pH modifies the oxidative potential and peroxide content of biomass burning HULIS under dark aging
Humic-like substances (HULIS) account for a major redox-active fraction of biomass burning organic aerosols (BBOA). During atmospheric transport, fresh acidic BB-HULIS in droplets and humid aerosols are subject to neutralization and pH-modified aging process. In this study, solutions containing HULI...
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| Published in | The Science of the total environment Vol. 834; p. 155365 |
|---|---|
| Main Authors | , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
Netherlands
Elsevier B.V
15.08.2022
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| Subjects | |
| Online Access | Get full text |
| ISSN | 0048-9697 1879-1026 1879-1026 |
| DOI | 10.1016/j.scitotenv.2022.155365 |
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| Abstract | Humic-like substances (HULIS) account for a major redox-active fraction of biomass burning organic aerosols (BBOA). During atmospheric transport, fresh acidic BB-HULIS in droplets and humid aerosols are subject to neutralization and pH-modified aging process. In this study, solutions containing HULIS isolated from wood smoldering emissions were first adjusted with NaOH and NH3 to pH values in the range of 3.6–9.0 and then aged under oxic dark conditions. Evolution of HULIS oxidative potential (OP) and total peroxide content (equivalent H2O2 concentration, H2O2eq) were measured together with the changes in solution absorbance and chemical composition. Notable immediate responses such as peroxide generation, HULIS autoxidation, and an increase in OP and light absorption were observed under alkaline conditions. Initial H2O2eq, OP, and absorption increased exponentially with pH, regardless of the alkaline species added. Dark aging further oxidized the HULIS and led to pH-dependent toxic and chemical changes, exhibiting an alkaline-facilitated initial increase followed by a decrease of OP and H2O2eq. Although highly correlated with HULIS OP, the contributions of H2O2eq to OP are minor but increased both with solution pH and dark aging time. Alkalinity-assisted autoxidation of phenolic compounds and quinoids with concomitant formation of H2O2 and other alkalinity-favored peroxide oxidation reactions are proposed here for explaining the observed HULIS OP and chemical changes in the dark. Our findings suggest that alkaline neutralization of fresh BB-HULIS represents a previously overlooked peroxide source and pathway for modifying aerosol redox-activity and composition. Additionally, these findings imply that the lung fluid neutral environment can modify the OP and peroxide content of inhaled BB-HULIS. The results also suggest that common separation protocols of HULIS using base extraction methods should be treated with caution when evaluating and comparing their composition, absorption, and relative toxicity.
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•pH plays a crucial role in determining fresh BB-HULIS characters•Light absorption, OP, and peroxide yield of fresh BB-HULIS increase exponentially with solution pH•Increase solution alkalinity promotes BB-HULIS autoxidation and facilitates OP and peroxides changes in dark aging•Alkalinity-assisted autoxidation of BB-HULIS in lung fluid represents potential health hazard |
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| AbstractList | Humic-like substances (HULIS) account for a major redox-active fraction of biomass burning organic aerosols (BBOA). During atmospheric transport, fresh acidic BB-HULIS in droplets and humid aerosols are subject to neutralization and pH-modified aging process. In this study, solutions containing HULIS isolated from wood smoldering emissions were first adjusted with NaOH and NH3 to pH values in the range of 3.6-9.0 and then aged under oxic dark conditions. Evolution of HULIS oxidative potential (OP) and total peroxide content (equivalent H2O2 concentration, H2O2eq) were measured together with the changes in solution absorbance and chemical composition. Notable immediate responses such as peroxide generation, HULIS autoxidation, and an increase in OP and light absorption were observed under alkaline conditions. Initial H2O2eq, OP, and absorption increased exponentially with pH, regardless of the alkaline species added. Dark aging further oxidized the HULIS and led to pH-dependent toxic and chemical changes, exhibiting an alkaline-facilitated initial increase followed by a decrease of OP and H2O2eq. Although highly correlated with HULIS OP, the contributions of H2O2eq to OP are minor but increased both with solution pH and dark aging time. Alkalinity-assisted autoxidation of phenolic compounds and quinoids with concomitant formation of H2O2 and other alkalinity-favored peroxide oxidation reactions are proposed here for explaining the observed HULIS OP and chemical changes in the dark. Our findings suggest that alkaline neutralization of fresh BB-HULIS represents a previously overlooked peroxide source and pathway for modifying aerosol redox-activity and composition. Additionally, these findings imply that the lung fluid neutral environment can modify the OP and peroxide content of inhaled BB-HULIS. The results also suggest that common separation protocols of HULIS using base extraction methods should be treated with caution when evaluating and comparing their composition, absorption, and relative toxicity.Humic-like substances (HULIS) account for a major redox-active fraction of biomass burning organic