Pub Date : 2023-04-05DOI: 10.1080/07366299.2023.2193592
Satyabrata Mishra, N. Desigan, K. A. Venkatesan, K. Ananthasivan
ABSTRACT The degradation behavior of gamma irradiated solution of 1.1 M tri-butyl phosphate (TBP) in n-dodecane (n-DD) and 1.1 M tri-iso-amyl phosphate (TiAP) in n-DD loaded with nitric acid and uranium were compared up to 5 cycles upon recycling of the degraded solvent after 80 kGy in each cycle. The solvent was recycled by stripping the loaded metal with dilute nitric acid followed by alkali wash using sodium carbonate after each cycle. Subsequently, the physico-chemical properties and the metal extraction – retention properties of the recycled solvent were measured. The recycled solvent was analyzed using gas chromatographic and FT-IR spectroscopic analysis. Among the physico-chemical properties the interfacial tension of the recycled solvent decreased drastically after three cycles of irradiation, but the variation in the measured phase separation time was not significant. But, the concentration of the extractant (TBP/TiAP) decreased significantly upon recycling. Though the formation of nitro compounds was obvious from FT-IR analysis, the metal retention by recycled organic phases were comparable after each cycle of irradiation. HIGHLIGHTS Cyclic irradiation behavior of TiAP/n-DD and TBP/n-DD was compared under acid loaded and uranium loaded condition. The number of cycles, the solvent can be reused upon recycling was evaluated. Cyclic irradiation under uranium loading condition leads to degradation of the extractant (TBP/TiAP) to a significant extent as evident from GC-analysis. Accumulation of unwashable degraded products takes place upon recycling based on FT-IR analysis. GRAPHICAL ABSTRACT
{"title":"Comparison of Cyclic Irradiation Behavior of Tri-Butyl Phosphate / Tri-Iso-Amyl Phosphate-Dodecane System in Nitric Acid Medium","authors":"Satyabrata Mishra, N. Desigan, K. A. Venkatesan, K. Ananthasivan","doi":"10.1080/07366299.2023.2193592","DOIUrl":"https://doi.org/10.1080/07366299.2023.2193592","url":null,"abstract":"ABSTRACT The degradation behavior of gamma irradiated solution of 1.1 M tri-butyl phosphate (TBP) in n-dodecane (n-DD) and 1.1 M tri-iso-amyl phosphate (TiAP) in n-DD loaded with nitric acid and uranium were compared up to 5 cycles upon recycling of the degraded solvent after 80 kGy in each cycle. The solvent was recycled by stripping the loaded metal with dilute nitric acid followed by alkali wash using sodium carbonate after each cycle. Subsequently, the physico-chemical properties and the metal extraction – retention properties of the recycled solvent were measured. The recycled solvent was analyzed using gas chromatographic and FT-IR spectroscopic analysis. Among the physico-chemical properties the interfacial tension of the recycled solvent decreased drastically after three cycles of irradiation, but the variation in the measured phase separation time was not significant. But, the concentration of the extractant (TBP/TiAP) decreased significantly upon recycling. Though the formation of nitro compounds was obvious from FT-IR analysis, the metal retention by recycled organic phases were comparable after each cycle of irradiation. HIGHLIGHTS Cyclic irradiation behavior of TiAP/n-DD and TBP/n-DD was compared under acid loaded and uranium loaded condition. The number of cycles, the solvent can be reused upon recycling was evaluated. Cyclic irradiation under uranium loading condition leads to degradation of the extractant (TBP/TiAP) to a significant extent as evident from GC-analysis. Accumulation of unwashable degraded products takes place upon recycling based on FT-IR analysis. GRAPHICAL ABSTRACT","PeriodicalId":22002,"journal":{"name":"Solvent Extraction and Ion Exchange","volume":null,"pages":null},"PeriodicalIF":2.0,"publicationDate":"2023-04-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"48586425","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}
Pub Date : 2023-04-03DOI: 10.1080/07366299.2023.2193229
J. Eberz, M. Doeker, Y. Ackermann, Dominik Schaffeld, N. Wierckx, A. Jupke
ABSTRACT The recycling of plastics such as polyurethane (PU) is a current challenge. The continuously increasing production volume and additionally growing end-of-life streams increase the urgency for solutions. Conventional recycling methods such as mechanical and chemical recycling are only economically and/or ecologically suitable to a limited extent. The three-step approach consisting of enzymatic PU decomposition, separation of amines (4,4’-methylenedianiline (MDA), isophoronediamine (IPDA), 2,4-toluenediamine (TDA)) and fermentation of the residual stream is a promising recycling concept. In this study, extraction methods for the separation of MDA and IPDA from an aqueous solution at neutral pH are developed. In addition, the influence of relevant PU hydrolysate components on the amine extraction is investigated. The results show that MDA can be efficiently separated using solvent extraction of 1-octanol. For IPDA separation, a reactive extraction with oleic acid as reactant is developed. The application of these two extraction methods to TDA shows extraction efficiencies of 52% to 86%. The other PU hydrolysate components adipic acid and selected salts have only a minor influence on the extraction efficiency. The diols ethylene glycol and 1,4-butanediol influence the equilibrium pH of IPDA extraction, raising it to higher values. For MDA, no influence of other PU hydrolysate components on the extraction efficiency can be observed. Since amines can have an inhibitory effect on microorganisms, toxicity experiments were carried out to determine the tolerable residual concentration of amines in the raffinate to avoid fermentation inhibition. Growth experiments with Pseudomonas putida KT240 show that MDA has an inhibitory effect at concentrations near the solubility limit, whereas IPDA does not affect growth.
