Reevaluation of the contributions of reactive intermediates to the photochemical transformation of 17β-estradiol in sewage effluent
•The reaction rate constants of PPRIs with E2 were measured at various pH.•EfOM can act as a photosensitizer and an inhibitor in the phototransformation of E2.•Solar photodegradation can reduce the risk of endocrine disruption impacted by E2. Photodegradation of the natural steroid 17β-estradiol (E2...
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| Published in | Water research (Oxford) Vol. 189; p. 116633 |
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| Main Authors | , , , , , , |
| Format | Journal Article |
| Language | English |
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Elsevier Ltd
01.02.2021
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| Abstract | •The reaction rate constants of PPRIs with E2 were measured at various pH.•EfOM can act as a photosensitizer and an inhibitor in the phototransformation of E2.•Solar photodegradation can reduce the risk of endocrine disruption impacted by E2.
Photodegradation of the natural steroid 17β-estradiol (E2), an endocrine-disrupting hormone that has been widely detected in aquatic environments, was investigated in wastewater effluents at various pH ranges under simulated solar irradiation. The rate of E2 degradation in the sewage effluents was stable at pH 6.0-7.0 but suddenly increased from pH 8.0-10.0. The second-order reaction rate constants of E2 with 3EfOM* and CO3•− were measured to increase 11.0-fold and 18.0-fold from pH 6.0 to 10.0, respectively. Two main reasons are proposed for this sharp increase. First, the change in the ionization state of E2 made it susceptible to oxidation by triplet-state effluent organic matter (3EfOM*) and carbonate radicals (CO3•−). Second, the steady-state concentration of CO3•− increased with increasing pH. Indirect photolysis was suggested to be the main degradation pathway in the sewage effluents, and 3EfOM* was proposed to play a major role at pH 8.0-9.0, while CO3•− played a significant role at pH 10.0. In this study, EfOM was shown for the first time to inhibit the oxidation of E2 initiated by 3EfOM* and CO3•−. Thus, we suggest that EfOM plays a dual role in the photodegradation of E2: EfOM can not only be activated as 3EfOM* to degrade E2 but also can inhibit the degradation of E2 by reducing the E2 oxidation intermediate back to E2. The estrogenic activity of the photodegradation products was also studied. The in vitro estrogenic activity of E2 solutions decreased approximately as fast as the E2 photodegradation occurred in the effluent water at various pH values, suggesting that solar photodegradation in sewage effluents reduces the risk of endocrine disruption in waters impacted by E2 and subject to continuing inputs. The results of this study are important for predicting the environmental fate of endocrine-disrupting chemicals and developing methods for their removal from aquatic environments.
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| AbstractList | Photodegradation of the natural steroid 17β-estradiol (E2), an endocrine-disrupting hormone that has been widely detected in aquatic environments, was investigated in wastewater effluents at various pH ranges under simulated solar irradiation. The rate of E2 degradation in the sewage effluents was stable at pH 6.0-7.0 but suddenly increased from pH 8.0-10.0. The second-order reaction rate constants of E2 with
EfOM* and CO
were measured to increase 11.0-fold and 18.0-fold from pH 6.0 to 10.0, respectively. Two main reasons are proposed for this sharp increase. First, the change in the ionization state of E2 made it susceptible to oxidation by triplet-state effluent organic matter (
EfOM*) and carbonate radicals (CO
). Second, the steady-state concentration of CO
increased with increasing pH. Indirect photolysis was suggested to be the main degradation pathway in the sewage effluents, and
EfOM* was proposed to play a major role at pH 8.0-9.0, while CO
played a significant role at pH 10.0. In this study, EfOM was shown for the first time to inhibit the oxidation of E2 initiated by
EfOM* and CO
. Thus, we suggest that EfOM plays a dual role in the photodegradation of E2: EfOM can not only be activated as
EfOM* to degrade E2 but also can inhibit the degradation of E2 by reducing the E2 oxidation intermediate back to E2. The estrogenic activity of the photodegradation products was also studied. The in vitro estrogenic activity of E2 solutions decreased approximately as fast as the E2 photodegradation occurred in the effluent water at various pH values, suggesting that solar photodegradation in sewage effluents reduces the risk of endocrine disruption in waters impacted by E2 and subject to continuing inputs. The results of this study are important for predicting the environmental fate of endocrine-disrupting chemicals and developing methods for their removal from aquatic environments. Photodegradation of the natural steroid 17β-estradiol (E2), an endocrine-disrupting hormone that has been widely detected in aquatic environments, was investigated in wastewater effluents at various pH ranges under simulated solar irradiation. The rate of E2 degradation in the sewage effluents was stable at pH 6.0-7.0 but suddenly increased from pH 8.0-10.0. The second-order reaction rate constants of E2 with 3EfOM* and CO3•- were measured to increase 11.0-fold and 18.0-fold from pH 6.0 to 10.0, respectively. Two main reasons are