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Gamma Radiolysis of Phenyl-Substituted TODGAs: Part I 苯基取代TODGAs的γ辐射分解:第一部分
IF 2 4区 化学 Q3 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2023-07-29 DOI: 10.1080/07366299.2023.2220765
C. Zarzana, J. McAlpine, A. Wilden, Michelle Hupert, Andrea Stärk, M. Iqbal, W. Verboom, B. Mincher, G. Groenewold, G. Modolo
ABSTRACT The radiolytic stabilities of three phenylated analogs of N,N,N’,N’-tetraoctyl diglycolamide (TODGA) were investigated: 2-(2-(di-n-octylamino)-2-oxoethoxy)-N,N-di-n-octyl-2-phenylacetamide (PhTODGA), which has a phenyl substituent bound to a central methylene, 2-(2-(di-n-octylamino)-2-oxo-1-phenylethoxy)-N,N-di-n-octylpropanamide (PhMeTODGA), which also contains a methyl substituent bound to the methylene on the other side of the ether moiety, and, 2-(2-N-n-hexyl-N-phenylamino)-2-oxoethoxy)-N-n-hexyl-N-phenylacetamide (DHDPDGA), which has phenyl substituents located on the amide groups instead of the central methylenes. The objective of Part I of this series of papers covers was to evaluate the contribution of the phenyl group to the radiolytic stability of these diglycolamides when irradiated in a) n-dodecane, and b) n-dodecane in the presence of a nitric acid-containing aqueous phase. The results indicate that the presence of the phenyl group decreases the overall radiolytic stability compared to unsubstituted TODGA. However, the results also indicate that the phenyl groups interact with nitric acid in a cooperative fashion that enhances the radiation stability of the phenylated diglycolamide (DGA) derivatives in the presence of a nitric acid-containing aqueous phase compared to irradiation in only n-dodecane. The results are consistent with the hypothesized formation of nitric acid-phenylated DGA complexes in the n-dodecane phase that are significantly more stable with respect to gamma irradiation, compared to the phenylated DGA molecules alone.
摘要研究了N,N,N’,N’-四辛基二甘醇酰胺(TODGA)的三种苯基化类似物的辐解稳定性:2-(二正辛基氨基)-2-氧代乙氧基)-N,N-二正辛基-2-苯基乙酰胺(PhTODGA),其具有与中心亚甲基结合的苯基取代基,其还包含在醚部分的另一侧与亚甲基结合的甲基取代基,以及2-(2-N-正己基-N-苯基氨基)-2-氧代乙氧基)-N-正己基-N-N-苯基乙酰胺(DHDPDGA),其具有位于酰胺基团而不是中心亚甲基上的苯基取代基。本系列论文第一部分的目的是评估当在a)正十二烷和b)正十二烷基中,在含硝酸的水相存在下辐照时,苯基对这些二甘醇酰胺的辐解稳定性的贡献。结果表明,与未取代的TODGA相比,苯基的存在降低了总的辐解稳定性。然而,结果也表明,与仅在正十二烷中照射相比,苯基以协同方式与硝酸相互作用,增强了苯基化二甘醇酰胺(DGA)衍生物在含硝酸水相存在下的辐射稳定性。结果与假设的在正十二烷相中形成的硝酸-苯基化DGA复合物一致,与单独的苯基化DGA分子相比,该复合物相对于伽马辐射明显更稳定。
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引用次数: 1
Investigation of f-Element Interactions with Functionalized Diamides of Phenanthroline-Based Ligands f元素与菲咯啉基配体功能化二酰胺相互作用的研究
IF 2 4区 化学 Q3 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2023-07-28 DOI: 10.1080/07366299.2023.2239866
Emma M. Archer, Shane S. Galley, J. Jackson, J. Shafer
ABSTRACT Separations relevant to trivalent actinides and lanthanides have been a focus of the f-element community in the past few decades. A central focus of this effort has been optimizing ligands for separations. From a fundamental perspective, one must investigate the metal–ligand interactions for optimal ligand design. A well-explored class of ligands, phenanthroline diamides, is reviewed to further elucidate the actinide or lanthanide–ligand interactions of primarily Am3+, Cm3+, and Eu3+. Mixed nitrogen