Assessing the Chemical-Free Oxidation of Trace Organic Chemicals by VUV/UV as an Alternative to Conventional UV/H2O2
Low-pressure mercury lamps with high-purity quartz can emit both vacuum-UV (VUV, 185 nm) and UV (254 nm) and are commercially available and promising for eliminating recalcitrant organic pollutants. The feasibility of VUV/UV as a chemical-free oxidation process was verified and quantitatively assess...
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creator | Wang, Wen-Long Jing, Zi-Bo Zhang, Yi-Lin Wu, Qian-Yuan Drewes, Jörg E. Lee, Min-Yong Hübner, Uwe |
description | Low-pressure mercury lamps with high-purity quartz can emit both vacuum-UV (VUV, 185 nm) and UV (254 nm) and are commercially available and promising for eliminating recalcitrant organic pollutants. The feasibility of VUV/UV as a chemical-free oxidation process was verified and quantitatively assessed by the concept of H2O2 equivalence (EQH2O2 ), at which UV/H2O2 showed the same performance as VUV/UV for the degradation of trace organic contaminants (TOrCs). Although VUV showed superior H2O activation and oxidation performance, its performance highly varied as a function of light path length (L p) in water, while that of UV/H2O2 proportionally decreased with decreasing H2O2 dose regardless of L p. On increasing L p from 1.0 to 3.0 cm, the EQH2O2 of VUV/UV decreased from 0.81 to 0.22 mM H2O2. Chloride and nitrate hardly influenced UV/H2O2, but they dramatically inhibited VUV/UV. The competitive absorbance of VUV by chloride and nitrate was verified as the main reason. The inhibitory effect was partially compensated by •OH formation from the propagation reactions of chloride or nitrate VUV photolysis, which was verified by kinetic modeling in Kintecus. In water with an L p of 2.0 cm, the EQH2O2 of VUV/UV decreased from 0.43 to 0.17 mM (60.8% decrease) on increasing the chloride concentration from 0 to 15 mM and to 0.20 mM (53.5% decrease) at 4 mM nitrate. The results of this study provide a comprehensive understanding of VUV/UV oxidation in comparison to UV/H2O2, which underscores the suitability and efficiency of chemical-free oxidation with VUV/UV. |
doi_str_mv | 10.1021/acs.est.3c08414 |
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The feasibility of VUV/UV as a chemical-free oxidation process was verified and quantitatively assessed by the concept of H2O2 equivalence (EQH2O2 ), at which UV/H2O2 showed the same performance as VUV/UV for the degradation of trace organic contaminants (TOrCs). Although VUV showed superior H2O activation and oxidation performance, its performance highly varied as a function of light path length (L p) in water, while that of UV/H2O2 proportionally decreased with decreasing H2O2 dose regardless of L p. On increasing L p from 1.0 to 3.0 cm, the EQH2O2 of VUV/UV decreased from 0.81 to 0.22 mM H2O2. Chloride and nitrate hardly influenced UV/H2O2, but they dramatically inhibited VUV/UV. The competitive absorbance of VUV by chloride and nitrate was verified as the main reason. The inhibitory effect was partially compensated by •OH formation from the propagation reactions of chloride or nitrate VUV photolysis, which was verified by kinetic modeling in Kintecus. In water with an L p of 2.0 cm, the EQH2O2 of VUV/UV decreased from 0.43 to 0.17 mM (60.8% decrease) on increasing the chloride concentration from 0 to 15 mM and to 0.20 mM (53.5% decrease) at 4 mM nitrate. The results of this study provide a comprehensive understanding of VUV/UV oxidation in comparison to UV/H2O2, which underscores the suitability and efficiency of chemical-free oxidation with VUV/UV.