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 |
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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. |
doi_str_mv | 10.1016/j.jhazmat.2022.129966 |
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fullrecord | <record><control><sourceid>proquest_cross</sourceid><recordid>TN_cdi_proquest_miscellaneous_2718637590</recordid><sourceformat>XML</sourceformat><sourcesystem>PC</sourcesystem><els_id>S0304389422017605</els_id><sourcerecordid>2718637590</sourcerecordid><originalsourceid>FETCH-LOGICAL-c389t-30029e532d44c5eee9f523adf106c4b07ce37650a35d71bef0cf559b27838e1e3</originalsourceid><addsrcrecordid>eNqFkctKBDEQRYMoOD4-QeilC3vMo9OPlYj4ggE3ug7ppIIZujtjkp5x_Ay_2IytuHRVRVXdQ10uQmcEzwkm5eVyvnyVH72Mc4opnRPaNGW5h2akrljOGCv30QwzXOSsbopDdBTCEmNMKl7M0OfCbfII_Qq8jKOHLDVh7IyMkEkV7VpG64as3WYrt9HgQf-OU6ekb9PSOJ8F249dlAO4MWQaQvSj-lY6s0OabnTeDn-q921nVUJZHTI56IxcFLm27j0RTtCBkV2A0596jF7ubp9vHvLF0_3jzfUiV8lHzBnGtAHOqC4KxQGgMZwyqQ3BpSpaXClgVcmxZFxXpAWDleG8aWlVsxoIsGN0PnFX3r2N6WXR26Cg6yYXglakLlnFG5xO-XSqvAvBgxErb3vpt4JgsctALMVPBmKXgZgySLqrSQfJx9qCF0FZGBRo60FFoZ39h_AFJOyW0g</addsrcrecordid><sourcetype>Aggregation Database</sourcetype><iscdi>true</iscdi><recordtype>article</recordtype><pqid>2718637590</pqid></control><display><type>article</type><title>Low-temperature persulfate activation by powdered activated carbon for simultaneous destruction of perfluorinated carboxylic acids and 1,4-dioxane</title><source>Elsevier ScienceDirect Journals</source><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.</creator><creatorcontrib>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.</creatorcontrib><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.</description><identifier>ISSN: 0304-3894</identifier><identifier>EISSN: 1873-3336</identifier><identifier>DOI: 10.1016/j.jhazmat.2022.129966</identifier><language>eng</language><publisher>Elsevier B.V</publisher><subject>4-dioxane ; DMPO radical adducts ; In-situ chemical oxidation (ISCO) ; Perfluorooctanoic acid (PFOA) ; Persulfate ; Powdered activated carbon (PAC) ; Spin trapping</subject><ispartof>Journal of hazardous materials, 2023-01, Vol.442, p.129966-129966, Article 129966</ispartof><rights>2022 Elsevier B.V.</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c389t-30029e532d44c5eee9f523adf106c4b07ce37650a35d71bef0cf559b27838e1e3</citedby><cites>FETCH-LOGICAL-c389t-30029e532d44c5eee9f523adf106c4b07ce37650a35d71bef0cf559b27838e1e3</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktohtml>$$Uhttps://www.sciencedirect.com/science/article/pii/S0304389422017605$$EHTML$$P50$$Gelsevier$$H</linktohtml><link.rule.ids>314,776,780,3537,27901,27902,65306</link.rule.ids></links><search><creatorcontrib>Manz, Katherine E.</creatorcontrib><creatorcontrib>Kulaots, Indrek</creatorcontrib><creatorcontrib>Greenley, Caroline A.</creatorcontrib><creatorcontrib>Landry, Patrick J.</creatorcontrib><creatorcontrib>Lakshmi, K.V.</creatorcontrib><creatorcontrib>Woodcock, Matthew J.</creatorcontrib><creatorcontrib>Hellerich, Lucas</creatorcontrib><creatorcontrib>Bryant, J. 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 (>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.