{"title":"Selective Separation of 4,4’-Methylenedianiline, Isophoronediamine and 2,4-Toluenediamine from Enzymatic Hydrolysis Solutions of Polyurethane","authors":"J. Eberz, M. Doeker, Y. Ackermann, Dominik Schaffeld, N. Wierckx, A. Jupke","doi":"10.1080/07366299.2023.2193229","DOIUrl":"https://doi.org/10.1080/07366299.2023.2193229","url":null,"abstract":"ABSTRACT The recycling of plastics such as polyurethane (PU) is a current challenge. The continuously increasing production volume and additionally growing end-of-life streams increase the urgency for solutions. Conventional recycling methods such as mechanical and chemical recycling are only economically and/or ecologically suitable to a limited extent. The three-step approach consisting of enzymatic PU decomposition, separation of amines (4,4’-methylenedianiline (MDA), isophoronediamine (IPDA), 2,4-toluenediamine (TDA)) and fermentation of the residual stream is a promising recycling concept. In this study, extraction methods for the separation of MDA and IPDA from an aqueous solution at neutral pH are developed. In addition, the influence of relevant PU hydrolysate components on the amine extraction is investigated. The results show that MDA can be efficiently separated using solvent extraction of 1-octanol. For IPDA separation, a reactive extraction with oleic acid as reactant is developed. The application of these two extraction methods to TDA shows extraction efficiencies of 52% to 86%. The other PU hydrolysate components adipic acid and selected salts have only a minor influence on the extraction efficiency. The diols ethylene glycol and 1,4-butanediol influence the equilibrium pH of IPDA extraction, raising it to higher values. For MDA, no influence of other PU hydrolysate components on the extraction efficiency can be observed. Since amines can have an inhibitory effect on microorganisms, toxicity experiments were carried out to determine the tolerable residual concentration of amines in the raffinate to avoid fermentation inhibition. Growth experiments with Pseudomonas putida KT240 show that MDA has an inhibitory effect at concentrations near the solubility limit, whereas IPDA does not affect growth.","PeriodicalId":22002,"journal":{"name":"Solvent Extraction and Ion Exchange","volume":null,"pages":null},"PeriodicalIF":2.0,"publicationDate":"2023-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49144906","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}
Pub Date : 2023-03-23DOI: 10.1080/07366299.2023.2188055
V. Babain, M. Alyapyshev, C. Ekberg, T. Todd
ABSTRACT The history of the development of fluorinated compounds as potential diluents in solvent extraction processes is described. Fluorinated diluents were first investigated in the former Soviet Union and later in the United States and Europe. Fluorinated diluents represent a class of compounds that can be used as primary diluents or as phase modifiers. They are of particular utility when extractant solubility is limited in traditional hydrocarbon diluents and a polar diluent is needed. The chemical and physical characterisitics of fluorinated diluents are provided for a broad range of compounds. Other properties such as toxidcity and resistance to radiolysis are described. Fluorinated compounds have been studied for over 40 years and have been used at industrial scale as a primary diluent for cesium and strontium extraction in Russia and as a phase modifer for an insustrial-scale cesium extraction process in the United States. The advantages and disadvantages of traditional hydrocarbon diluents are compared with chlorinated diluents, chlorinated and fluorinated diluents, and a number of different types of fluorinated diluents. Developing trends for teh use of fluorinated diluents in solvent extraction processes are discussed. This article should provide assistance to researchers investigating new or improved solvent extraction processes where traditional hydrocarbon diluents may not be appropriate.