aerosols (BBOA). During atmospheric transport, fresh acidic BB-HULIS in droplets and humid aerosols are subject to neutralization and pH-modified aging process. In this study, solutions containing HULIS isolated from wood smoldering emissions were first adjusted with NaOH and NH3 to pH values in the range of 3.6-9.0 and then aged under oxic dark conditions. Evolution of HULIS oxidative potential (OP) and total peroxide content (equivalent H2O2 concentration, H2O2eq) were measured together with the changes in solution absorbance and chemical composition. Notable immediate responses such as peroxide generation, HULIS autoxidation, and an increase in OP and light absorption were observed under alkaline conditions. Initial H2O2eq, OP, and absorption increased exponentially with pH, regardless of the alkaline species added. Dark aging further oxidized the HULIS and led to pH-dependent toxic and chemical changes, exhibiting an alkaline-facilitated initial increase followed by a decrease of OP and H2O2eq. Although highly correlated with HULIS OP, the contributions of H2O2eq to OP are minor but increased both with solution pH and dark aging time. Alkalinity-assisted autoxidation of phenolic compounds and quinoids with concomitant formation of H2O2 and other alkalinity-favored peroxide oxidation reactions are proposed here for explaining the observed HULIS OP and chemical changes in the dark. Our findings suggest that alkaline neutralization of fresh BB-HULIS represents a previously overlooked peroxide source and pathway for modifying aerosol redox-activity and composition. Additionally, these findings imply that the lung fluid neutral environment can modify the OP and peroxide content of inhaled BB-HULIS. The results also suggest that common separation protocols of HULIS using base extraction methods should be treated with caution when evaluating and comparing their composition, absorption, and relative toxicity. Humic-like substances (HULIS) account for a major redox-active fraction of biomass burning organic aerosols (BBOA). During atmospheric transport, fresh acidic BB-HULIS in droplets and humid aerosols are subject to neutralization and pH-modified aging process. In this study, solutions containing HULIS isolated from wood smoldering emissions were first adjusted with NaOH and NH to pH values in the range of 3.6-9.0 and then aged under oxic dark conditions. Evolution of HULIS oxidative potential (OP) and total peroxide content (equivalent H O concentration, H O eq) were measured together with the changes in solution absorbance and chemical composition. Notable immediate responses such as peroxide generation, HULIS autoxidation, and an increase in OP and light absorption were observed under alkaline conditions. Initial H O eq, OP, and absorption increased exponentially with pH, regardless of the alkaline species added. Dark aging further oxidized the HULIS and led to pH-dependent toxic and chemical changes, exhibiting an alkaline-facilitated initial increase followed by a decrease of OP and H O eq. Although highly correlated with HULIS OP, the contributions of H O eq to OP are minor but increased both with solution pH and dark aging time. Alkalinity-assisted autoxidation of phenolic compounds and quinoids with concomitant formation of H O and other alkalinity-favored peroxide oxidation reactions are proposed here for explaining the observed HULIS OP and chemical changes in the dark. Our findings suggest that alkaline neutralization of fresh BB-HULIS represents a previously overlooked peroxide source and pathway for modifying aerosol redox-activity and composition. Additionally, these findings imply that the lung fluid neutral environment can modify the OP and peroxide content of inhaled BB-HULIS. The results also suggest that common separation protocols of HULIS using base extraction methods should be treated with caution when evaluating and comparing their composition, absorption, and relative toxicity. Humic-like substances (HULIS) account for a major redox-active fraction of biomass burning organic aerosols (BBOA). During atmospheric transport, fresh acidic BB-HULIS in droplets and humid aerosols are subject to neutralization and pH-modified aging process. In this study, solutions containing HULIS isolated from wood smoldering emissions were first adjusted with NaOH and NH3 to pH values in the range of 3.6–9.0 and then aged under oxic dark conditions. Evolution of HULIS oxidative potential (OP) and total peroxide content (equivalent H2O2 concentration, H2O2eq) were measured together with the changes in solution absorbance and chemical composition. Notable immediate responses such as peroxide generation, HULIS autoxidation, and an increase in OP and light absorption were observed under alkaline conditions. Initial H2O2eq, OP, and absorption increased exponentially with pH, regardless of the alkaline species added. Dark aging further oxidized the HULIS and led to pH-dependent toxic and chemical changes, exhibiting an alkaline-facilitated initial increase followed by a decrease of OP and H2O2eq. Although highly correlated with HULIS OP, the contributions of H2O2eq to OP are minor but increased both with solution pH and dark aging time. Alkalinity-assisted autoxidation of phenolic compounds and quinoids with concomitant formation of H2O2 and other alkalinity-favored peroxide oxidation reactions are proposed here for explaining the observed HULIS OP and chemical changes in the dark. Our findings suggest that alkaline neutralization of fresh BB-HULIS represents a previously overlooked