and oxygen donors of this nature are of interest to explore due to their increased selectivity for the trivalent actinides over the trivalent lanthanides. Phenanthroline diamide ligands have shown to have promise in industrial-scale separations compared to bipyridine and pyridine diamide ligands with larger selectivity for the trivalent actinides. These interactions are studied through solvent extraction, spectroscopic, and thermodynamic techniques. Further analysis provided in this review includes an overview of the computational results provided and relevant comparisons to experimental data. The computational parameters considered are the calculated bond lengths, thermodynamic parameters, and values that provide insight to a discussion of covalent interactions between metal and ligand. The information provided is important to benchmark the state-of-the-art basic, applied, and computational chemistry of the phenanthroline diamide class of ligands. GRAPHICAL ABSTRACT
在过去的几十年里,与三价锕系元素和镧系元素相关的分离一直是f元素界关注的焦点。这项工作的中心焦点是优化用于分离的配体。从基本的角度来看,必须研究金属-配体的相互作用,以优化配体设计。综述了一类研究得很好的配体,菲咯啉二酰胺,以进一步阐明主要是Am3+、Cm3+和Eu3+的锕系元素或镧系元素-配体相互作用。这种性质的混合氮和氧供体值得探索,因为它们对三价锕系元素的选择性高于三价镧系元素。与对三价锕系元素具有更大选择性的联吡啶和吡啶二酰胺配体相比,菲罗啉二酰胺配体在工业规模的分离中显示出前景。通过溶剂萃取、光谱和热力学技术研究了这些相互作用。本综述中提供的进一步分析包括对所提供的计算结果的概述以及与实验数据的相关比较。所考虑的计算参数是计算出的键长、热力学参数和为讨论金属和配体之间的共价相互作用提供见解的值。所提供的信息对于菲咯啉二酰胺类配体的最新基础、应用和计算化学的基准测试非常重要。图形摘要
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引用次数: 0
Selective Extraction of Cu (II) Using Novel C=O–NOH-Contained Compound-Dodecyl Phenyl Ethyl Hydroxamic Acid and Its Extraction Mechanism 新型含C= o - noh化合物-十二烷基苯基乙基羟肟酸选择性萃取铜(II)及其萃取机理
IF 2 4区 化学 Q3 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2023-07-25 DOI: 10.1080/07366299.2023.2229888
D. Cao, Shuai Wang, Xin Ma, Jia Yang, Hong Zhong
ABSTRACT Herein, a novel C=O–NOH-contained compound was synthesized and used in the extraction and recovery of copper from sulfate solution. Dodecyl phenyl ethyl hydroxamic acid (DPEHA) exhibited high selectivity to Cu(II) over the competing ions, and the separation factors (β) obtained were β Cu/Zn = 227.370, β Cu/Co = 199.094, β Cu/Ni = 188.889, respectively. The separation effect was stronger than that of 2-hydroxy-5-nonyl acetophenone oxime. Meanwhile, extraction capacity of 0.10 g Cu(II) per gram DPEHA was reached, and the extracted Cu(II) can be stripped effectively. The investigation of extraction mechanism revealed that O atoms in C=O and O-H groups of DPEHA operate as active sites, which could powerfully chelate with Cu(II) by forming stable five-membered rings. The high copper extraction efficiency and selectivity associated with a simple synthesis of DPEHA make it to serve as the potential selective Cu(II) extractant, which also provide a novel insight for the research and development of economical Cu(II) extractants. Graphical Abstract
摘要本文合成了一种新型含C= o - noh化合物,并将其用于硫酸盐溶液中铜的提取和回收。十二烷基苯基乙基羟肟酸(DPEHA)对Cu(II)具有较高的选择性,得到的分离因子(β)分别为β Cu/Zn = 227.370, β Cu/Co = 199.094, β Cu/Ni = 188.889。分离效果优于2-羟基-5-壬基苯乙酮肟。同时,每g DPEHA萃取量为0.10 g Cu(II),萃取后的Cu(II)可以有效剥离。萃取机理研究表明,DPEHA的C=O和O- h基团中的O原子作为活性位点,能与Cu(II)形成稳定的五元环进行强螯合。DPEHA具有较高的铜萃取效率和选择性,且合成简单,可作为铜(II)的选择性萃取剂,这也为经济型铜(II)萃取剂的研究和开发提供了新的思路。图形抽象
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引用次数: 0