{"title":"Fluorinated Diluents- A Review","authors":"V. Babain, M. Alyapyshev, C. Ekberg, T. Todd","doi":"10.1080/07366299.2023.2188055","DOIUrl":"https://doi.org/10.1080/07366299.2023.2188055","url":null,"abstract":"ABSTRACT The history of the development of fluorinated compounds as potential diluents in solvent extraction processes is described. Fluorinated diluents were first investigated in the former Soviet Union and later in the United States and Europe. Fluorinated diluents represent a class of compounds that can be used as primary diluents or as phase modifiers. They are of particular utility when extractant solubility is limited in traditional hydrocarbon diluents and a polar diluent is needed. The chemical and physical characterisitics of fluorinated diluents are provided for a broad range of compounds. Other properties such as toxidcity and resistance to radiolysis are described. Fluorinated compounds have been studied for over 40 years and have been used at industrial scale as a primary diluent for cesium and strontium extraction in Russia and as a phase modifer for an insustrial-scale cesium extraction process in the United States. The advantages and disadvantages of traditional hydrocarbon diluents are compared with chlorinated diluents, chlorinated and fluorinated diluents, and a number of different types of fluorinated diluents. Developing trends for teh use of fluorinated diluents in solvent extraction processes are discussed. This article should provide assistance to researchers investigating new or improved solvent extraction processes where traditional hydrocarbon diluents may not be appropriate.","PeriodicalId":22002,"journal":{"name":"Solvent Extraction and Ion Exchange","volume":null,"pages":null},"PeriodicalIF":2.0,"publicationDate":"2023-03-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"44063523","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}
Pub Date : 2023-03-14DOI: 10.1080/07366299.2023.2186180
A. E. Mubark, Samar E. Abd-El Razek, A. Eliwa, S. M. El-Gamasy
ABSTRACT Sulfadiazine Schiff base (SDSB) was prepared using an inexpensive technique by modification of sulfadiazine drug (SD) to be used as an adsorbent material for recovery of Y(III) ions from aqueous solutions. Chemical and physical characterizations of SDSB were performed using different techniques. The maximum static adsorption capacity of the modified SD was 0.9 mmolg−1 for Y(III) ions and at pH 5.0. The kinetics results revealed that the sorption of Y(III) ions upon the synthesized SDSB followed the pseudo-second-order with R2 of >0.999. Temkin, Dubinin – Radushkevich, Freundlich, and Langmuir models accurately described the adsorption isotherm data. The activation energy (Ea) for adsorption was 17.52 kJmol−1, indicating the process is to be chemisorption. Thermodynamic characteristics with ΔHo of 11.33 kJmol−1 and a ΔSo 110.2 Jmol−1K−1. Using FT-IR and EDAX analysis proved the yttrium adsorption upon the SDSB. The desorption process for Y(III) ions was successfully achieved using 1 M HNO3 and it reduced from 95% to 70% after five consecutive cycles. A pre-concentration process for yttrium ions presented in a waste solution was achieved using SDSB adsorbent with a pre-concentration factor of about 10. As a result, it is regarded as a promising adsorbent for Y(III) ions in a variety of industrial applications.
摘要以磺胺嘧啶类药物（SD）为吸附剂，采用廉价的工艺制备了磺胺嘧啶席夫碱（SDSB）。使用不同的技术对SDSB进行了化学和物理表征。在pH 5.0时，改性SD对Y（III）离子的最大静态吸附容量为0.9 mmol−1。动力学结果表明，Y（III）离子在合成的SDSB上的吸附遵循伪二阶，R2＞0.999。Temkin、Dubinin–Radushkevich、Freundlich和Langmuir模型准确地描述了吸附等温线数据。吸附的活化能（Ea）为17.52kJmol−1，表明该过程为化学吸附。ΔHo为11.33 kJmol−1，ΔSo为110.2 Jmol−1K−1时的热力学特性。用FT-IR和EDAX分析证实了钇在SDSB上的吸附。使用1 M HNO3，并且在连续五个循环后从95%降低到70%。使用预浓缩因子约为10的SDSB吸附剂实现了废溶液中存在的钇离子的预浓缩过程。因此，它被认为是一种在各种工业应用中很有前途的Y（III）离子吸附剂。
{"title":"Investigation on the Sulfadiazine Schiff Base Adsorption Ability of Y(III) Ions from Nitrate Solutions, Kinetics, and Thermodynamic Studies","authors":"A. E. Mubark, Samar E. Abd-El Razek, A. Eliwa, S. M. El-Gamasy","doi":"10.1080/07366299.2023.2186180","DOIUrl":"https://doi.org/10.1080/07366299.2023.2186180","url":null,"abstract":"ABSTRACT Sulfadiazine Schiff base (SDSB) was prepared using an inexpensive technique by modification of sulfadiazine drug (SD) to be used as an adsorbent material for recovery of Y(III) ions from aqueous solutions. Chemical and physical characterizations of SDSB were performed using different techniques. The maximum static adsorption capacity of the modified SD was 0.9 mmolg−1 for Y(III) ions and at pH 5.0. The kinetics results revealed that the sorption of Y(III) ions upon the synthesized SDSB followed the pseudo-second-order with R2 of >0.999. Temkin, Dubinin – Radushkevich, Freundlich, and Langmuir models accurately described the adsorption isotherm data. The activation energy (Ea) for adsorption was 17.52 kJmol−1, indicating the process is to