Enzymatic post-treatment of ozonation: laccase-mediated removal of the by-products of acetaminophen ozonation
Ozonation is a powerful technique to remove micropollutants from wastewater. As chemical oxidation of wastewater comes with the formation of varying, possibly persistent and toxic by-products, post-treatment of the ozonated effluent is routinely suggested. This study explored an enzymatic treatment...
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| Veröffentlicht in: | Environmental science and pollution research international 2023-04, Vol.30 (18), p.53128-53139 |
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| creator | Schmiemann, Dorothee Hohenschon, Lisa Bartels, Indra Hermsen, Andrea Bachmann, Felix Cordes, Arno Jäger, Martin Gutmann, Jochen Stefan Hoffmann-Jacobsen, Kerstin |
| description | Ozonation is a powerful technique to remove micropollutants from wastewater. As chemical oxidation of wastewater comes with the formation of varying, possibly persistent and toxic by-products, post-treatment of the ozonated effluent is routinely suggested. This study explored an enzymatic treatment of ozonation products using the laccase from
Trametes versicolor
. A high-performance liquid chromatography coupled with high-resolution mass spectrometry (HPLC-HRMS) analysis revealed that the major by-products were effectively degraded by the enzymatic post-treatment. The enzymatic removal of the by-products reduced the ecotoxicity of the ozonation effluent, as monitored by the inhibition of
Aliivibrio fischeri.
The ecotoxicity was more effectively reduced by enzymatic post-oxidation at pH 7 than at the activity maximum of the laccase at pH 5. A mechanistic HPLC-HRMS and UV/Vis spectroscopic analysis revealed that acidic conditions favored rapid conversion of the phenolic by-products to dead-end products in the absence of nucleophiles. In contrast, the polymerization to harmless insoluble polymers was favored at neutral conditions. Hence, coupling ozonation with laccase-catalyzed post-oxidation at neutral conditions, which are present in wastewater effluents, is suggested as a new resource-efficient method to remove persistent micropollutants while excluding the emission of potentially harmful by-products.
Graphical abstract |
| doi_str_mv | 10.1007/s11356-023-25913-w |
| format | Article |
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Trametes versicolor
. A high-performance liquid chromatography coupled with high-resolution mass spectrometry (HPLC-HRMS) analysis revealed that the major by-products were effectively degraded by the enzymatic post-treatment. The enzymatic removal of the by-products reduced the ecotoxicity of the ozonation effluent, as monitored by the inhibition of
Aliivibrio fischeri.
The ecotoxicity was more effectively reduced by enzymatic post-oxidation at pH 7 than at the activity maximum of the laccase at pH 5. A mechanistic HPLC-HRMS and UV/Vis spectroscopic analysis revealed that acidic conditions favored rapid conversion of the phenolic by-products to dead-end products in the absence of nucleophiles. In contrast, the polymerization to harmless insoluble polymers was favored at neutral conditions. Hence, coupling ozonation with laccase-catalyzed post-oxidation at neutral conditions, which are present in wastewater effluents, is suggested as a new resource-efficient method to remove persistent micropollutants while excluding the emission of potentially harmful by-products.
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Trametes versicolor
. A high-performance liquid chromatography coupled with high-resolution mass spectrometry (HPLC-HRMS) analysis revealed that the major by-products were effectively degraded by the enzymatic post-treatment. The enzymatic removal of the by-products reduced the ecotoxicity of the ozonation effluent, as monitored by the inhibition of
Aliivibrio fischeri.
The ecotoxicity was more effectively reduced by enzymatic post-oxidation at pH 7 than at the activity maximum of the laccase at pH 5. A mechanistic HPLC-HRMS and UV/Vis spectroscopic analysis revealed that acidic conditions favored rapid conversion of the phenolic by-products to dead-end products in the absence of nucleophiles. In contrast, the polymerization to harmless insoluble polymers was favored at neutral conditions. Hence, coupling ozonation with laccase-catalyzed post-oxidation at neutral conditions, which are present in wastewater effluents, is suggested as a new resource-efficient method to remove persistent micropollutants while excluding the emission of potentially harmful by-products.
