{"title":"EDTA、柠檬酸盐和邻苯二甲酸盐对蒙脱石吸附Cs、Sr、Eu和U的影响及地球化学模型评价","authors":"Tiziana Missana, Miguel García-Gutiérrez","doi":"10.1016/j.apgeochem.2023.105811","DOIUrl":null,"url":null,"abstract":"<div><p>The presence of organic ligands may exacerbate the mobility of contaminants by stabilizing them in the aqueous phase and reducing their retention on the solid phases, representing an additional environmental hazard.</p><p>We investigated the impact of EDTA, citrate and phthalate on the adsorption of four different radionuclides (RN = <sup>137</sup>Cs, <sup>85</sup>Sr, <sup>152</sup>Eu and <sup>233</sup>U) by a well-characterized smectite clay and evaluated the capability of sorption modeling to incorporate the impact of these organic ligands.</p><p>We analyzed the effect of ligand concentration (from 1·10<sup>−6</sup> to 1·10<sup>−3</sup> M) on RN retention at two different pH values (approximately 5 and 9) to contemplate the occurrence of different adsorption mechanisms in clays (cation exchange or surface complexation) as well as the RN and organic speciation.</p><p>The results suggested that phthalate had a minimal effect on the retention of the studied RNs, while EDTA and citrate significantly decreased the adsorption of Eu, Sr and U, even making it drop to zero in some cases. The simulation outcomes demonstrated that, in most cases, the variation in the distribution coefficient (<em>K</em><sub>d</sub>) as a function of the organic concentration could be accurately replicated with the available thermodynamic data, but few relevant discrepancies were identified.</p><p>The importance of the possible competitive effects of trace ions in the equilibrium water (notably Ca) for the overall assessment of the role of organic matter on RN retention was highlighted.</p></div>","PeriodicalId":8064,"journal":{"name":"Applied Geochemistry","volume":"159 ","pages":"Article 105811"},"PeriodicalIF":3.1000,"publicationDate":"2023-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Role of EDTA, citrate and phthalate on Cs, Sr, Eu and U adsorption by smectite and evaluation by geochemical modeling\",\"authors\":\"Tiziana Missana, Miguel García-Gutiérrez\",\"doi\":\"10.1016/j.apgeochem.2023.105811\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>The presence of organic ligands may exacerbate the mobility of contaminants by stabilizing them in the aqueous phase and reducing their retention on the solid phases, representing an additional environmental hazard.</p><p>We investigated the impact of EDTA, citrate and phthalate on the adsorption of four different radionuclides (RN = <sup>137</sup>Cs, <sup>85</sup>Sr, <sup>152</sup>Eu and <sup>233</sup>U) by a well-characterized smectite clay and evaluated the capability of sorption modeling to incorporate the impact of these organic ligands.</p><p>We analyzed the effect of ligand concentration (from 1·10<sup>−6</sup> to 1·10<sup>−3</sup> M) on RN retention at two different pH values (approximately 5 and 9) to contemplate the occurrence of different adsorption mechanisms in clays (cation exchange or surface complexation) as well as the RN and organic speciation.</p><p>The results suggested that phthalate had a minimal effect on the retention of the studied RNs, while EDTA and citrate significantly decreased the adsorption of Eu, Sr and U, even making it drop to zero in some cases. The simulation outcomes demonstrated that, in most cases, the variation in the distribution coefficient (<em>K</em><sub>d</sub>) as a function of the organic concentration could be accurately replicated with the available thermodynamic data, but few relevant discrepancies were identified.</p><p>The importance of the possible competitive effects of trace ions in the equilibrium water (notably Ca) for the overall assessment of the role of organic matter on RN retention was highlighted.</p></div>\",\"PeriodicalId\":8064,\"journal\":{\"name\":\"Applied Geochemistry\",\"volume\":\"159 \",\"pages\":\"Article 105811\"},\"PeriodicalIF\":3.1000,\"publicationDate\":\"2023-10-22\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Applied Geochemistry\",\"FirstCategoryId\":\"89\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0883292723002561\",\"RegionNum\":3,\"RegionCategory\":\"地球科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"GEOCHEMISTRY & GEOPHYSICS\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Applied Geochemistry","FirstCategoryId":"89","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0883292723002561","RegionNum":3,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"GEOCHEMISTRY & GEOPHYSICS","Score":null,"Total":0}
Role of EDTA, citrate and phthalate on Cs, Sr, Eu and U adsorption by smectite and evaluation by geochemical modeling
The presence of organic ligands may exacerbate the mobility of contaminants by stabilizing them in the aqueous phase and reducing their retention on the solid phases, representing an additional environmental hazard.
We investigated the impact of EDTA, citrate and phthalate on the adsorption of four different radionuclides (RN = 137Cs, 85Sr, 152Eu and 233U) by a well-characterized smectite clay and evaluated the capability of sorption modeling to incorporate the impact of these organic ligands.
We analyzed the effect of ligand concentration (from 1·10−6 to 1·10−3 M) on RN retention at two different pH values (approximately 5 and 9) to contemplate the occurrence of different adsorption mechanisms in clays (cation exchange or surface complexation) as well as the RN and organic speciation.
The results suggested that phthalate had a minimal effect on the retention of the studied RNs, while EDTA and citrate significantly decreased the adsorption of Eu, Sr and U, even making it drop to zero in some cases. The simulation outcomes demonstrated that, in most cases, the variation in the distribution coefficient (Kd) as a function of the organic concentration could be accurately replicated with the available thermodynamic data, but few relevant discrepancies were identified.
The importance of the possible competitive effects of trace ions in the equilibrium water (notably Ca) for the overall assessment of the role of organic matter on RN retention was highlighted.
期刊介绍：
Applied Geochemistry is an international journal devoted to publication of original research papers, rapid research communications and selected review papers in geochemistry and urban geochemistry which have some practical application to an aspect of human endeavour, such as the preservation of the environment, health, waste disposal and the search for resources. Papers on applications of inorganic, organic and isotope geochemistry and geochemical processes are therefore welcome provided they meet the main criterion. Spatial and temporal monitoring case studies are only of interest to our international readership if they present new ideas of broad application.
Topics covered include: (1) Environmental geochemistry (including natural and anthropogenic aspects, and protection and remediation strategies); (2) Hydrogeochemistry (surface and groundwater); (3) Medical (urban) geochemistry; (4) The search for energy resources (in particular unconventional oil and gas or emerging metal resources); (5) Energy exploitation (in particular geothermal energy and CCS); (6) Upgrading of energy and mineral resources where there is a direct geochemical application; and (7) Waste disposal, including nuclear waste disposal.
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