be chemisorption. Thermodynamic characteristics with ΔHo of 11.33 kJmol−1 and a ΔSo 110.2 Jmol−1K−1. Using FT-IR and EDAX analysis proved the yttrium adsorption upon the SDSB. The desorption process for Y(III) ions was successfully achieved using 1 M HNO3 and it reduced from 95% to 70% after five consecutive cycles. A pre-concentration process for yttrium ions presented in a waste solution was achieved using SDSB adsorbent with a pre-concentration factor of about 10. As a result, it is regarded as a promising adsorbent for Y(III) ions in a variety of industrial applications.","PeriodicalId":22002,"journal":{"name":"Solvent Extraction and Ion Exchange","volume":null,"pages":null},"PeriodicalIF":2.0,"publicationDate":"2023-03-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"46866820","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}
Pub Date : 2023-02-28DOI: 10.1080/07366299.2023.2185097
Lili Cui, Jungang Cao, Shihui Jiao, G. Pang, Zhonglin Wei
ABSTRACT A selective extraction process for recovering vanadium (IV) over chromium was proposed with use of a mixed extractant consisting of di(2-ethylhexyl) phosphate (D2EHPA) and tri-n-butyl phosphate (TBP). The influence of various factors, which included the initial aqueous pH value, the concentration of leach solution and D2EHPA, phase ratio (O/A), extraction equilibrium time and extraction temperature in the extraction process on the separation of V and Cr was investigated. Under the condition of the optimum extraction, vanadium extraction was above 94.0%. Meanwhile, under the optimum stripping conditions, the vanadium stripping was above 93.0% utilizing 1.5 mol/L sulfuric acid as the effective stripping reagent. The regeneration and reusability of the loaded organic phases after stripping were discussed. In addition, continuous three-stage extraction and stripping strategy indicated that the aggregate loss of vanadium was 0.885% and that the purity of vanadium was more than 99.9%. Under the condition of the optimum precipitation, when the pH value of the stripping solution was adjusted to 7.0 with ammonia water, the precipitation efficiency reached 99.93%. The calcination conditions (above 680 °C in air) were finally determined by TG-DTA and TG-MS experiments, and the V2O5 obtained by calcination was characterized by XRD. Additionally, a method for detecting impurity elements in vanadium matrix without interference was established. The recovery technology has practical significance in enlarging production scale, reducing specific energy consumption and cost, and realizing automatic control in vanadium leaching process.
{"title":"Selective Solvent Extraction of Vanadium Over Chromium from Alkaline Leaching Solution of Vanadium Slag by D2EHPA/TBP","authors":"Lili Cui, Jungang Cao, Shihui Jiao, G. Pang, Zhonglin Wei","doi":"10.1080/07366299.2023.2185097","DOIUrl":"https://doi.org/10.1080/07366299.2023.2185097","url":null,"abstract":"ABSTRACT A selective extraction process for recovering vanadium (IV) over chromium was proposed with use of a mixed extractant consisting of di(2-ethylhexyl) phosphate (D2EHPA) and tri-n-butyl phosphate (TBP). The influence of various factors, which included the initial aqueous pH value, the concentration of leach solution and D2EHPA, phase ratio (O/A), extraction equilibrium time and extraction temperature in the extraction process on the separation of V and Cr was investigated. Under the condition of the optimum extraction, vanadium extraction was above 94.0%. Meanwhile, under the optimum stripping conditions, the vanadium stripping was above 93.0% utilizing 1.5 mol/L sulfuric acid as the effective stripping reagent. The regeneration and reusability of the loaded organic phases after stripping were discussed. In addition, continuous three-stage extraction and stripping strategy indicated that the aggregate loss of vanadium was 0.885% and that the purity of vanadium was more than 99.9%. Under the condition of the optimum precipitation, when the pH value of the stripping solution was adjusted to 7.0 with ammonia water, the precipitation efficiency reached 99.93%. The calcination conditions (above 680 °C in air) were finally determined by TG-DTA and TG-MS experiments, and the V2O5 obtained by calcination was characterized by XRD. Additionally, a method for detecting impurity elements in vanadium matrix without interference was established. The recovery technology has practical significance in enlarging production scale, reducing specific energy consumption and cost, and realizing automatic control in vanadium leaching process.","PeriodicalId":22002,"journal":{"name":"Solvent Extraction and Ion Exchange","volume":null,"pages":null},"PeriodicalIF":2.0,"publicationDate":"2023-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"44538567","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}
Pub Date : 2023-02-23DOI: 10.1080/07366299.2023.2181090
