Mechanism unravelling for highly efficient and selective 99TcO4− sequestration utilising crown ether based solvent system from nuclear liquid waste: experimental and computational investigations

Patra, Kankan; Sengupta, Arijit; Boda, Anil; Ali, Musharaf; Mittal, Vinit K.; Valsala, T.P.; Kaushik, C.P.

doi:10.1039/d1ra07738d

Cited by 13 publications

(5 citation statements)

References 55 publications

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“…The effects of acidity increase in the order of H 2 SO 4 < HCl < HNO 3 , and D2EHAG exhibits better extraction ability than M2EHAG and PLLAG. By comprehensive comparison with the extractants reported recently, most extractants have strict requirements on pH, but D2EHAG can have ultrahigh selectivity in a wide range of acidic pH values. ,, …”

Section: Results and Discussionmentioning

confidence: 99%

“…To determine the ratio of complexes formed by D2EHAG and 99 TcO 4 – /ReO 4 – in the extraction process, slope analysis was used Figure clearly shows that D2EHAG is directly involved in the extraction of ReO 4 – ions.…”

Section: Results and Discussionmentioning

confidence: 99%

“…99 Tc has high solubility in water, and radioactive waste liquid contains more competitive anions. The current removal technologies are mainly divided into two categories: extraction and adsorption; the extraction systems mainly include carbazole derivatives, 5 crown ethers, 6 eutectic solvents, 7 ionic liquids, 8 and amides. 9 These extractants may have high cost, complex synthesis, and low selectivity.…”

Section: Introductionmentioning

confidence: 99%

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Ultraselective Extraction Reprocessing of ⁹⁹TcO₄^–/ReO₄^– with a Promising Carbamic Acid Extractant System

Yinqiao

Qin

et al. 2023

Inorg. Chem.

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With the development of nuclear energy, the reprocessing of 99TcO4 –/ReO4 – has become a very difficult problem due to environmental issues such as high output, long life, and easy leakage. In this study, three extraction systems containing carbamic acid were introduced into the reprocessing of 99TcO4 –/ReO4 – for the first time. The results involving one of the three results show that N-[N,N-di(2-ethylhexyl) aminocarbonylmethyl] glycine (D2EHAG) has ultrahigh selectivity for removal to 99TcO4 –/ReO4 –. When the extreme concentration ratio of SO4 2– and Cl– to ReO4 – of D2EHAG is 10,000:1, the distribution coefficient of ReO4 – still reaches 12.73 and 2.67, respectively. Additionally, the most hydrophilic NO3 –, when the extreme concentration ratio of NO3 – and ReO4 – is 1000:1, still has a distribution coefficient close to 2.33, which is more than the most reported MOF adsorption materials. Moreover, the reaction kinetics, stripping rate, and reuse rate were studied. After five cycles, the removal rate is still 98.12%, with a decrease of less than 0.7%. The system containing carbamic acid is a potential extraction removal system to remove 99TcO4 –/ReO4 – from nuclear radioactive wastewater.

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Section: Results and Discussionmentioning

confidence: 99%

Section: Results and Discussionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Ultraselective Extraction Reprocessing of ⁹⁹TcO₄^–/ReO₄^– with a Promising Carbamic Acid Extractant System

Yinqiao

Qin

et al. 2023

Inorg. Chem.

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“…Several methods, such as ion exchange, 5,6 solvent extraction, 7,8 reduction–immobilization 9,10 and adsorption, 11,12 have been explored to separate TcO 4 − from wastewater. Various ion exchange resins are used as adsorbents for TcO 4 − capture, but poor irradiation stability and slow kinetics seriously limit their widespread application.…”

Section: Introductionmentioning

confidence: 99%

Efficient and selective separation of Re(VII), an analogue of Tc(VII), by a defective biochar with honeycomb‐like porous structure