Reliable Identification of Relevant Factors for the Reactive Extraction of Succinic Acid from Electrolyte Containing Solutions 从含电解质溶液中反应萃取琥珀酸相关因素的可靠鉴定
IF 2 4区 化学 Q3 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2023-07-24 DOI: 10.1080/07366299.2023.2221708
M. Gausmann, Diana Wall, A. Jupke
ABSTRACT Reactive extraction of succinic acid by tertiary amines is an effective separation technique. Its potential application for the initial recovery of bio-based succinic acid from fermentation broth. However, the co-extraction of inorganic anions significantly impairs the extraction performance. In this study, we use a statistically backed design of experiments method (DoE) to screen and identify the factors with a significant effect and relevant impact on extraction yield and selectivity. Eight operational factors (Extractant, solvent, succinic acid concentration, amine concentration, initial pH, the type of anion, electrolyte concentration, and temperature) were screened by applying an orthogonal design plan for the experiments. The choice of the extractant and diluent as well as the type of anion had the most significant effect on the extraction yield. In contrast, the selectivity was mainly affected by the concentration ratios of succinic acid and electrolyte. The screening plan reduced the number of experiments from 1728 possible combinations to 72 experiments required to identify the factors while maintaining the significance of the identified effects. We suggest competing mass-action relationships between the pH-dependent protonation of amines and the complexation of succinic acid to explain the observed trends. Graphical abstract
叔胺反应萃取琥珀酸是一种有效的分离技术。它在从发酵液中初步回收生物基琥珀酸方面的潜在应用。然而,无机阴离子的共萃取显著削弱了萃取性能。在本研究中,我们使用统计支持的实验设计方法(DoE)来筛选和确定对提取产率和选择性有显著影响和相关影响的因素。采用正交设计方案筛选了8个操作因素(萃取剂、溶剂、琥珀酸浓度、胺浓度、初始pH、阴离子类型、电解质浓度和温度)进行实验。萃取剂和稀释剂的选择以及阴离子的类型对萃取收率的影响最为显著。相反,选择性主要受琥珀酸和电解质的浓度比的影响。筛选计划将实验数量从1728个可能的组合减少到72个实验,以确定因素,同时保持已确定影响的显著性。我们提出了胺的pH依赖性质子化和琥珀酸的络合之间的竞争性质量作用关系,以解释观察到的趋势。图形摘要
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引用次数: 0
Gamma Radiolysis of Phenyl-Substituted TODGAs: Part II 苯基取代TODGAs的γ辐射分解:第二部分
IF 2 4区 化学 Q3 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2023-07-06 DOI: 10.1080/07366299.2023.2221290
C. Zarzana, J. McAlpine, A. Wilden, Michelle Hupert, Andrea Stärk, M. Iqbal, W. Verboom, B. Mincher, G. Groenewold, G. Modolo
ABSTRACT The radiolytic degradation chemistry of three phenylated analogs of N,N,N’,N’-tetraoctyl diglycolamide (TODGA) was investigated: 2-(2-(di-n-octylamino)-2-oxoethoxy)-N,N-di-n-octyl-2-phenylacetamide (PhTODGA), which has a phenyl substituent bound to a central methylene, 2-(2-(di-n-octylamino)-2-oxo-1-phenylethoxy)-N,N-di-n-octylpropanamide (PhMeTODGA), which also contains a methyl substituent bound to the methylene on the other side of the ether moiety, and, 2-(2-N-n-hexyl-N-phenylamino)-2-oxoethoxy)-N-n-hexyl-N-phenylacetamide (DHDPDGA), which has phenyl substituents located on the amide groups instead of the central methylenes. In Part II of this series of papers radiolytic degradation products were identified after separation with liquid chromatography by High Resolution, Accurate-Mass mass spectrometry and collision-induced dissociation. At least twenty-two radiolytic