Jelena Toropitsyna, L. Jelínek, Ross Wilson, M. Paidar
ABSTRACT The low pH and high salinity of acid mine drainage (AMD) fundamentally complicates the sorption processes. We explored the selective removal of Cu, Ni and Co ions present in AMD from the excess of ferrous ions of using a chelating resins Lewatit® MonoPlus TP 220 and Lewatit® TP 208. Also, the recovery of metal copper from desorption solution using electrolysis was investigated. The results showed that the most effective sorption of metal ions was achieved with chelating sorbent Lewatit® TP 220. The dynamic capacity of the sorbent under the given conditions (pH= 2.5 ± 0.03, presence of Fe(II/III), Zn(II), Mn(II)) decreased in the following order: Cu(II) (43.3 ± 1.4 g/L) > Ni(II) (22.1 ± 2.1 g/L) > Co(II) (3.6 ± 0.4 g/L). Chelating resin Lewatit® TP 208 under the same conditions showed lower efficiency: Cu(II) (30.6 ± 1.3 g/L) > Ni(II) (9.1 ± 0.17 g/L) > Co(II) (1.3 ± 0.08 g/L). The weak base anion exchanger Purolite® A 832 was successfully used to take up Cu(II) from ammonia solution and easily regenerated with sulfuric acid. The sorption capacity for Cu(II) was calculated to be 19.2 ± 0.5 g/L. Electrolysis experiments were performed with a fluidized bed electrolysis reactor where metallic copper was regenerated from desorption solutions and purified sulfuric acid solutions were obtained. GRAPHICAL ABSTRACT
{"title":"Selective Removal of Transient Metal Ions from Acid Mine Drainage and the Possibility of Metallic Copper Recovery with Electrolysis","authors":"Jelena Toropitsyna, L. Jelínek, Ross Wilson, M. Paidar","doi":"10.1080/07366299.2023.2181090","DOIUrl":"https://doi.org/10.1080/07366299.2023.2181090","url":null,"abstract":"ABSTRACT The low pH and high salinity of acid mine drainage (AMD) fundamentally complicates the sorption processes. We explored the selective removal of Cu, Ni and Co ions present in AMD from the excess of ferrous ions of using a chelating resins Lewatit® MonoPlus TP 220 and Lewatit® TP 208. Also, the recovery of metal copper from desorption solution using electrolysis was investigated. The results showed that the most effective sorption of metal ions was achieved with chelating sorbent Lewatit® TP 220. The dynamic capacity of the sorbent under the given conditions (pH= 2.5 ± 0.03, presence of Fe(II/III), Zn(II), Mn(II)) decreased in the following order: Cu(II) (43.3 ± 1.4 g/L) > Ni(II) (22.1 ± 2.1 g/L) > Co(II) (3.6 ± 0.4 g/L). Chelating resin Lewatit® TP 208 under the same conditions showed lower efficiency: Cu(II) (30.6 ± 1.3 g/L) > Ni(II) (9.1 ± 0.17 g/L) > Co(II) (1.3 ± 0.08 g/L). The weak base anion exchanger Purolite® A 832 was successfully used to take up Cu(II) from ammonia solution and easily regenerated with sulfuric acid. The sorption capacity for Cu(II) was calculated to be 19.2 ± 0.5 g/L. Electrolysis experiments were performed with a fluidized bed electrolysis reactor where metallic copper was regenerated from desorption solutions and purified sulfuric acid solutions were obtained. GRAPHICAL ABSTRACT","PeriodicalId":22002,"journal":{"name":"Solvent Extraction and Ion Exchange","volume":null,"pages":null},"PeriodicalIF":2.0,"publicationDate":"2023-02-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"41463147","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}
Pub Date : 2023-02-22DOI: 10.1080/07366299.2023.2182646
Zhaofei Zhang, W. Duan, Xinwei Cheng, Wenbing Li, Jing Chen, Jianchen Wang, T. Sun
ABSTRACT Denitration is a proven technique that can reduce the nitric acid concentration of high-level liquid waste (HLLW) to meet the aqueous acidity requirement of the TRPO (TriAlkyl Phosphine Oxide) process. However, interfacial crud is generated in the TRPO extraction of the HLLW after denitration. In this work, the interfacial crud was characterized by Fourier-transform infrared spectroscopy and dynamic light scattering. The extraction distribution ratio of zirconium by 30% TRPO in kerosene decreases dramatically after the simulated HLLW is denitrated, and we proposed that the presence of zirconium in the simulated HLLW after denitration is responsible for the generation of interfacial crud. Using ammonium molybdate as a precipitant, the concentration of zirconium in the simulated HLLW was successfully reduced without essentially changing the concentration of other metal ions. The effects of reaction time, temperature, and amount of ammonium molybdate added on the zirconium removal process were investigated and the precipitates formed in the removal of zirconium were characterized by scanning electron microscope, energy dispersive X-ray spectroscopy, and X-ray photoelectron spectroscopy. Finally, after reducing the concentration of zirconium in the simulated HLLW to below 10 mg/L by using ammonium molybdate, the extraction experiment was performed again and no interfacial crud was observed.