Graphical abstract</description><subject>Acetaminophen</subject><subject>Aquatic Pollution</subject><subject>Atmospheric Protection/Air Quality Control/Air Pollution</subject><subject>By products</subject><subject>Byproducts</subject><subject>Coriolus versicolor</subject><subject>Earth and Environmental Science</subject><subject>Ecotoxicology</subject><subject>Effluents</subject><subject>Environment</subject><subject>Environmental Chemistry</subject><subject>Environmental Health</subject><subject>Environmental science</subject><subject>enzymatic treatment</subject><subject>High performance liquid chromatography</subject><subject>Laccase</subject><subject>Lewis bases</subject><subject>Liquid chromatography</subject><subject>Mass spectrometry</subject><subject>Mass spectroscopy</subject><subject>Micropollutants</subject><subject>Nucleophiles</subject><subject>Oxidation</subject><subject>Ozonation</subject><subject>Ozone - chemistry</subject><subject>Phenolic compounds</subject><subject>Phenols</subject><subject>pollutants</subject><subject>polymerization</subject><subject>Polymers</subject><subject>Research Article</subject><subject>spectral analysis</subject><subject>toxicity</subject><subject>Trametes</subject><subject>Vibrio fischeri</subject><subject>Waste Disposal, Fluid - methods</subject><subject>Waste Water Technology</subject><subject>Wastewater</subject><subject>Wastewater oxidation</subject><subject>Wastewater treatment</subject><subject>Water Management</subject><subject>Water Pollutants, Chemical - analysis</subject><subject>Water Pollution Control</subject><subject>Water Purification - methods</subject><issn>1614-7499</issn><issn>0944-1344</issn><issn>1614-7499</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2023</creationdate><recordtype>article</recordtype><sourceid>C6C</sourceid><sourceid>EIF</sourceid><sourceid>BENPR</sourceid><recordid>eNqFkUtv1TAQhSNERUvhD7BAkdiwcfEjfrFBVVUoUqVuytpyfMe9qRI72E6r21-PL7cvWMDKls83xzNzmuYdwUcEY_kpE8K4QJgyRLkmDN2-aA6IIB2SndYvn933m9c5X2NMsabyVbPPhOKMM3nQTKfhbjPZMrh2jrmgksCWCUJpo2_jXQxViuFzO1rnbAY0wWqwBVZtgine2HGLlTW0_QbNKa4WV_L2yToodhpCnNcQnnzeNHvejhne3p-HzY-vp5cnZ-j84tv3k-Nz5DhWBfkegHQr6ggohbF2ymneU648FsLbOjDDhHay5x6YxL7XnlOiKiM0E9yxw-bLznde-tqxq_MkO5o5DZNNGxPtYP5UwrA2V_HGEEyIphRXh4_3Din-XCAXMw3ZwTjaAHHJhhHOaN0n_j9KpcJSSN2Jin74C72OSwp1FYZWSCsipKwU3VEuxZwT-MfGCTbb5M0ueVMXYX4nb25r0fvnIz-WPERdAbYDcpXCFaSnv_9h-wvBhrt5</recordid><startdate>20230401</startdate><enddate>20230401</enddate><creator>Schmiemann, Dorothee</creator><creator>Hohenschon, Lisa</creator><creator>Bartels, Indra</creator><creator>Hermsen, Andrea</creator><creator>Bachmann, Felix</creator><creator>Cordes, Arno</creator><creator>Jäger, Martin</creator><creator>Gutmann, Jochen Stefan</creator><creator>Hoffmann-Jacobsen, Kerstin</creator><general>Springer Berlin Heidelberg</general><general>Springer Nature B.V</general><scope>C6C</scope><scope>CGR</scope><scope>CUY</scope><scope>CVF</scope><scope>ECM</scope><scope>EIF</scope><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>3V.</scope><scope>7QL</scope><scope>7SN</scope><scope>7T7</scope><scope>7TV</scope><scope>7U7</scope><scope>7WY</scope><scope>7WZ</scope><scope>7X7</scope><scope>7XB</scope><scope>87Z</scope><scope>88E</scope><scope>88I</scope><scope>8AO</scope><scope>8C1</scope><scope>8FD</scope><scope>8FI</scope><scope>8FJ</scope><scope>8FK</scope><scope>8FL</scope><scope>ABUWG</scope><scope>AEUYN</scope><scope>AFKRA</scope><scope>ATCPS</scope><scope>AZQEC</scope><scope>BENPR</scope><scope>BEZIV</scope><scope>BHPHI</scope><scope>C1K</scope><scope>CCPQU</scope><scope>DWQXO</scope><scope>FR3</scope><scope>FRNLG</scope><scope>FYUFA</scope><scope>F~G</scope><scope>GHDGH</scope><scope>GNUQQ</scope><scope>HCIFZ</scope><scope>K60</scope><scope>K6~</scope><scope>K9.</scope><scope>L.-</scope><scope>M0C</scope><scope>M0S</scope><scope>M1P</scope><scope>M2P</scope><scope>M7N</scope><scope>P64</scope><scope>PATMY</scope><scope>PHGZM</scope><scope>PHGZT</scope><scope>PJZUB</scope><scope>PKEHL</scope><scope>PPXIY</scope><scope>PQBIZ</scope><scope>PQBZA</scope><scope>PQEST</scope><scope>PQQKQ</scope><scope>PQUKI</scope><scope>PYCSY</scope><scope>Q9U</scope><scope>7X8</scope><scope>7S9</scope><scope>L.6</scope><scope>5PM</scope><orcidid>https://orcid.org/0000-0002-7526-0953</orcidid></search><sort><creationdate>20230401</creationdate><title>Enzymatic post-treatment of ozonation: laccase-mediated removal of the by-products of acetaminophen ozonation</title><author>Schmiemann, Dorothee ; Hohenschon, Lisa ; Bartels, Indra ; Hermsen, Andrea ; Bachmann, Felix ; Cordes, Arno ; Jäger, Martin ; Gutmann, Jochen