degradation products were identified for PhTODGA, twenty-nine for PhMeTODGA, and over three dozen for DHDPDGA. The suite of radiolytic degradation products of these three investigated ligands was significantly larger than has been reported for previously studied diglycolamides, owing to their asymmetric nature, and to the identification of several new degradation mechanisms, including addition of methyl, hydroxyl, and nitrogen oxide radicals, that have not been previously reported for diglycolamides. Degradation products that contained addition of a NO2 or NO3 group were particularly prevalent for DHDPDGA, likely due to the phenyl side-groups. Several of these newly observed mechanisms do not appear to depend on the presence of the phenyl groups, suggesting these novel mechanisms may apply to other diglycolamides
研究了三种苯基化N,N,N ',N ' -四辛基二甘醇酰胺(TODGA)的辐射降解化学性质。2-(2-(二-正辛胺)-2-氧乙氧基)- n, n-二-正辛基-2-苯乙醯乙酰胺(PhTODGA),它有一个苯基取代基与中心亚甲基结合,2-(二-正辛胺)-2-氧-1-苯乙氧基)- n, n-二-正辛基-2-苯乙醯丙酰胺(PhMeTODGA),它也含有一个甲基取代基与醚部分另一侧的亚甲基结合,以及2-(2- n-正己基-n-苯基苯基)-2-正己基-n-苯基乙醯乙酰胺(DHDPDGA)。苯基取代基位于酰胺基上而不是中间的亚甲基上。在本系列论文的第二部分中,通过液相色谱、高分辨率、精确质谱和碰撞诱导解离分离,对辐射降解产物进行了鉴定。PhTODGA至少鉴定出22种放射性降解产物,PhMeTODGA鉴定出29种,DHDPDGA鉴定出超过36种。由于这三种配体的不对称性质,以及发现了几种新的降解机制,包括甲基自由基、羟基自由基和氮氧化物自由基的加入,这在以前的二糖酰胺研究中没有报道过,因此这三种配体的辐射降解产物明显大于先前报道的二糖酰胺。含有NO2或NO3基团的降解产物对DHDPDGA尤其普遍,可能是由于苯基侧基。这些新观察到的机制中的一些似乎并不依赖于苯基的存在,这表明这些新的机制可能适用于其他二醇酰胺
{"title":"Gamma Radiolysis of Phenyl-Substituted TODGAs: Part II","authors":"C. Zarzana, J. McAlpine, A. Wilden, Michelle Hupert, Andrea Stärk, M. Iqbal, W. Verboom, B. Mincher, G. Groenewold, G. Modolo","doi":"10.1080/07366299.2023.2221290","DOIUrl":"https://doi.org/10.1080/07366299.2023.2221290","url":null,"abstract":"ABSTRACT The radiolytic degradation chemistry of three phenylated analogs of N,N,N’,N’-tetraoctyl diglycolamide (TODGA) was investigated: 2-(2-(di-n-octylamino)-2-oxoethoxy)-N,N-di-n-octyl-2-phenylacetamide (PhTODGA), which has a phenyl substituent bound to a central methylene, 2-(2-(di-n-octylamino)-2-oxo-1-phenylethoxy)-N,N-di-n-octylpropanamide (PhMeTODGA), which also contains a methyl substituent bound to the methylene on the other side of the ether moiety, and, 2-(2-N-n-hexyl-N-phenylamino)-2-oxoethoxy)-N-n-hexyl-N-phenylacetamide (DHDPDGA), which has phenyl substituents located on the amide groups instead of the central methylenes. In Part II of this series of papers radiolytic degradation products were identified after separation with liquid chromatography by High Resolution, Accurate-Mass mass spectrometry and collision-induced dissociation. At least twenty-two radiolytic degradation products were identified for PhTODGA, twenty-nine for PhMeTODGA, and over three dozen for DHDPDGA. The suite of radiolytic degradation products of these three investigated ligands was significantly larger than has been reported for previously studied diglycolamides, owing to their asymmetric nature, and to the identification of several new degradation mechanisms, including addition of methyl, hydroxyl, and nitrogen oxide radicals, that have not been previously reported for diglycolamides. Degradation products that contained addition of a NO2 or NO3 group were particularly prevalent for DHDPDGA, likely due to the phenyl side-groups. Several of these newly observed mechanisms do not appear to depend on the presence of the phenyl groups, suggesting these novel mechanisms may apply to other diglycolamides","PeriodicalId":22002,"journal":{"name":"Solvent Extraction and Ion Exchange","volume":"41 1","pages":"582 - 605"},"PeriodicalIF":2.0,"publicationDate":"2023-07-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"44118557","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 1