{"title":"Elimination of the Interfacial Crud in the Extraction of Simulated High-Level Liquid Waste After Denitration in the TRPO Process","authors":"Zhaofei Zhang, W. Duan, Xinwei Cheng, Wenbing Li, Jing Chen, Jianchen Wang, T. Sun","doi":"10.1080/07366299.2023.2182646","DOIUrl":"https://doi.org/10.1080/07366299.2023.2182646","url":null,"abstract":"ABSTRACT Denitration is a proven technique that can reduce the nitric acid concentration of high-level liquid waste (HLLW) to meet the aqueous acidity requirement of the TRPO (TriAlkyl Phosphine Oxide) process. However, interfacial crud is generated in the TRPO extraction of the HLLW after denitration. In this work, the interfacial crud was characterized by Fourier-transform infrared spectroscopy and dynamic light scattering. The extraction distribution ratio of zirconium by 30% TRPO in kerosene decreases dramatically after the simulated HLLW is denitrated, and we proposed that the presence of zirconium in the simulated HLLW after denitration is responsible for the generation of interfacial crud. Using ammonium molybdate as a precipitant, the concentration of zirconium in the simulated HLLW was successfully reduced without essentially changing the concentration of other metal ions. The effects of reaction time, temperature, and amount of ammonium molybdate added on the zirconium removal process were investigated and the precipitates formed in the removal of zirconium were characterized by scanning electron microscope, energy dispersive X-ray spectroscopy, and X-ray photoelectron spectroscopy. Finally, after reducing the concentration of zirconium in the simulated HLLW to below 10 mg/L by using ammonium molybdate, the extraction experiment was performed again and no interfacial crud was observed.","PeriodicalId":22002,"journal":{"name":"Solvent Extraction and Ion Exchange","volume":null,"pages":null},"PeriodicalIF":2.0,"publicationDate":"2023-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"59691550","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}
ABSTRACT The extraction of Am3+ and Eu3+ with 6,6’-bis(5-alkyl-1H-pyrazol-3-yl)-2,2’-bipyridine (BPzBPy, alkyl = i-Bu, n-Bu, n-Oct) from HNO3 medium and the complexation of BPzBPy with Eu3+ were investigated. By using meta-nitrobenzotrifluoride (F-3) as a diluent, iBu-BPzBPy ligand in combination with 2-bromohexanoic acid was able to extract Am3+ over Eu3+ with the nature of significantly high efficiency, relatively fast extraction kinetics, and easy stripping. Slope analysis showed the formation of a 1:2 metal/ligand extraction species. The analyses of electrospray ionization mass spectrometry (ESI-MS), Fourier transform infrared (FT-IR) and time-resolved laser fluorescence spectrum (TRLFS) revealed that the composition of the extracted complex was [Eu(H2O)L2]A3 (L = ligand; HA = 2-bromohexanoic acid). The complexation of iBu-BPzBPy ligand with Eu3+ was an enthalpy-driven spontaneous, exothermic, and entropy-decreasing process. Besides, the complex stability constants were also obtained via UV–vis spectrophotometric titration. Combining the results of solvent extraction and complexation studies, a cation exchange extraction model was also proposed. GRAPHICAL ABSTRACT
{"title":"A Novel Type of Tetradentate Dipyridyl-Derived Bis(pyrazole) Ligands for Highly Efficient and Selective Extraction of Am3+ Over Eu3+ From HNO3 Solution","authors":"Lianjun Song, Xueyu Wang, Long Li, Zhuang Wang, Lanlan He, Qiuju Li, Qingjiang Pan, Songdong Ding","doi":"10.1080/07366299.2023.2173014","DOIUrl":"https://doi.org/10.1080/07366299.2023.2173014","url":null,"abstract":"ABSTRACT The extraction of Am3+ and Eu3+ with 6,6’-bis(5-alkyl-1H-pyrazol-3-yl)-2,2’-bipyridine (BPzBPy, alkyl = i-Bu, n-Bu, n-Oct) from HNO3 medium and the complexation of BPzBPy with Eu3+ were investigated. By using meta-nitrobenzotrifluoride (F-3) as a diluent, iBu-BPzBPy ligand in combination with 2-bromohexanoic acid was able to extract Am3+ over Eu3+ with the nature of significantly high efficiency, relatively