</description><subject>4-dioxane</subject><subject>DMPO radical adducts</subject><subject>In-situ chemical oxidation (ISCO)</subject><subject>Perfluorooctanoic acid (PFOA)</subject><subject>Persulfate</subject><subject>Powdered activated carbon (PAC)</subject><subject>Spin trapping</subject><issn>0304-3894</issn><issn>1873-3336</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2023</creationdate><recordtype>article</recordtype><recordid>eNqFkctKBDEQRYMoOD4-QeilC3vMo9OPlYj4ggE3ug7ppIIZujtjkp5x_Ay_2IytuHRVRVXdQ10uQmcEzwkm5eVyvnyVH72Mc4opnRPaNGW5h2akrljOGCv30QwzXOSsbopDdBTCEmNMKl7M0OfCbfII_Qq8jKOHLDVh7IyMkEkV7VpG64as3WYrt9HgQf-OU6ekb9PSOJ8F249dlAO4MWQaQvSj-lY6s0OabnTeDn-q921nVUJZHTI56IxcFLm27j0RTtCBkV2A0596jF7ubp9vHvLF0_3jzfUiV8lHzBnGtAHOqC4KxQGgMZwyqQ3BpSpaXClgVcmxZFxXpAWDleG8aWlVsxoIsGN0PnFX3r2N6WXR26Cg6yYXglakLlnFG5xO-XSqvAvBgxErb3vpt4JgsctALMVPBmKXgZgySLqrSQfJx9qCF0FZGBRo60FFoZ39h_AFJOyW0g</recordid><startdate>20230115</startdate><enddate>20230115</enddate><creator>Manz, Katherine E.</creator><creator>Kulaots, Indrek</creator><creator>Greenley, Caroline A.</creator><creator>Landry, Patrick J.</creator><creator>Lakshmi, K.V.</creator><creator>Woodcock, Matthew J.</creator><creator>Hellerich, Lucas</creator><creator>Bryant, J. Daniel</creator><creator>Apfelbaum, Mike</creator><creator>Pennell, Kurt D.</creator><general>Elsevier B.V</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7X8</scope></search><sort><creationdate>20230115</creationdate><title>Low-temperature persulfate activation by powdered activated carbon for simultaneous destruction of perfluorinated carboxylic acids and 1,4-dioxane</title><author>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.</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c389t-30029e532d44c5eee9f523adf106c4b07ce37650a35d71bef0cf559b27838e1e3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2023</creationdate><topic>4-dioxane</topic><topic>DMPO radical adducts</topic><topic>In-situ chemical oxidation (ISCO)</topic><topic>Perfluorooctanoic acid (PFOA)</topic><topic>Persulfate</topic><topic>Powdered activated carbon (PAC)</topic><topic>Spin trapping</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Manz, Katherine E.</creatorcontrib><creatorcontrib>Kulaots, Indrek</creatorcontrib><creatorcontrib>Greenley, Caroline A.</creatorcontrib><creatorcontrib>Landry, Patrick J.</creatorcontrib><creatorcontrib>Lakshmi, K.V.</creatorcontrib><creatorcontrib>Woodcock, Matthew J.</creatorcontrib><creatorcontrib>Hellerich, Lucas</creatorcontrib><creatorcontrib>Bryant, J. Daniel</creatorcontrib><creatorcontrib>Apfelbaum, Mike</creatorcontrib><creatorcontrib>Pennell, Kurt D.</creatorcontrib><collection>CrossRef</collection><collection>MEDLINE - Academic</collection><jtitle>Journal of hazardous materials</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Manz, Katherine E.</au><au>Kulaots, Indrek</au><au>Greenley, Caroline A.</au><au>Landry, Patrick J.</au><au>Lakshmi, K.V.</au><au>Woodcock, Matthew J.</au><au>Hellerich, Lucas</au><au>Bryant, J. 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 (>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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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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