Selective Separation of Zr(IV) from Simulated High-Level Liquid Wastes by Zeolites 沸石从模拟高放废液中选择性分离Zr(IV
IF 2 4区 化学 Q3 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2023-07-04 DOI: 10.1080/07366299.2023.2231493
Yifu Hu, Wenfeng Hao, Wentao Wang, Ye Zhang, Qi Chen, Wenfu Yan, T. Yan
ABSTRACT Effectively separating Zr(IV) from strong acidic and radioactive solutions is crucial for spent fuel reprocessing plants, but it remains a challenging task. This study investigated the adsorption of Zr(IV) in HNO3 solutions using zeolites as adsorbents. The zeolites were characterized by X-ray diffraction (XRD),scanning electron microscopy (SEM), transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS). The effects of adsorption time, HNO3 concentration, the initial concentration of Zr(IV), zeolites dosage, and temperature on the Zr(IV) adsorption behaviors were investigated. The results demonstrated that HY zeolite had a higher adsorption capacity for Zr(IV) than H-SSZ-13 zeolite. The adsorption capacity of HY zeolite was influenced by its Si/Al ratio, which determined the density of adsorption sites. The optimal HY zeolite (HY-25) exhibited a maximum adsorption capacity of 30.438 mg/g in 3 M HNO3 solution. Furthermore, the adsorption isotherms and kinetics of Zr(IV) adsorption were investigated. The adsorption of Zr(IV) on zeolites was endothermic and spontaneous, in accordance with the Freundlich’s isotherm model and pseudo-second-order kinetic model. In a simulated strong acidic solution of Zr(IV) and 10 co-existing cations (Ag+, Ba2+, Cs+, Ce3+, Eu3+, Fe3+, La3+, Nd3+, Sm3+, Sr2+), HY-25 exhibited good selective adsorption of Zr(IV), indicating its potential application in the treatment of high-level radioactive liquid waste.
摘要从强酸和强放射性溶液中有效分离Zr(IV)对乏燃料后处理厂至关重要,但这仍然是一项具有挑战性的任务。本研究以沸石为吸附剂,研究了Zr(IV)在HNO3溶液中的吸附。用X射线衍射(XRD)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)和X射线光电子能谱(XPS)对沸石进行了表征。研究了吸附时间、HNO3浓度、Zr(IV)的初始浓度、沸石用量和温度对Zr(Ⅳ)吸附行为的影响。结果表明,HY沸石对Zr(IV)的吸附能力高于H-SSZ-13沸石。HY沸石的吸附容量受其Si/Al比的影响,Si/Al比值决定了吸附位点的密度。最佳HY沸石(HY-25)的最大吸附量为30.438 mg/g,3 M HNO3溶液。此外,还研究了Zr(IV)的吸附等温线和吸附动力学。根据Freundlich等温线模型和拟二阶动力学模型,Zr(IV)在沸石上的吸附是吸热和自发的。在Zr(IV)和10种共存阳离子(Ag+、Ba2+、Cs+、Ce3+、Eu3+、Fe3+、La3+、Nd3+、Sm3+、Sr2+)的模拟强酸溶液中,HY-25对Zr(Ⅳ)表现出良好的选择性吸附,表明其在高放射性废液处理中具有潜在的应用前景。
{"title":"Selective Separation of Zr(IV) from Simulated High-Level Liquid Wastes by Zeolites","authors":"Yifu Hu, Wenfeng Hao, Wentao Wang, Ye Zhang, Qi Chen, Wenfu Yan, T. Yan","doi":"10.1080/07366299.2023.2231493","DOIUrl":"https://doi.org/10.1080/07366299.2023.2231493","url":null,"abstract":"ABSTRACT Effectively separating Zr(IV) from strong acidic and radioactive solutions is crucial for spent fuel reprocessing plants, but it remains a challenging task. This study investigated the adsorption of Zr(IV) in HNO3 solutions using zeolites as