proposed for this sharp increase. First, the change in the ionization state of E2 made it susceptible to oxidation by triplet-state effluent organic matter (3EfOM*) and carbonate radicals (CO3•-). Second, the steady-state concentration of CO3•- increased with increasing pH. Indirect photolysis was suggested to be the main degradation pathway in the sewage effluents, and 3EfOM* was proposed to play a major role at pH 8.0-9.0, while CO3•- played a significant role at pH 10.0. In this study, EfOM was shown for the first time to inhibit the oxidation of E2 initiated by 3EfOM* and CO3•-. Thus, we suggest that EfOM plays a dual role in the photodegradation of E2: EfOM can not only be activated as 3EfOM* to degrade E2 but also can inhibit the degradation of E2 by reducing the E2 oxidation intermediate back to E2. The estrogenic activity of the photodegradation products was also studied. The in vitro estrogenic activity of E2 solutions decreased approximately as fast as the E2 photodegradation occurred in the effluent water at various pH values, suggesting that solar photodegradation in sewage effluents reduces the risk of endocrine disruption in waters impacted by E2 and subject to continuing inputs. The results of this study are important for predicting the environmental fate of endocrine-disrupting chemicals and developing methods for their removal from aquatic environments.Photodegradation of the natural steroid 17β-estradiol (E2), an endocrine-disrupting hormone that has been widely detected in aquatic environments, was investigated in wastewater effluents at various pH ranges under simulated solar irradiation. The rate of E2 degradation in the sewage effluents was stable at pH 6.0-7.0 but suddenly increased from pH 8.0-10.0. The second-order reaction rate constants of E2 with 3EfOM* and CO3•- were measured to increase 11.0-fold and 18.0-fold from pH 6.0 to 10.0, respectively. Two main reasons are proposed for this sharp increase. First, the change in the ionization state of E2 made it susceptible to oxidation by triplet-state effluent organic matter (3EfOM*) and carbonate radicals (CO3•-). Second, the steady-state concentration of CO3•- increased with increasing pH. Indirect photolysis was suggested to be the main degradation pathway in the sewage effluents, and 3EfOM* was proposed to play a major role at pH 8.0-9.0, while CO3•- played a significant role at pH 10.0. In this study, EfOM was shown for the first time to inhibit the oxidation of E2 initiated by 3EfOM* and CO3•-. Thus, we suggest that EfOM plays a dual role in the photodegradation of E2: EfOM can not only be activated as 3EfOM* to degrade E2 but also can inhibit the degradation of E2 by reducing the E2 oxidation intermediate back to E2. The estrogenic activity of the photodegradation products was also studied. The in vitro estrogenic activity of E2 solutions decreased approximately as fast as the E2 photodegradation occurred in the effluent water at various pH values, suggesting that solar photodegradation in sewage effluents reduces the risk of endocrine disruption in waters impacted by E2 and subject to continuing inputs. The results of this study are important for predicting the environmental fate of endocrine-disrupting chemicals and developing methods for their removal from aquatic environments. •The reaction rate constants of PPRIs with E2 were measured at various pH.•EfOM can act as a photosensitizer and an inhibitor in the phototransformation of E2.•Solar photodegradation can reduce the risk of endocrine disruption impacted by E2. Photodegradation of the natural steroid 17β-estradiol (E2), an endocrine-disrupting hormone that has been widely detected in aquatic environments, was investigated in wastewater effluents at various pH ranges under simulated solar irradiation. The rate of E2 degradation in the sewage effluents was stable at pH 6.0-7.0 but suddenly increased from pH 8.0-10.0. The second-order reaction rate constants of E2 with 3EfOM* and CO3•− were measured to increase 11.0-fold and 18.0-fold from pH 6.0 to 10.0, respectively. Two main reasons are proposed for this sharp increase. First, the change in the ionization state of E2 made it susceptible to oxidation by triplet-state effluent organic matter (3EfOM*) and carbonate radicals (CO3•−). Second, the steady-state concentration of CO3•− increased with increasing pH. Indirect photolysis was suggested to be the main degradation pathway in the sewage effluents, and 3EfOM* was proposed to play a major role at pH 8.0-9.0, while CO3•− played a significant role at pH 10.0. In this study, EfOM was shown for the first time to inhibit the oxidation of E2 initiated by 3EfOM* and CO3•−. Thus, we suggest that EfOM plays a dual role in the photodegradation of E2: EfOM can not only be activated as 3EfOM* to degrade E2 but also can inhibit the degradation of E2 by reducing the E2 oxidation intermediate back to E2. The estrogenic activity of the photodegradation products was also studied. The in vitro estrogenic activity of E2 solutions decreased approximately as fast as the E2 photodegradation occurred in the effluent water at various pH values, suggesting that solar photodegradation in sewage effluents reduces the risk of endocrine disruption in waters impacted by E2 and subject to continuing inputs. The results of this study are important for predicting the environmental fate of endocrine-disrupting chemicals and developing methods for their removal from aquatic environments. [Display omitted] Photodegradation