Low-temperature persulfate activation by powdered activated carbon for simultaneous destruction of perfluorinated carboxylic acids and 1,4-dioxane

Carbonaceous materials have emerged as a method of persulfate activation for remediation. In this study, persulfate activation using powdered activated carbon (PAC) was demonstrated at temperatures relevant to groundwater (5–25 °C). At room temperature, increasing doses of PAC (1–20 g L-1) led to in...

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Veröffentlicht in:Journal of hazardous materials 2023-01, Vol.442, p.129966-129966, Article 129966
Hauptverfasser: Manz, Katherine E., Kulaots, Indrek, Greenley, Caroline A., Landry, Patrick J., Lakshmi, K.V., Woodcock, Matthew J., Hellerich, Lucas, Bryant, J. Daniel, Apfelbaum, Mike, Pennell, Kurt D.
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container_issue
container_start_page 129966
container_title Journal of hazardous materials
container_volume 442
creator Manz, Katherine E.
Kulaots, Indrek
Greenley, Caroline A.
Landry, Patrick J.
Lakshmi, K.V.
Woodcock, Matthew J.
Hellerich, Lucas
Bryant, J. Daniel
Apfelbaum, Mike
Pennell, Kurt D.
description Carbonaceous materials have emerged as a method of persulfate activation for remediation. In this study, persulfate activation using powdered activated carbon (PAC) was demonstrated at temperatures relevant to groundwater (5–25 °C). At room temperature, increasing doses of PAC (1–20 g L-1) led to increased persulfate activation (3.06 × 10-6s-1 to 2.10 × 10-4 with 1 and 20 g L-1 PAC). Activation slowed at lower temperatures (5 and 11 °C); however, substantial (>70 %) persulfate activation was achieved. PAC characterization showed that persulfate is activated at the surface of the PAC, as indicated by an increase in the PAC C:O ratio. Similarly, electron paramagnetic resonance (EPR) spectroscopy studies with a spin trapping agents (5,5-dimethyl-1-pyrroline N-oxide (DMPO)) and 2,2,6,6-tetramethylpiperidine (TEMP) revealed that singlet oxygen was not the main oxidizing species in the reaction. DMPO was oxidized to form 5,5-dimethylpyrrolidone-2(2)-oxyl-(1) (DMPOX), which forms in the presence of strong oxidizers, such as sulfate radicals. The persulfate/PAC system is demonstrated to simultaneously degrade both perfluorooctanoic acid (PFOA) and 1,4-dioxane at room temperature and 11 °C. With a 20 g L-1 PAC and 75 mM persulfate, 80 % and 70 % of the PFOA and 1,4-dioxane, respectively, degraded within 6 h at room temperature. At 11 °C, the same PAC and persulfate doses led to 57% dioxane degradation and 54 % PFOA degradation within 6 h. Coupling PAC with persulfate offers an effective, low-cost treatment for simultaneous destruction of 1,4-dioxane and PFOA. [Display omitted] •Persulfate is activated by powder activated carbon (PAC) at temperatures less than 25 °C.•Co-contaminants 1,4-dioxane and perfluorooctanoic acid are degraded at relevant temperatures.•Targeted and non-targeted mass spectrometry are used to establish PFOA degradation mechanism.
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Similarly, electron paramagnetic resonance (EPR) spectroscopy studies with a spin trapping agents (5,5-dimethyl-1-pyrroline N-oxide (DMPO)) and 2,2,6,6-tetramethylpiperidine (TEMP) revealed that singlet oxygen was not the main oxidizing species in the reaction. DMPO was oxidized to form 5,5-dimethylpyrrolidone-2(2)-oxyl-(1) (DMPOX), which forms in the presence of strong oxidizers, such as sulfate radicals. The persulfate/PAC system is demonstrated to simultaneously degrade both perfluorooctanoic acid (PFOA) and 1,4-dioxane at room temperature and 11 °C. With a 20 g L-1 PAC and 75 mM persulfate, 80 % and 70 % of the PFOA and 1,4-dioxane, respectively, degraded within 6 h at room temperature. At 11 °C, the same PAC and persulfate doses led to 57% dioxane degradation and 54 % PFOA degradation within 6 h. Coupling PAC with persulfate offers an effective, low-cost treatment for simultaneous destruction of 1,4-dioxane and PFOA. 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Daniel</creatorcontrib><creatorcontrib>Apfelbaum, Mike</creatorcontrib><creatorcontrib>Pennell, Kurt D.