adsorbents. The zeolites were characterized by X-ray diffraction (XRD),scanning electron microscopy (SEM), transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS). The effects of adsorption time, HNO3 concentration, the initial concentration of Zr(IV), zeolites dosage, and temperature on the Zr(IV) adsorption behaviors were investigated. The results demonstrated that HY zeolite had a higher adsorption capacity for Zr(IV) than H-SSZ-13 zeolite. The adsorption capacity of HY zeolite was influenced by its Si/Al ratio, which determined the density of adsorption sites. The optimal HY zeolite (HY-25) exhibited a maximum adsorption capacity of 30.438 mg/g in 3 M HNO3 solution. Furthermore, the adsorption isotherms and kinetics of Zr(IV) adsorption were investigated. The adsorption of Zr(IV) on zeolites was endothermic and spontaneous, in accordance with the Freundlich’s isotherm model and pseudo-second-order kinetic model. In a simulated strong acidic solution of Zr(IV) and 10 co-existing cations (Ag+, Ba2+, Cs+, Ce3+, Eu3+, Fe3+, La3+, Nd3+, Sm3+, Sr2+), HY-25 exhibited good selective adsorption of Zr(IV), indicating its potential application in the treatment of high-level radioactive liquid waste.","PeriodicalId":22002,"journal":{"name":"Solvent Extraction and Ion Exchange","volume":"41 1","pages":"767 - 788"},"PeriodicalIF":2.0,"publicationDate":"2023-07-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"42618838","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
A Comparison Between Trioctylamine (TOA) and Tris(2-Ethylhexyl) Amine (TEHA) in Solvent Extraction of Sulfuric Acid* 三辛基胺(TOA)和三(2-乙基己基)胺(TEHA)在硫酸溶剂萃取中的比较*
IF 2 4区 化学 Q3 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2023-06-21 DOI: 10.1080/07366299.2023.2225067
A. Heidari, S. Shahini, Davoud Haghshenas Fatmehsari, E. Keshavarz Alamdari
ABSTRACT The study investigated the behavior of two amines, Trioctylamine (TOA) and Tris(2-Ethylhexyl) amine (TEHA), in the sulfuric acid extraction system, with varying concentrations of extractants and modifiers, as well as the temperature of the sulfuric acid extraction. The study found that TOA had a higher ability in the extraction of sulfuric acid and was less dependent on temperature. However, an increase in the initial sulfuric acid concentration resulted in a drop in acid extraction percentage when TOA was employed, while such a drop was not observed in the case of TEHA. The study also illustrated the necessity of using Octanol as a modifier, with different minimum levels required for TOA and TEHA. Additionally, Octanol showed a positive effect on the extraction level of sulfuric acid in the TEHA – H2SO4 extraction system, which can be considered an advantage in the facile stripping of the loaded organic phase. The slope analysis method revealed that more than 1 mol of TOA is necessary to extract 1 mol of sulfuric acid, while 1 mol of TEHA can absorb 2 mol of sulfuric acid. FTIR spectra analysis confirmed TOA's participation in the extraction of sulfuric acid and provided insights into the chemical bonds formed. Overall, the study provides a comprehensive understanding of the solvent extraction of sulfuric acid and can be useful in optimizing the extraction process for industrial applications.