peroxide source and pathway for modifying aerosol redox-activity and composition. Additionally, these findings imply that the lung fluid neutral environment can modify the OP and peroxide content of inhaled BB-HULIS. The results also suggest that common separation protocols of HULIS using base extraction methods should be treated with caution when evaluating and comparing their composition, absorption, and relative toxicity. [Display omitted] •pH plays a crucial role in determining fresh BB-HULIS characters•Light absorption, OP, and peroxide yield of fresh BB-HULIS increase exponentially with solution pH•Increase solution alkalinity promotes BB-HULIS autoxidation and facilitates OP and peroxides changes in dark aging•Alkalinity-assisted autoxidation of BB-HULIS in lung fluid represents potential health hazard Humic-like substances (HULIS) account for a major redox-active fraction of biomass burning organic aerosols (BBOA). During atmospheric transport, fresh acidic BB-HULIS in droplets and humid aerosols are subject to neutralization and pH-modified aging process. In this study, solutions containing HULIS isolated from wood smoldering emissions were first adjusted with NaOH and NH₃ to pH values in the range of 3.6–9.0 and then aged under oxic dark conditions. Evolution of HULIS oxidative potential (OP) and total peroxide content (equivalent H₂O₂ concentration, H₂O₂eq) were measured together with the changes in solution absorbance and chemical composition. Notable immediate responses such as peroxide generation, HULIS autoxidation, and an increase in OP and light absorption were observed under alkaline conditions. Initial H₂O₂eq, OP, and absorption increased exponentially with pH, regardless of the alkaline species added. Dark aging further oxidized the HULIS and led to pH-dependent toxic and chemical changes, exhibiting an alkaline-facilitated initial increase followed by a decrease of OP and H₂O₂eq. Although highly correlated with HULIS OP, the contributions of H₂O₂eq to OP are minor but increased both with solution pH and dark aging time. Alkalinity-assisted autoxidation of phenolic compounds and quinoids with concomitant formation of H₂O₂ and other alkalinity-favored peroxide oxidation reactions are proposed here for explaining the observed HULIS OP and chemical changes in the dark. Our findings suggest that alkaline neutralization of fresh BB-HULIS represents a previously overlooked peroxide source and pathway for modifying aerosol redox-activity and composition. Additionally, these findings imply that the lung fluid neutral environment can modify the OP and peroxide content of inhaled BB-HULIS. The results also suggest that common separation protocols of HULIS using base extraction methods should be treated with caution when evaluating and comparing their composition, absorption, and relative toxicity. |
| ArticleNumber | 155365 |
| Author | Czech, Hendryk Pardo, Michal Zimmermann, Ralf Schneider, Eric Rüger, Christopher P. Fang, Zheng Chen, Jianmin Li, Chunlin Laskin, Alexandre Rudich, Yinon |
| Author_xml | – sequence: 1 givenname: Chunlin surname: Li fullname: Li, Chunlin email: chunlin.li@weizmann.ac.il organization: Department of Earth and Planetary Sciences, Weizmann Institute of Science, Rehovot 76100, Israel – sequence: 2 givenname: Zheng surname: Fang fullname: Fang, Zheng organization: Department of Earth and Planetary Sciences, Weizmann Institute of Science, Rehovot 76100, Israel – sequence: 3 givenname: Hendryk surname: Czech fullname: Czech, Hendryk organization: Joint Mass Spectrometry Centre, Institute of Chemistry, University of Rostock, 18059 Rostock, Germany – sequence: 4 givenname: Eric surname: Schneider fullname: Schneider, Eric organization: Joint Mass Spectrometry Centre, Institute of Chemistry, University of Rostock, 18059 Rostock, Germany – sequence: 5 givenname: Christopher P. surname: Rüger fullname: Rüger, Christopher P. organization: Joint Mass Spectrometry Centre, Institute of Chemistry, University of Rostock, 18059 Rostock, Germany – sequence: 6 givenname: Michal surname: Pardo fullname: Pardo, Michal organization: Department of Earth and Planetary Sciences, Weizmann Institute of Science, Rehovot 76100, Israel – sequence: 7 givenname: Ralf surname: Zimmermann fullname: Zimmermann, Ralf organization: Joint Mass Spectrometry Centre, Institute of Chemistry, University of Rostock, 18059 Rostock, Germany – sequence: 8 givenname: Jianmin surname: Chen fullname: Chen, Jianmin organization: Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention, Department of Environmental Science and Engineering, Institute of Atmospheric Sciences, Fudan University, Shanghai 200438, China – sequence: 9 givenname: Alexandre surname: Laskin fullname: Laskin, Alexandre organization: Department of Chemistry, Purdue University, West Lafayette, Indiana 47907, United States – sequence: 10 givenname: Yinon surname: Rudich fullname: Rudich, Yinon email: yinon.rudich@weizmann.ac.il organization: Department of Earth and Planetary Sciences, Weizmann Institute of Science, Rehovot 76100, Israel |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/35460777$$D View this record in MEDLINE/PubMed |
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| Keywords | Autoxidation Biomass burning HULIS Peroxides Aqueous aging Oxidative potential pH influence |
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| Title | pH modifies the oxidative potential and peroxide content of biomass burning HULIS under dark aging |
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