</description><identifier>ISSN: 0013-936X</identifier><identifier>EISSN: 1520-5851</identifier><identifier>DOI: 10.1021/acs.est.3c08414</identifier><language>eng</language><publisher>Easton: American Chemical Society</publisher><subject>Chloride ; Chlorides ; Contaminants ; Hydrogen peroxide ; Low pressure ; Mercury ; Mercury lamps ; Nitrates ; Occurrence, Fate, and Transport of Aquatic and Terrestrial Contaminants ; Organic chemicals ; Organic chemistry ; Organic contaminants ; Oxidation ; Oxidation process ; Photolysis</subject><ispartof>Environmental science & technology, 2024-04, Vol.58 (16), p.7113-7123</ispartof><rights>2024 American Chemical Society</rights><rights>Copyright American Chemical Society Apr 23, 2024</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><orcidid>0009-0005-2026-9220 ; 0000-0001-8355-3863 ; 0000-0003-2547-6366 ; 0009-0003-7121-1147 ; 0000-0002-9935-8533 ; 0000-0001-5132-2147 ; 0000-0003-2520-7596</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://pubs.acs.org/doi/pdf/10.1021/acs.est.3c08414$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/acs.est.3c08414$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>314,780,784,27076,27924,27925,56738,56788</link.rule.ids></links><search><creatorcontrib>Wang, Wen-Long</creatorcontrib><creatorcontrib>Jing, Zi-Bo</creatorcontrib><creatorcontrib>Zhang, Yi-Lin</creatorcontrib><creatorcontrib>Wu, Qian-Yuan</creatorcontrib><creatorcontrib>Drewes, Jörg E.</creatorcontrib><creatorcontrib>Lee, Min-Yong</creatorcontrib><creatorcontrib>Hübner, Uwe</creatorcontrib><title>Assessing the Chemical-Free Oxidation of Trace Organic Chemicals by VUV/UV as an Alternative to Conventional UV/H2O2</title><title>Environmental science & technology</title><addtitle>Environ. Sci. Technol</addtitle><description>Low-pressure mercury lamps with high-purity quartz can emit both vacuum-UV (VUV, 185 nm) and UV (254 nm) and are commercially available and promising for eliminating recalcitrant organic pollutants. The feasibility of VUV/UV as a chemical-free oxidation process was verified and quantitatively assessed by the concept of H2O2 equivalence (EQH2O2 ), at which UV/H2O2 showed the same performance as VUV/UV for the degradation of trace organic contaminants (TOrCs). Although VUV showed superior H2O activation and oxidation performance, its performance highly varied as a function of light path length (L p) in water, while that of UV/H2O2 proportionally decreased with decreasing H2O2 dose regardless of L p. On increasing L p from 1.0 to 3.0 cm, the EQH2O2 of VUV/UV decreased from 0.81 to 0.22 mM H2O2. Chloride and nitrate hardly influenced UV/H2O2, but they dramatically inhibited VUV/UV. The competitive absorbance of VUV by chloride and nitrate was verified as the main reason. The inhibitory effect was partially compensated by •OH formation from the propagation reactions of chloride or nitrate VUV photolysis, which was verified by kinetic modeling in Kintecus. In water with an L p of 2.0 cm, the EQH2O2 of VUV/UV decreased from 0.43 to 0.17 mM (60.8% decrease) on increasing the chloride concentration from 0 to 15 mM and to 0.20 mM (53.5% decrease) at 4 mM nitrate. The results of this study provide a comprehensive understanding of VUV/UV oxidation in comparison to UV/H2O2, which underscores the suitability and efficiency of chemical-free oxidation with VUV/UV.