</creatorcontrib><title>Low-temperature persulfate activation by powdered activated carbon for simultaneous destruction of perfluorinated carboxylic acids and 1,4-dioxane</title><title>Journal of hazardous materials</title><description>Carbonaceous materials have emerged as a method of persulfate activation for remediation. In this study, persulfate activation using powdered activated carbon (PAC) was demonstrated at temperatures relevant to groundwater (5–25 °C). At room temperature, increasing doses of PAC (1–20 g L-1) led to increased persulfate activation (3.06 × 10-6s-1 to 2.10 × 10-4 with 1 and 20 g L-1 PAC). Activation slowed at lower temperatures (5 and 11 °C); however, substantial (&gt;70 %) persulfate activation was achieved. PAC characterization showed that persulfate is activated at the surface of the PAC, as indicated by an increase in the PAC C:O ratio. Similarly, electron paramagnetic resonance (EPR) spectroscopy studies with a spin trapping agents (5,5-dimethyl-1-pyrroline N-oxide (DMPO)) and 2,2,6,6-tetramethylpiperidine (TEMP) revealed that singlet oxygen was not the main oxidizing species in the reaction. DMPO was oxidized to form 5,5-dimethylpyrrolidone-2(2)-oxyl-(1) (DMPOX), which forms in the presence of strong oxidizers, such as sulfate radicals. The persulfate/PAC system is demonstrated to simultaneously degrade both perfluorooctanoic acid (PFOA) and 1,4-dioxane at room temperature and 11 °C. With a 20 g L-1 PAC and 75 mM persulfate, 80 % and 70 % of the PFOA and 1,4-dioxane, respectively, degraded within 6 h at room temperature. At 11 °C, the same PAC and persulfate doses led to 57% dioxane degradation and 54 % PFOA degradation within 6 h. Coupling PAC with persulfate offers an effective, low-cost treatment for simultaneous destruction of 1,4-dioxane and PFOA. 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Daniel</au><au>Apfelbaum, Mike</au><au>Pennell, Kurt D.</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Low-temperature persulfate activation by powdered activated carbon for simultaneous destruction of perfluorinated carboxylic acids and 1,4-dioxane</atitle><jtitle>Journal of hazardous materials</jtitle><date>2023-01-15</date><risdate>2023</risdate><volume>442</volume><spage>129966</spage><epage>129966</epage><pages>129966-129966</pages><artnum>129966</artnum><issn>0304-3894</issn><eissn>1873-3336</eissn><abstract>Carbonaceous materials have emerged as a method of persulfate activation for remediation. In this study, persulfate activation using powdered activated carbon (PAC) was demonstrated at temperatures relevant to groundwater (5–25 °C). At room temperature, increasing doses of PAC (1–20 g L-1) led to increased persulfate activation (3.06 × 10-6s-1 to 2.10 × 10-4 with 1 and 20 g L-1 PAC). Activation slowed at lower temperatures (5 and 11 °C); however, substantial (&gt;70 %) persulfate activation was achieved. PAC characterization showed that persulfate is activated at the surface of the PAC, as indicated by an increase in the PAC C:O ratio. Similarly, electron paramagnetic resonance (EPR) spectroscopy studies with a spin trapping agents (5,5-dimethyl-1-pyrroline N-oxide (DMPO)) and 2,2,6,6-tetramethylpiperidine (TEMP) revealed that singlet oxygen was not the main oxidizing species in the reaction. DMPO was oxidized to form 5,5-dimethylpyrrolidone-2(2)-oxyl-(1) (DMPOX), which forms in the presence of strong oxidizers, such as sulfate radicals. The persulfate/PAC system is demonstrated to simultaneously degrade both perfluorooctanoic acid (PFOA) and 1,4-dioxane at room temperature and 11 °C. With a 20 g L-1 PAC and 75 mM persulfate, 80 % and 70 % of the PFOA and 1,4-dioxane, respectively, degraded within 6 h at room temperature. At 11 °C, the same PAC and persulfate doses led to 57% dioxane degradation and 54 % PFOA degradation within 6 h. Coupling PAC with persulfate offers an effective, low-cost treatment for simultaneous destruction of 1,4-dioxane and PFOA. [Display omitted] •Persulfate is activated by powder activated carbon (PAC) at temperatures less than 25 °C.•Co-contaminants 1,4-dioxane and perfluorooctanoic acid are degraded at relevant temperatures.•Targeted and non-targeted mass spectrometry are used to establish PFOA degradation mechanism.</abstract><pub>Elsevier B.V</pub><doi>10.1016/j.jhazmat.2022.129966</doi><tpages>1</tpages><oa>free_for_read</oa></addata></record>
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1873-3336
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source Elsevier ScienceDirect Journals
subjects 4-dioxane
DMPO radical adducts
In-situ chemical oxidation (ISCO)
Perfluorooctanoic acid (PFOA)
Persulfate
Powdered activated carbon (PAC)
Spin trapping
title Low-temperature persulfate activation by powdered activated carbon for simultaneous destruction of perfluorinated carboxylic acids and 1,4-dioxane
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