Stefan ; Hoffmann-Jacobsen, Kerstin</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c508t-fbee14d2c1e88009c8c95b258f066fa023301247b5fe370fb9f521895b69365c3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2023</creationdate><topic>Acetaminophen</topic><topic>Aquatic Pollution</topic><topic>Atmospheric Protection/Air Quality Control/Air Pollution</topic><topic>By products</topic><topic>Byproducts</topic><topic>Coriolus versicolor</topic><topic>Earth and Environmental Science</topic><topic>Ecotoxicology</topic><topic>Effluents</topic><topic>Environment</topic><topic>Environmental Chemistry</topic><topic>Environmental Health</topic><topic>Environmental science</topic><topic>enzymatic treatment</topic><topic>High performance liquid chromatography</topic><topic>Laccase</topic><topic>Lewis bases</topic><topic>Liquid chromatography</topic><topic>Mass spectrometry</topic><topic>Mass spectroscopy</topic><topic>Micropollutants</topic><topic>Nucleophiles</topic><topic>Oxidation</topic><topic>Ozonation</topic><topic>Ozone - 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Academic</collection><collection>AGRICOLA</collection><collection>AGRICOLA - Academic</collection><collection>PubMed Central (Full Participant titles)</collection><jtitle>Environmental science and pollution research international</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Schmiemann, Dorothee</au><au>Hohenschon, Lisa</au><au>Bartels, Indra</au><au>Hermsen, Andrea</au><au>Bachmann, Felix</au><au>Cordes, Arno</au><au>Jäger, Martin</au><au>Gutmann, Jochen Stefan</au><au>Hoffmann-Jacobsen, Kerstin</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Enzymatic post-treatment of ozonation: laccase-mediated removal of the by-products of acetaminophen ozonation</atitle><jtitle>Environmental science and pollution research international</jtitle><stitle>Environ Sci Pollut Res</stitle><addtitle>Environ Sci Pollut Res Int</addtitle><date>2023-04-01</date><risdate>2023</risdate><volume>30</volume><issue>18</issue><spage>53128</spage><epage>53139</epage><pages>53128-53139</pages><issn>1614-7499</issn><issn>0944-1344</issn><eissn>1614-7499</eissn><abstract>Ozonation is a powerful technique to remove micropollutants from wastewater. As chemical oxidation of wastewater comes with the formation of varying, possibly persistent and toxic by-products, post-treatment of the ozonated effluent is routinely suggested. This study explored an enzymatic treatment of ozonation products using the laccase from
Trametes versicolor
. A high-performance liquid chromatography coupled with high-resolution mass spectrometry (HPLC-HRMS) analysis revealed that the major by-products were effectively degraded by the enzymatic post-treatment. The enzymatic removal of the by-products reduced the ecotoxicity of the ozonation effluent, as monitored by the inhibition of
Aliivibrio fischeri.
The ecotoxicity was more effectively reduced by enzymatic post-oxidation at pH 7 than at the activity maximum of the laccase at pH 5. A mechanistic HPLC-HRMS and UV/Vis spectroscopic analysis revealed that acidic conditions favored rapid conversion of the phenolic by-products to dead-end products in the absence of nucleophiles. In contrast, the polymerization to harmless insoluble polymers was favored at neutral conditions. Hence, coupling ozonation with laccase-catalyzed post-oxidation at neutral conditions, which are present in wastewater effluents, is suggested as a new resource-efficient method to remove persistent micropollutants while excluding the emission of potentially harmful by-products.
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| subjects | Acetaminophen Aquatic Pollution Atmospheric Protection/Air Quality Control/Air Pollution By products Byproducts Coriolus versicolor Earth and Environmental Science Ecotoxicology Effluents Environment Environmental Chemistry Environmental Health Environmental science enzymatic treatment High performance liquid chromatography Laccase Lewis bases Liquid chromatography Mass spectrometry Mass spectroscopy Micropollutants Nucleophiles Oxidation Ozonation Ozone - chemistry Phenolic compounds Phenols pollutants polymerization Polymers Research Article spectral analysis toxicity Trametes Vibrio fischeri Waste Disposal, Fluid - methods Waste Water Technology Wastewater Wastewater oxidation Wastewater treatment Water Management Water Pollutants, Chemical - analysis Water Pollution Control Water Purification - methods |
| title | Enzymatic post-treatment of ozonation: laccase-mediated removal of the by-products of acetaminophen ozonation |
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