</description><subject>Chloride</subject><subject>Chlorides</subject><subject>Contaminants</subject><subject>Hydrogen peroxide</subject><subject>Low pressure</subject><subject>Mercury</subject><subject>Mercury lamps</subject><subject>Nitrates</subject><subject>Occurrence, Fate, and Transport of Aquatic and Terrestrial Contaminants</subject><subject>Organic chemicals</subject><subject>Organic chemistry</subject><subject>Organic contaminants</subject><subject>Oxidation</subject><subject>Oxidation process</subject><subject>Photolysis</subject><issn>0013-936X</issn><issn>1520-5851</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2024</creationdate><recordtype>article</recordtype><recordid>eNpdkcFLwzAUxoMoOKdnrwEvgnR7SZo0PY7inDDYZRveSpKmW0eXatON-d-bsqHg6cHj931873sIPRIYEaBkrIwfWd-NmAEZk_gKDQinEHHJyTUaABAWpUx83KI773cAQBnIAeom3lvvK7fB3dbibGv3lVF1NG2txYtTVaiuahxuSrxslQmrdqNcZX5Bj_U3Xq_W49UaK4-Vw5O6s60LsqPFXYOzxh2t601UjQM3owt6j27KILUPlzlEy-nrMptF88XbezaZR4py2kWljrnQiuok1TJmIbEsCg1lmRS8EDKFNJYQQplCGBCCc1XK0pik0FpqS9gQPZ9tP9vm6xC6yfeVN7aulbPNwefBkfKE0kQE9OkfumsO4Yq6p2IhKSMyDdTLmQpd_wEE8v4Beb_slZcHsB8903nj</recordid><startdate>20240423</startdate><enddate>20240423</enddate><creator>Wang, Wen-Long</creator><creator>Jing, Zi-Bo</creator><creator>Zhang, Yi-Lin</creator><creator>Wu, Qian-Yuan</creator><creator>Drewes, Jörg E.</creator><creator>Lee, Min-Yong</creator><creator>Hübner, Uwe</creator><general>American Chemical Society</general><scope>7QO</scope><scope>7ST</scope><scope>7T7</scope><scope>7U7</scope><scope>8FD</scope><scope>C1K</scope><scope>FR3</scope><scope>P64</scope><scope>SOI</scope><scope>7X8</scope><orcidid>https://orcid.org/0009-0005-2026-9220</orcidid><orcidid>https://orcid.org/0000-0001-8355-3863</orcidid><orcidid>https://orcid.org/0000-0003-2547-6366</orcidid><orcidid>https://orcid.org/0009-0003-7121-1147</orcidid><orcidid>https://orcid.org/0000-0002-9935-8533</orcidid><orcidid>https://orcid.org/0000-0001-5132-2147</orcidid><orcidid>https://orcid.org/0000-0003-2520-7596</orcidid></search><sort><creationdate>20240423</creationdate><title>Assessing the Chemical-Free Oxidation of Trace Organic Chemicals by VUV/UV as an Alternative to Conventional UV/H2O2</title><author>Wang, Wen-Long ; Jing, Zi-Bo ; Zhang, Yi-Lin ; Wu, Qian-Yuan ; Drewes, Jörg E. ; Lee, Min-Yong ; Hübner, Uwe</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a252t-fb456ba2b79b8430238ddb0ff7d5d68909480acecd6c06655af8fcc7dbb8be13</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2024</creationdate><topic>Chloride</topic><topic>Chlorides</topic><topic>Contaminants</topic><topic>Hydrogen peroxide</topic><topic>Low pressure</topic><topic>Mercury</topic><topic>Mercury lamps</topic><topic>Nitrates</topic><topic>Occurrence, Fate, and Transport of Aquatic and Terrestrial Contaminants</topic><topic>Organic chemicals</topic><topic>Organic chemistry</topic><topic>Organic contaminants</topic><topic>Oxidation</topic><topic>Oxidation process</topic><topic>Photolysis</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Wang, Wen-Long</creatorcontrib><creatorcontrib>Jing, Zi-Bo</creatorcontrib><creatorcontrib>Zhang, Yi-Lin</creatorcontrib><creatorcontrib>Wu, Qian-Yuan</creatorcontrib><creatorcontrib>Drewes, Jörg E.</creatorcontrib><creatorcontrib>Lee, Min-Yong</creatorcontrib><creatorcontrib>Hübner, Uwe</creatorcontrib><collection>Biotechnology Research Abstracts</collection><collection>Environment Abstracts</collection><collection>Industrial and Applied Microbiology Abstracts (Microbiology A)</collection><collection>Toxicology Abstracts</collection><collection>Technology Research Database</collection><collection>Environmental Sciences and Pollution Management</collection><collection>Engineering Research Database</collection><collection>Biotechnology and BioEngineering Abstracts</collection><collection>Environment Abstracts</collection><collection>MEDLINE - Academic</collection><jtitle>Environmental science & technology</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Wang, Wen-Long</au><au>Jing, Zi-Bo</au><au>Zhang, Yi-Lin</au><au>Wu, Qian-Yuan</au><au>Drewes, Jörg E.