo> </mrow> </mmultiscripts> </math></EquationSource> </InlineEquation> and its ability to oxidize adsorbed diclofenac within the zeolite pores. When the Fe(II)–EDDS complex was used at pH 3, the regeneration rates increased to 75.2% (second cycle) and 39.1% (third cycle), and at pH 7, the Fe(II)–EDDS complex further improved adsorption capacity recovery. Overall, immobilizing the Fe(II)–EDDS catalyst on the zeolite surface enhances regeneration efficiency for DAY.</p>

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Regeneration of dealuminated zeolite Y for diclofenac adsorption using Fenton and peroxodisulfate advanced oxidation processes

  • Lionel Domergue

摘要

This study investigates the removal of diclofenac from water by adsorption onto a dealuminated Y-type zeolite (DAY), followed by destructive regeneration of the spent adsorbent using homogeneous advanced oxidation processes. Two oxidation systems were evaluated: the Fenton reaction ( \(\text {HO}^{\bullet }\) HO ) and thermally activated peroxodisulfate (SO \(_{4}^{\bullet -}\) 4 - ). For the Fenton process, two catalysts were tested: ferrous ion (Fe \(^{2+}\) 2 + ) and the Fe(II)–EDDS complex, using ethylenediamine-N,N′-disuccinic acid as a chelating agent. The influence of the oxidation process and of the localization of radical generation on regeneration efficiency was assessed. Regeneration performance was quantified by the adsorption capacity recovery ratio ( \(q_0/q_{0,1}\) q 0 / q 0 , 1 ) obtained from Langmuir isotherm modelling. The results show that adsorbent regeneration is feasible over several adsorption-regeneration cycles, but that the recovered adsorption capacity decreases with cycle number. For Fenton regeneration with Fe \(^{2+}\) 2 + , the adsorption capacity recovery was 71.9% after the second cycle and decreased to 19.8% after the third. In contrast, thermally activated peroxodisulfate yielded higher regeneration efficiencies, with 91.1% and 50.5% recovery after the second and third cycles, respectively, which is attributed to the greater persistence of SO \(_{4}^{\bullet -}\) 4 - and its ability to oxidize adsorbed diclofenac within the zeolite pores. When the Fe(II)–EDDS complex was used at pH 3, the regeneration rates increased to 75.2% (second cycle) and 39.1% (third cycle), and at pH 7, the Fe(II)–EDDS complex further improved adsorption capacity recovery. Overall, immobilizing the Fe(II)–EDDS catalyst on the zeolite surface enhances regeneration efficiency for DAY.