Hu,

Yu,

Wang

et al. 2024

J of Chemical Tech & Biotech

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BACKGROUNDIn this study, a defective biochar with honeycomb‐like porous structure (BC‐PH) was successfully prepared by the activation of pristine biochar derived from bamboo shoot shell with the chemical reagent KOH, and was applied to selectively separate ReO4− (a chemical analogue for radioactive TcO4−) from acidic solutions.RESULTSThe diffusion, mass transfer and recovery for ReO4− could be significantly improved by the large specific surface area (SBET, 2412 m2 g−1) and high total volume (Vtot, 1.26 cm3 g−1) of BC‐PH. The influence of adsorbent dosage, system pH and coexisting ions with different valence states on the adsorption capability and selectivity of BC‐PH toward ReO4− was systematically investigated. BC‐PH exhibited high adsorption capacity and selectivity for ReO4− with a maximal sorption capacity (qm) of 73.11 mg g−1 at initial pH 2. By applying an analysis of kinetics and isotherm adsorption studies, the liquid film diffusion was verified to be the primary rate‐controlling step for the sorption of ReO4− and the multilayer adsorption process occurred on the heterogeneous surface of BC‐PH. Besides, the recovery of ReO4− using BC‐PH occurred in an exothermic and spontaneous manner according to thermodynamic analysis. Furthermore, an investigation of the adsorption mechanism suggested that pore filling and electron donor–acceptor interaction were mainly related to the removal of ReO4−.CONCLUSIONThese results suggest that BC‐PH has great potential for the application of TcO4− separation in consideration of its high adsorption capacity and selectivity. © 2024 Society of Chemical Industry (SCI).

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“…It has always been a difficult point for researchers to remove and capture 99 TcO 4 − in radioactive wastewater under the condition of strong acid, strong alkali, and a large number of anions [ 8 ]. The current research methods for removing and capturing 99 TcO 4 − in radioactive wastewater can be divided into solvent extraction and solid-phase extraction [ 9 , 10 , 11 , 12 ]. Compared with solvent extraction, solid phase extraction has a faster extraction rate, better reusability, simpler operation, and easier separation [ 13 ].…”

Section: Introductionmentioning

confidence: 99%

Highly Selective Adsorption of 99TcO4−/ReO4− by a Novel Polyamide-Functionalized Polyacrylamide Polymer Material

Qin

Yinqiao

Xie

et al. 2022

Toxics

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The treatment of radioactive wastewater is one of the major problems in the current research. With the development of nuclear energy, the efficient removal of 99TcO4− in radioactive wastewater has attracted the attention of countries all over the world. In this study, a novel functional polyamide polymer p-(Amide)-PAM was synthesized by the two-step method. The experimental results show that p-(Amide)-PAM has good adsorptive properties for 99TcO4−/ReO4− and has good selectivity in the nitric acid system. The kinetics of the reaction of p-(Amide)-PAM with 99TcO4−/ReO4− was studied. The results show that p-(Amide)-PAM has a fast adsorption rate for 99TcO4−/ReO4−, the saturated adsorption capacity reaches 346.02 mg/g, and the material has good reusability. This new polyamide-functionalized polyacrylamide polymer material has good application prospects in the removal of 99TcO4− from radioactive wastewater.

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Mechanism unravelling for highly efficient and selective ⁹⁹TcO₄⁻ sequestration utilising crown ether based solvent system from nuclear liquid waste: experimental and computational investigations

Abstract: Highly efficient and selective 99TcO4− sequestration utilising crown ether based solvent system from reprocessing low level liquid waste.

Cited by 13 publications

References 55 publications

Ultraselective Extraction Reprocessing of ⁹⁹TcO₄^–/ReO₄^– with a Promising Carbamic Acid Extractant System

Ultraselective Extraction Reprocessing of ⁹⁹TcO₄^–/ReO₄^– with a Promising Carbamic Acid Extractant System

Efficient and selective separation of Re(VII), an analogue of Tc(VII), by a defective biochar with honeycomb‐like porous structure

Highly Selective Adsorption of 99TcO4−/ReO4− by a Novel Polyamide-Functionalized Polyacrylamide Polymer Material

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Mechanism unravelling for highly efficient and selective 99TcO4− sequestration utilising crown ether based solvent system from nuclear liquid waste: experimental and computational investigations

Abstract: Highly efficient and selective 99TcO4− sequestration utilising crown ether based solvent system from reprocessing low level liquid waste.

Cited by 13 publications

References 55 publications

Ultraselective Extraction Reprocessing of 99TcO4–/ReO4– with a Promising Carbamic Acid Extractant System

Ultraselective Extraction Reprocessing of 99TcO4–/ReO4– with a Promising Carbamic Acid Extractant System

Efficient and selective separation of Re(VII), an analogue of Tc(VII), by a defective biochar with honeycomb‐like porous structure

Highly Selective Adsorption of 99TcO4−/ReO4− by a Novel Polyamide-Functionalized Polyacrylamide Polymer Material

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Mechanism unravelling for highly efficient and selective ⁹⁹TcO₄⁻ sequestration utilising crown ether based solvent system from nuclear liquid waste: experimental and computational investigations

Ultraselective Extraction Reprocessing of ⁹⁹TcO₄^–/ReO₄^– with a Promising Carbamic Acid Extractant System

Ultraselective Extraction Reprocessing of ⁹⁹TcO₄^–/ReO₄^– with a Promising Carbamic Acid Extractant System