of the natural steroid 17β-estradiol (E2), an endocrine-disrupting hormone that has been widely detected in aquatic environments, was investigated in wastewater effluents at various pH ranges under simulated solar irradiation. The rate of E2 degradation in the sewage effluents was stable at pH 6.0-7.0 but suddenly increased from pH 8.0-10.0. The second-order reaction rate constants of E2 with ³EfOM* and CO₃•⁻ were measured to increase 11.0-fold and 18.0-fold from pH 6.0 to 10.0, respectively. Two main reasons are proposed for this sharp increase. First, the change in the ionization state of E2 made it susceptible to oxidation by triplet-state effluent organic matter (³EfOM*) and carbonate radicals (CO₃•⁻). Second, the steady-state concentration of CO₃•⁻ increased with increasing pH. Indirect photolysis was suggested to be the main degradation pathway in the sewage effluents, and ³EfOM* was proposed to play a major role at pH 8.0-9.0, while CO₃•⁻ played a significant role at pH 10.0. In this study, EfOM was shown for the first time to inhibit the oxidation of E2 initiated by ³EfOM* and CO₃•⁻. Thus, we suggest that EfOM plays a dual role in the photodegradation of E2: EfOM can not only be activated as ³EfOM* to degrade E2 but also can inhibit the degradation of E2 by reducing the E2 oxidation intermediate back to E2. The estrogenic activity of the photodegradation products was also studied. The in vitro estrogenic activity of E2 solutions decreased approximately as fast as the E2 photodegradation occurred in the effluent water at various pH values, suggesting that solar photodegradation in sewage effluents reduces the risk of endocrine disruption in waters impacted by E2 and subject to continuing inputs. The results of this study are important for predicting the environmental fate of endocrine-disrupting chemicals and developing methods for their removal from aquatic environments. |
| ArticleNumber | 116633 |
| Author | Yan, Shuwen Liu, Qian Hao, Zhenyu Liu, Yingjie Song, Weihua Lian, Lushi Miao, Chenyong |
| Author_xml | – sequence: 1 givenname: Lushi surname: Lian fullname: Lian, Lushi organization: Department of Environmental Science & Engineering, Fudan University, Shanghai 200433, PR China – sequence: 2 givenname: Chenyong surname: Miao fullname: Miao, Chenyong organization: Department of Environmental Science & Engineering, Fudan University, Shanghai 200433, PR China – sequence: 3 givenname: Zhenyu surname: Hao fullname: Hao, Zhenyu organization: Department of Environmental Science & Engineering, Fudan University, Shanghai 200433, PR China – sequence: 4 givenname: Qian surname: Liu fullname: Liu, Qian organization: National Engineering Laboratory for Lake Pollution Control and Ecological Restoration, Institute of Lake Environment, Chinese Research Academy of Environmental Sciences, Beijing, 100012, PR China – sequence: 5 givenname: Yingjie surname: Liu fullname: Liu, Yingjie organization: Department of Environmental Science & Engineering, Fudan University, Shanghai 200433, PR China – sequence: 6 givenname: Weihua orcidid: 0000-0001-7633-7919 surname: Song fullname: Song, Weihua organization: Department of Environmental Science & Engineering, Fudan University, Shanghai 200433, PR China – sequence: 7 givenname: Shuwen surname: Yan fullname: Yan, Shuwen email: yanshuwen@fudan.edu.cn organization: Department of Environmental Science & Engineering, Fudan University, Shanghai 200433, PR China |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/33221582$$D View this record in MEDLINE/PubMed |
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| CitedBy_id | crossref_primary_10_1021_acs_est_1c02630 crossref_primary_10_1039_D2EW00082B crossref_primary_10_1016_j_watres_2024_122720 crossref_primary_10_1039_D1EW00863C crossref_primary_10_1016_j_cej_2023_143778 crossref_primary_10_1016_j_watres_2023_120438 crossref_primary_10_1016_j_chemosphere_2023_140660 crossref_primary_10_1016_j_chemosphere_2024_141195 crossref_primary_10_1016_j_watres_2023_120714 crossref_primary_10_1021_acs_est_3c08782 crossref_primary_10_1016_j_psep_2023_02_003 crossref_primary_10_1007_s43630_021_00107_w crossref_primary_10_1016_j_watres_2022_118967 crossref_primary_10_1016_j_apcatb_2023_123573 crossref_primary_10_1016_j_jhazmat_2023_132759 crossref_primary_10_1016_j_cej_2024_149353 crossref_primary_10_1016_j_watres_2021_116904 |
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| Keywords | Photodegradation Reactive oxygen species Sewage effluent Endocrine-disrupting chemicals Inhibitory effect |
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| Snippet | •The reaction rate constants of PPRIs with E2 were measured at various pH.•EfOM can act as a photosensitizer and an inhibitor in the phototransformation of... Photodegradation of the natural steroid 17β-estradiol (E2), an endocrine-disrupting hormone that has been widely detected in aquatic environments, was... |
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| SubjectTerms | carbonates Endocrine-disrupting chemicals environmental fate Estradiol estrogenic properties Inhibitory effect ionization organic matter oxidation Photodegradation Photolysis Reactive oxygen species risk Sewage Sewage effluent solar radiation Waste Water wastewater water Water Pollutants, Chemical - analysis |
| Title | Reevaluation of the contributions of reactive intermediates to the photochemical transformation of 17β-estradiol in sewage effluent |
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