摘要研究了三辛基胺(TOA)和三(2-乙基己基)胺(TEHA)两种胺在硫酸萃取体系中的行为,考察了不同浓度的萃取剂和改性剂以及硫酸萃取温度。研究发现,TOA对硫酸的萃取能力较高,对温度的依赖性较小。然而,当使用TOA时,初始硫酸浓度的增加导致酸提取百分比的下降,而在TEHA的情况下没有观察到这种下降。该研究还说明了使用辛醇作为改性剂的必要性,TOA和TEHA需要不同的最低水平。此外,辛醇对TEHA–H2SO4萃取系统中硫酸的萃取水平有积极影响,这可以被认为是容易汽提负载有机相的优势。斜率分析法表明,提取1摩尔硫酸需要超过1摩尔的TOA,而1摩尔的TEHA可以吸收2摩尔的硫酸。FTIR光谱分析证实了TOA参与硫酸的提取,并提供了对所形成化学键的深入了解。总的来说,该研究提供了对硫酸溶剂萃取的全面了解,并有助于优化工业应用的萃取工艺。
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引用次数: 0
Adsorptive Removal of Selenium(IV) from Aqueous Solution by Ferrous Hydroxide Complex-Zero Nickel Composites 氢氧化亚铁络合物-零镍复合材料吸附去除水溶液中的硒(IV)
IF 2 4区 化学 Q3 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2023-05-31 DOI: 10.1080/07366299.2023.2218918
Yan Du, Qing Zhou, Jiankun Zhao, Hexi Wu, Xiaoyan Li, Yibao Liu, Z. Le
ABSTRACT Nanoscale ferrous hydroxide complex-zero nickel composites (FHC/Ni0) were fabricated by ball milling method for Se(IV) adsorption from aqueous solution. The effects of pH, solid-liquid ratio, time, temperature, initial concentration of Se(IV) on the adsorption of Se(IV) by FHC/Ni0 were investigated. FHC/Ni0 was characterized by SEM, XPS, XRD, FT-IR, BET and Zeta potential, and the mechanism of removing Se(IV) was analyzed. The results showed that FHC/Ni0 had a good removal effect on Se(IV). When pH was 5.0, the solid-liquid ratio was 0.15 g L−1, the reaction time was 40 min, the maximum adsorption capacity of Se(IV) by FHC/Ni0 could reach 216 mg g−1. The pseudo-second-order kinetic model and Langmuir had a good fit for the Se(IV) adsorption process of FHC/Ni0, indicating that the monolayer and chemical adsorption played a leading role in the adsorption process. XPS analysis further confirmed that the adsorption of Se on FHC/Ni0 was mainly due to the formation of stable complexes with a large number of functional groups containing Fe, Ni and S, meanwhile, the removal of Se(IV) by the material is achieved through a combination of chemical adsorption and reduction reactions. The research results can demonstrate the feasibility of FHC/Ni0 in Se(IV) removal and provide a theoretical basis for the treatment of wastewater containing Se(IV).
采用球磨法制备了纳米级氢氧化铁-零镍复合材料(FHC/Ni0),并对Se(IV)进行了吸附。考察了pH、料液比、时间、温度、初始浓度对FHC/Ni0吸附Se(IV)的影响。采用SEM、XPS、XRD、FT-IR、BET和Zeta电位对FHC/Ni0进行了表征,并对其去除Se(IV)的机理进行了分析。结果表明,FHC/Ni0对Se(IV)有较好的去除效果。当pH = 5.0,料液比为0.15 g L−1,反应时间为40 min时,FHC/Ni0对Se(IV)的最大吸附量可达216 mg g−1。拟二级动力学模型和Langmuir对FHC/Ni0的Se(IV)吸附过程拟合较好,说明在吸附过程中,单层吸附和化学吸附起主导作用。XPS分析进一步证实了Se在FHC/Ni0上的吸附主要是由于与大量含Fe、Ni和S的官能团形成稳定的配合物,同时材料对Se(IV)的去除是通过化学吸附和还原反应相结合的方式实现的。研究结果验证了FHC/Ni0去除Se(IV)的可行性,为含Se废水的处理提供了理论依据。
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引用次数: 1
Extraction of Neptunium, Plutonium, Americium, Zirconium, and Technetium by Di-(2-Ethylhexyl)-Iso-Butyramide (DEHiBA) at High Metal Loadings 高金属负荷双-(2-乙基己基)-异丁胺(DEHiBA)萃取镎、钚、镅、锆和锝
IF 2 4区 化学 Q3 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2023-05-26 DOI: 10.1080/07366299.2023.2215833
G. Hall, N. Bessen, P. Zalupski, Emily L. Campbell, T. Grimes, D. Peterman, G. Lumetta
ABSTRACT Increased focus on carbon neutral energy has generated a resurgence of interest in nuclear power, and in particular advanced reactors which are likely to utilize high assay low enriched uranium (HALEU). This in turn could increase the economic attractiveness of recovering still partially enriched uranium from used nuclear fuel. Concomitant to development of advanced reactors, advanced reprocessing schemes should be developed which address the disadvantages to well established reprocessing schemes. The present study focuses on using di-(2-ethylhexyl)-iso-butyramide (DEHiBA) under high metal loading conditions for the reprocessing of used nuclear fuel. The elements examined in the study include the dominant transuranic actinides (Np, Pu, Am) as well as the often-problematic Tc and Zr. By increasing the concentration of the extractant from the more commonly reported 1.0 M – 1.5 M, the extraction of hexavalent actinides is substantially increased, while maintaining effective rejection of tri, tetra, and pentavalent actinides, particularly in the presence of high loadings of uranium. The extraction of Zr by 1.5 M DEHiBA is noted to be negligible by comparison to tributyl phosphate (TBP), however the coextraction of Tc with U is observed to be nominally twice the quantity that is extracted by TBP indicating a need for effective Tc management.