fast extraction kinetics, and easy stripping. Slope analysis showed the formation of a 1:2 metal/ligand extraction species. The analyses of electrospray ionization mass spectrometry (ESI-MS), Fourier transform infrared (FT-IR) and time-resolved laser fluorescence spectrum (TRLFS) revealed that the composition of the extracted complex was [Eu(H2O)L2]A3 (L = ligand; HA = 2-bromohexanoic acid). The complexation of iBu-BPzBPy ligand with Eu3+ was an enthalpy-driven spontaneous, exothermic, and entropy-decreasing process. Besides, the complex stability constants were also obtained via UV–vis spectrophotometric titration. Combining the results of solvent extraction and complexation studies, a cation exchange extraction model was also proposed. GRAPHICAL ABSTRACT","PeriodicalId":22002,"journal":{"name":"Solvent Extraction and Ion Exchange","volume":null,"pages":null},"PeriodicalIF":2.0,"publicationDate":"2023-02-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"43765868","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}
Pub Date : 2023-01-31DOI: 10.1080/07366299.2023.2165405
N. Vieceli, Claudia Vonderstein, Thomas Swiontekc, S. Stopić, Christian Dertmann, Reiner Sojka, Niclas Reinhardt, C. Ekberg, B. Friedrich, M. Petranikova
ABSTRACT Manganese plays a central role in lithium-ion batteries (LIBs) but its recycling is rarely addressed when compared to other valuable metals present in LIBs, such as Co and Ni. Thus, the main goal of this work was to study and achieve the separation of Mn from Co and Ni by solvent extraction from a leachate obtained from LIBs using hydrochloric acid in an upscaled reactor, which is an innovative aspect of this work. The results confirmed the high selectivity of D2EHPA towards Mn, which could be completely extracted in two stages (0.5 M D2EHPA at pH 2.5). The main co-extracted metals were Al, Cu and Co, but with lower concentrations than Mn. The behavior of minor impurities such as Zn and Mg was also monitored. Scrubbing using manganese chloride was crucial to remove impurities from the loaded organic and prevent their presence in the stripping product, and high O:A ratios negatively affected the scrubbing efficiency. Keeping the concentration of HCl up to 0.5 M in the stripping stage helped to limit the stripping of impurities. Manganese oxide was precipitated as a product with 99.5% purity (with traces of Zn, Cu and Co), which could be reused in the battery value chain.
锰在锂离子电池(LIBs)中起着核心作用，但与锂离子电池中存在的其他有价金属(如Co和Ni)相比，锰的回收利用很少得到解决。因此，本工作的主要目标是研究并实现在升级反应器中使用盐酸从lib获得的渗滤液中溶剂萃取Mn与Co和Ni的分离，这是本工作的一个创新方面。结果证实了D2EHPA对Mn具有较高的选择性，可通过两个阶段(0.5 M D2EHPA, pH为2.5)完全提取。共萃取金属主要为Al、Cu和Co，但浓度低于Mn。同时还对锌、镁等微量杂质的行为进行了监测。使用氯化锰进行洗涤对于去除负载有机物中的杂质并防止其出现在汽提产品中至关重要，高O:A比对洗涤效率产生负面影响。在汽提阶段将HCl浓度保持在0.5 M以内有助于限制杂质的汽提。氧化锰的析出产物纯度为99.5%(含微量Zn、Cu和Co)，可在电池价值链中重复利用。
{"title":"Recycling of Li-Ion Batteries from Industrial Processing: Upscaled Hydrometallurgical Treatment and Recovery of High Purity Manganese by Solvent Extraction","authors":"N. Vieceli, Claudia Vonderstein, Thomas Swiontekc, S. Stopić, Christian Dertmann, Reiner Sojka, Niclas Reinhardt, C. Ekberg, B. Friedrich, M. Petranikova","doi":"10.1080/07366299.2023.2165405","DOIUrl":"https://doi.org/10.1080/07366299.2023.2165405","url":null,"abstract":"ABSTRACT Manganese plays a central role in lithium-ion batteries (LIBs) but its recycling is rarely addressed when compared to other valuable metals present in LIBs, such as Co and Ni. Thus, the main goal of this work was to study and achieve the separation of Mn from Co and Ni by solvent extraction from a leachate obtained from LIBs using hydrochloric acid in an upscaled reactor, which is an innovative aspect of this work. The results confirmed the high selectivity of D2EHPA towards Mn, which could be completely extracted in two stages (0.5 M D2EHPA at pH 2.5). The main co-extracted metals were Al, Cu and Co, but with lower concentrations than Mn. The behavior of minor impurities such as Zn and Mg was also monitored. Scrubbing using manganese chloride