</au><au>Lee, Min-Yong</au><au>Hübner, Uwe</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Assessing the Chemical-Free Oxidation of Trace Organic Chemicals by VUV/UV as an Alternative to Conventional UV/H2O2</atitle><jtitle>Environmental science & technology</jtitle><addtitle>Environ. Sci. Technol</addtitle><date>2024-04-23</date><risdate>2024</risdate><volume>58</volume><issue>16</issue><spage>7113</spage><epage>7123</epage><pages>7113-7123</pages><issn>0013-936X</issn><eissn>1520-5851</eissn><abstract>Low-pressure mercury lamps with high-purity quartz can emit both vacuum-UV (VUV, 185 nm) and UV (254 nm) and are commercially available and promising for eliminating recalcitrant organic pollutants. The feasibility of VUV/UV as a chemical-free oxidation process was verified and quantitatively assessed by the concept of H2O2 equivalence (EQH2O2 ), at which UV/H2O2 showed the same performance as VUV/UV for the degradation of trace organic contaminants (TOrCs). Although VUV showed superior H2O activation and oxidation performance, its performance highly varied as a function of light path length (L p) in water, while that of UV/H2O2 proportionally decreased with decreasing H2O2 dose regardless of L p. On increasing L p from 1.0 to 3.0 cm, the EQH2O2 of VUV/UV decreased from 0.81 to 0.22 mM H2O2. Chloride and nitrate hardly influenced UV/H2O2, but they dramatically inhibited VUV/UV. The competitive absorbance of VUV by chloride and nitrate was verified as the main reason. The inhibitory effect was partially compensated by •OH formation from the propagation reactions of chloride or nitrate VUV photolysis, which was verified by kinetic modeling in Kintecus. In water with an L p of 2.0 cm, the EQH2O2 of VUV/UV decreased from 0.43 to 0.17 mM (60.8% decrease) on increasing the chloride concentration from 0 to 15 mM and to 0.20 mM (53.5% decrease) at 4 mM nitrate. The results of this study provide a comprehensive understanding of VUV/UV oxidation in comparison to UV/H2O2, which underscores the suitability and efficiency of chemical-free oxidation with VUV/UV.</abstract><cop>Easton</cop><pub>American Chemical Society</pub><doi>10.1021/acs.est.3c08414</doi><tpages>11</tpages><orcidid>https://orcid.org/0009-0005-2026-9220</orcidid><orcidid>https://orcid.org/0000-0001-8355-3863</orcidid><orcidid>https://orcid.org/0000-0003-2547-6366</orcidid><orcidid>https://orcid.org/0009-0003-7121-1147</orcidid><orcidid>https://orcid.org/0000-0002-9935-8533</orcidid><orcidid>https://orcid.org/0000-0001-5132-2147</orcidid><orcidid>https://orcid.org/0000-0003-2520-7596</orcidid></addata></record> |
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subjects | Chloride Chlorides Contaminants Hydrogen peroxide Low pressure Mercury Mercury lamps Nitrates Occurrence, Fate, and Transport of Aquatic and Terrestrial Contaminants Organic chemicals Organic chemistry Organic contaminants Oxidation Oxidation process Photolysis |
title | Assessing the Chemical-Free Oxidation of Trace Organic Chemicals by VUV/UV as an Alternative to Conventional UV/H2O2 |
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