对碳中和能源的日益关注已经引起了人们对核能,特别是可能使用高含量低浓缩铀(HALEU)的先进反应堆的兴趣的复苏。这反过来又会增加从乏燃料中回收仍然部分浓缩的铀的经济吸引力。在发展先进反应堆的同时,应开发先进的后处理方案,以解决现有后处理方案的缺点。研究了在高金属负荷条件下使用二-(2-乙基己基)-异丁酰胺(DEHiBA)进行乏燃料后处理的方法。研究中检查的元素包括主要的超铀锕系元素(Np, Pu, Am)以及经常出现问题的Tc和Zr。通过增加萃取剂的浓度,从更常见的1.0 M - 1.5 M,六价锕系元素的萃取量大大增加,同时保持有效的拒绝三,四,和五价锕系元素,特别是在存在高铀负荷的情况下。与磷酸三丁酯(TBP)相比,1.5 M DEHiBA对Zr的萃取可以忽略不计,然而,与U的共萃取在名义上是TBP萃取量的两倍,这表明需要有效的Tc管理。
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引用次数: 0
CFD Analysis of Simultaneous Removal of Copper (II) and Zinc from Aqueous Solution Using a Hollow Fiber Membrane Contactor 中空纤维膜接触器同时去除水溶液中铜(II)和锌的CFD分析
IF 2 4区 化学 Q3 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2023-05-26 DOI: 10.1080/07366299.2023.2214589
Borhan Pourtalebi, Mohammad Valibeknejad, S. M. Abdoli, A. Akbari
ABSTRACT The current study is a new method for liquid–liquid extraction of copper (II) and zinc that was carried out using an efficient solvent called trifluoroacetylacetone in a hollow fiber membrane contactor (HFMC). To analyze the extraction process and understand its underlying mechanisms, computational fluid dynamics (CFD) was employed. The extraction was performed in three domains by coupling the mass and momentum equation to express the solute transport from the tube side to the shell side through the membrane in a hollow fiber membrane contactor. The finite element approach simulates the governing equation and validates the results. This work aims to obtain the distribution of copper (II) and zinc by performing a simulation. The effect of some crucial parameters was investigated. The results illustrate that the extraction efficiency increases by increasing the partition coefficient and decreasing the flow rate on the tube side. Also, the temperature significantly affects extraction, and by enhancing the temperature from 298 to 313 K, the efficiency increases by 12% for copper (II) and 6.6% for zinc. Furthermore, the membrane porosity was found to be another influential parameter. By increasing the membrane porosity of 25% to 90%, the efficiency increases to 95% for copper (II) and 98% for zinc.
摘要本研究是一种在中空纤维膜接触器(HFMC)中使用一种名为三氟乙酰丙酮的高效溶剂进行液-液萃取铜(II)和锌的新方法。为了分析提取过程并了解其潜在机制,采用了计算流体动力学(CFD)。通过耦合质量和动量方程,在三个域中进行萃取,以表达溶质在中空纤维膜接触器中通过膜从管侧到壳侧的传输。有限元方法模拟了控制方程,并验证了结果。本工作旨在通过模拟获得铜(II)和锌的分布。研究了一些关键参数的影响。结果表明,提高分配系数和降低管侧流量可以提高萃取效率。此外,温度显著影响萃取,通过将温度从298 K提高到313 K,铜(II)的效率提高了12%,锌的效率增加了6.6%。此外,发现膜孔隙率是另一个有影响的参数。通过将膜孔隙率提高25%至90%,铜(II)的效率提高至95%,锌的效率提高到98%。
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Solvent Extraction and Ion Exchange
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