was crucial to remove impurities from the loaded organic and prevent their presence in the stripping product, and high O:A ratios negatively affected the scrubbing efficiency. Keeping the concentration of HCl up to 0.5 M in the stripping stage helped to limit the stripping of impurities. Manganese oxide was precipitated as a product with 99.5% purity (with traces of Zn, Cu and Co), which could be reused in the battery value chain.","PeriodicalId":22002,"journal":{"name":"Solvent Extraction and Ion Exchange","volume":null,"pages":null},"PeriodicalIF":2.0,"publicationDate":"2023-01-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"47869044","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}
Pub Date : 2023-01-25DOI: 10.1080/07366299.2022.2156798
B. Mahanty, P. Mohapatra, R. Egberink, J. Huskens, W. Verboom
ABSTRACT Pertraction of Np(IV) across a PTFE membrane containing two different aza-crown ether-based multiple diglycolamide (DGA) ligands termed as L I (3 DGA arms) or L II (4 DGA arms) was investigated using nitric acid as feed solution. A few of the studies were also carried out with Pu(IV) for comparison purposes. The kinetics of the extraction of Np(IV) and Pu(IV) was fast at 3 M HNO3 and within 10 min reaches the equilibrium distribution (D) ratio with both ligands. However, the stripping kinetics was slower especially with ligand L II . The extraction and transport studies were carried out using 1.0 × 10−3 M ligand solution in 95% n-dodecane + 5% isodecanol. The transport rates were slower with ligand L II than with L I at higher nitric acid concentrations (>1 M HNO3) and the transport rates decreased with nitric acid concentration with both ligands. The effective diffusion coefficients (D eff) of Np(IV) were estimated using the lag-time method as 6.2 × 10−8 cm2 s−1 (L I ) and 4.6 × 10−8 cm2 s−1 (L II ). The stability data suggest that the L I containing supported liquid membrane (SLM) is comparatively more stable than that of L II and the transport flux remains the same up to nine days of operation in case of ligand L I .
{"title":"Highly Efficient Pertraction of Tetravalent Neptunium Ions Across a Flat Sheet Supported Liquid Membrane Containing Two Different Aza-Crown Ether-Based Multiple Diglycolamide Ligands","authors":"B. Mahanty, P. Mohapatra, R. Egberink, J. Huskens, W. Verboom","doi":"10.1080/07366299.2022.2156798","DOIUrl":"https://doi.org/10.1080/07366299.2022.2156798","url":null,"abstract":"ABSTRACT Pertraction of Np(IV) across a PTFE membrane containing two different aza-crown ether-based multiple diglycolamide (DGA) ligands termed as L I (3 DGA arms) or L II (4 DGA arms) was investigated using nitric acid as feed solution. A few of the studies were also carried out with Pu(IV) for comparison purposes. The kinetics of the extraction of Np(IV) and Pu(IV) was fast at 3 M HNO3 and within 10 min reaches the equilibrium distribution (D) ratio with both ligands. However, the stripping kinetics was slower especially with ligand L II . The extraction and transport studies were carried out using 1.0 × 10−3 M ligand solution in 95% n-dodecane + 5% isodecanol. The transport rates were slower with ligand L II than with L I at higher nitric acid concentrations (>1 M HNO3) and the transport rates decreased with nitric acid concentration with both ligands. The effective diffusion coefficients (D eff) of Np(IV) were estimated using the lag-time method as 6.2 × 10−8 cm2 s−1 (L I ) and 4.6 × 10−8 cm2 s−1 (L II ). The stability data suggest that the L I containing supported liquid membrane (SLM) is comparatively more stable than that of L II and the transport flux remains the same up to nine days of operation in case of ligand L I .","PeriodicalId":22002,"journal":{"name":"Solvent Extraction and Ion Exchange","volume":null,"pages":null},"PeriodicalIF":2.0,"publicationDate":"2023-01-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"43682425","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}
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