Oscar Almendros-Ginestà , M. Angeles Clavero-Sánchez , Miguel García-Gutiérrez , Tiziana Missana
{"title":"在异糖酸盐和邻苯二甲酸盐存在下，波特兰铁矿对放射性核素的保留以及三元配合物的可能作用","authors":"Oscar Almendros-Ginestà , M. Angeles Clavero-Sánchez , Miguel García-Gutiérrez , Tiziana Missana","doi":"10.1016/j.chemosphere.2025.144224","DOIUrl":null,"url":null,"abstract":"<div><div>This research evaluates the retention mechanisms for various radionuclides (RN) specifically, <sup>63</sup>Ni, <sup>233</sup>U, <sup>152</sup>Eu and <sup>238</sup>Pu, on portlandite, in the presence of two organic ligands (ORG): isosaccharinate (ISA) and phthalate (PHTH).</div><div>The potential negative impact of ORG on RN uptake by the solid phase may arise from two main mechanisms that were analysed: (a) the competitive adsorption of ORG or (b) the formation of RN-ORG complexes in the aqueous phase.</div><div>The sorption of ISA on portlandite exhibited a maximum log(K<sub>d</sub>) value of 2.1 mL g<sup>−1</sup>, decreasing when the total ISA concentration exceeded 1·10<sup>−3</sup> M. No sorption of PHTH was detected. Aqueous RN speciation, calculated using the Thermochimie 12a thermodynamic database, revealed formation of RN-ORG complexes only in the presence of ISA.</div><div>The observed RN sorption behavior in the presence of ISA or PHTH aligned with these findings. The calculated sorption reduction factors (SRFs) were significantly higher for ISA compared to PHTH, particularly for <sup>152</sup>Eu and <sup>238</sup>Pu. However, the detrimental effect of ISA on RN retention was orders of magnitude lower than the predicted by geochemical modelling and, sometimes, the presence of ORG (especially at low concentrations) increased RN sorption, suggesting the formation of RN + ORG + portlandite ternary complexes.</div></div>","PeriodicalId":276,"journal":{"name":"Chemosphere","volume":"374 ","pages":"Article 144224"},"PeriodicalIF":8.1000,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Radionuclide retention by portlandite in the presence of isosaccharinate and phthalate and possible role of ternary complexes\",\"authors\":\"Oscar Almendros-Ginestà , M. Angeles Clavero-Sánchez , Miguel García-Gutiérrez , Tiziana Missana\",\"doi\":\"10.1016/j.chemosphere.2025.144224\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>This research evaluates the retention mechanisms for various radionuclides (RN) specifically, <sup>63</sup>Ni, <sup>233</sup>U, <sup>152</sup>Eu and <sup>238</sup>Pu, on portlandite, in the presence of two organic ligands (ORG): isosaccharinate (ISA) and phthalate (PHTH).</div><div>The potential negative impact of ORG on RN uptake by the solid phase may arise from two main mechanisms that were analysed: (a) the competitive adsorption of ORG or (b) the formation of RN-ORG complexes in the aqueous phase.</div><div>The sorption of ISA on portlandite exhibited a maximum log(K<sub>d</sub>) value of 2.1 mL g<sup>−1</sup>, decreasing when the total ISA concentration exceeded 1·10<sup>−3</sup> M. No sorption of PHTH was detected. Aqueous RN speciation, calculated using the Thermochimie 12a thermodynamic database, revealed formation of RN-ORG complexes only in the presence of ISA.</div><div>The observed RN sorption behavior in the presence of ISA or PHTH aligned with these findings. The calculated sorption reduction factors (SRFs) were significantly higher for ISA compared to PHTH, particularly for <sup>152</sup>Eu and <sup>238</sup>Pu. However, the detrimental effect of ISA on RN retention was orders of magnitude lower than the predicted by geochemical modelling and, sometimes, the presence of ORG (especially at low concentrations) increased RN sorption, suggesting the formation of RN + ORG + portlandite ternary complexes.</div></div>\",\"PeriodicalId\":276,\"journal\":{\"name\":\"Chemosphere\",\"volume\":\"374 \",\"pages\":\"Article 144224\"},\"PeriodicalIF\":8.1000,\"publicationDate\":\"2025-04-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Chemosphere\",\"FirstCategoryId\":\"93\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0045653525001663\",\"RegionNum\":2,\"RegionCategory\":\"环境科学与生态学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"2025/2/17 0:00:00\",\"PubModel\":\"Epub\",\"JCR\":\"Q1\",\"JCRName\":\"ENVIRONMENTAL SCIENCES\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemosphere","FirstCategoryId":"93","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0045653525001663","RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2025/2/17 0:00:00","PubModel":"Epub","JCR":"Q1","JCRName":"ENVIRONMENTAL SCIENCES","Score":null,"Total":0}
Radionuclide retention by portlandite in the presence of isosaccharinate and phthalate and possible role of ternary complexes
This research evaluates the retention mechanisms for various radionuclides (RN) specifically, 63Ni, 233U, 152Eu and 238Pu, on portlandite, in the presence of two organic ligands (ORG): isosaccharinate (ISA) and phthalate (PHTH).
The potential negative impact of ORG on RN uptake by the solid phase may arise from two main mechanisms that were analysed: (a) the competitive adsorption of ORG or (b) the formation of RN-ORG complexes in the aqueous phase.
The sorption of ISA on portlandite exhibited a maximum log(Kd) value of 2.1 mL g−1, decreasing when the total ISA concentration exceeded 1·10−3 M. No sorption of PHTH was detected. Aqueous RN speciation, calculated using the Thermochimie 12a thermodynamic database, revealed formation of RN-ORG complexes only in the presence of ISA.
The observed RN sorption behavior in the presence of ISA or PHTH aligned with these findings. The calculated sorption reduction factors (SRFs) were significantly higher for ISA compared to PHTH, particularly for 152Eu and 238Pu. However, the detrimental effect of ISA on RN retention was orders of magnitude lower than the predicted by geochemical modelling and, sometimes, the presence of ORG (especially at low concentrations) increased RN sorption, suggesting the formation of RN + ORG + portlandite ternary complexes.
期刊介绍：
Chemosphere, being an international multidisciplinary journal, is dedicated to publishing original communications and review articles on chemicals in the environment. The scope covers a wide range of topics, including the identification, quantification, behavior, fate, toxicology, treatment, and remediation of chemicals in the bio-, hydro-, litho-, and atmosphere, ensuring the broad dissemination of research in this field.
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