This work is a comparative study of the efficiency of the lutetium (III) extraction in membrane-assisted liquid-phase extraction (LPE) carried out under static and continuous operation mode using di(2-ethylhexyl)phosphoric acid (DEHPA) as a carrier. The removal of Lu(III) from the donor solution and its recovery into the acceptor phase were compared for the two operation modes investigated. Additionally, the applicability of both systems for purification of 177Lu-radiopharmaceutical was discussed

Goran Vladisavljevic (1253448)

Ksenija R. Kumric (7128653)

Tatjana M. Trtic-Petrovic (7128662)

English

Loughborough University Institutional Repository

   This item was submitted to Loughborough’s Institutional Repository (https://dspace.lboro.ac.uk/) by the author and is made available under the following Creative Commons Licence conditions.      For the full text of this licence, please go to: http://creativecommons.org/licenses/by-nc-nd/2.5/  COMPARISON OF STATIC AND CONTINUOUS HOLLOW FIBRE LIQUID-PHASE EXTRACTION OF LUTETIUM  Ksenija R. Kumrić1, Tatjana M. Trtić-Petrović1, Goran T. Vladisavljević2 1Laboratory of Physics, Vinča Institute of Nuclear Sciences, University of Belgrade, P.O. Box 522, Belgrade, Serbia, 2Loughborough University, Department of Chemical Engineering, Leicestershire LE11 3TU UK  ABSTRACT This work is a comparative study of the efficiency of the lutetium (III) extraction in membrane-assisted liquid-phase extraction (LPE) carried out under static and continuous operation mode using di(2-ethylhexyl)phosphoric acid (DEHPA) as a carrier. The removal of Lu(III) from the donor solution and its recovery into the acceptor phase were compared for the two operation modes investigated. Additionally, the applicability of both systems for purification of 177Lu-radiopharmaceutical was discussed. INTRODUCTION Radionuclide 177Lu possesses favorable radiophysical characteristics for therapeutic application in nuclear medicine [1]. One of the main steps in the production process of 177Lu-radiopharmaceutical is the separation of bound from unbound radionuclide. Membrane-assisted LPE offers the possibility of purification of the 177Lu-radiopharmaceuticals, after the labeling procedure [2, 3]. Membrane-assisted LPE operates in a three-phase system and involves simultaneous extraction and re-extraction. The pores of a microporous hydrophobic membrane are filled with the organic phase (extractant) held by the action of capillary forces, while the feed (donor) and the stripping (acceptor) solutions are placed on each side of the membrane. Membrane-assisted LPE can be performed in a miniaturized system under static or continuous mode of operation. The aim of the present study was to compare the removal efficiency and re-extraction of Lu(III) achieved in a static and continuous flow membrane-assisted LPE system. The systems were investigated with regard to the potential application in purification of 177Lu-radiopharmaceutical. RESULTS AND DISCUSSION Lutetium was extracted using two different membrane-assisted LPE systems: (i) static, hollow fibre LPE system (HF-LPE) in the absence of flow of any phase, and (ii) dynamic, HF-LPE system with recirculation of the aqueous donor and acceptor phases. Microporous polypropylene hollow fibre membrane, ACCUREL 50/280 (Membrana GmbH, Wuppertal, Germany) was used in the experiments. The extraction was performed under predetermined optimum experimental conditions [3]: the donor phase of 2 mg dm-3 Lu(III) in 0.2 M sodium acetate buffer at pH 3.5, the organic phase composed of 5% DEHPA in di-hexyl ether and the acceptor phase of 2 M HCl. The membrane wall was impregnated with the organic phase, the acceptor phase was in the lumen of HF, and the donor phase was outside the HF. The efficiency of mass transfer of Lu(III) through the liquid membrane was evaluated using the following parameters: the removal efficiency (R) that represents the fraction of Lu(III) removed from the donor phase, the extraction efficiency (E ) that represents a fraction of Lu(III) initially present in the donor phase that was found in the acceptor after extraction and the memory effect (M ) that is the fraction of Lu(III) captured in the organic phase. 0 50 100 150 200 250051060708090100  R, E or M, %Time, min Fig. 1. Time dependence of the efficiency parameters R (■), E (●) and M (○) in the static three phase HF-LPE system Fig. 1 shows the time-dependent parameters of Lu(III) transfer in HF-LPE under stagnant mode of operation with a volume of acceptor of 0.01 cm3. As can be seen, the stagnant system was efficient in terms of the removal of Lu(III) from the donor phase, but poorly efficient in terms of Lu(III) recovery from the organic into the acceptor phase. As the acceptor volume increased from 0.01 to 0.06 cm3 as a result of increased HF length, the extraction efficiency improved from 5 to 15 % but even at the highest acceptor volume, 85% of the extracted amount of Lu(III) remained in the membrane. A further increase of the acceptor volume beyond 0.06 cm3 was impractical. Continuous HF-LPE of Lu(III) was carried out in the self-designed membrane contactor containing a single HF membrane. This configuration enables recirculation of both aqueous phases. Fig. 2 shows the time-dependent efficiency parameters in HF-LPE under recirculation of the acceptor phase (3 cm3) through the lumen of the fibre and donor phase (20 cm3) outside the fibre. As can be seen from Fig. 2, continuous HF-LPE system enables not only efficient removal of Lu(III) from the donor to the organic phase, but also its recovery from the organic to the acceptor phase. The accumulation of Lu(III) in the membrane was less than 5%, meaning that re-extraction of Lu(III) was almost complete. 0 50 100 150 200 250020406080100  R, E or M, %Time, min  Fig. 2. Time dependence of the efficiency parameters R (■), E (●) and M (○) in the HF-LPE system with the recirculation of aqueous phases (donor flow rate: 5.3 cm3 min-1, acceptor flow rate: 0.4 cm3 min-1) CONCLUSION The removal efficiency of Lu(III) from the aqueous donor solution was very high when both static and continuous HF-LPE were applied, which is of prime importance with regard to the potential application in purification of 177Lu-based radiopharmaceuticals. The main advantage of continuous over static system is almost complete re-extraction of Lu(III) into the acceptor phase. Considering practical aspects, static HF-LPE is easier to operate, which is very important when working with radioactive material, and more suitable for low volume production, as is often the case in radiopharmaceutical production. Continuous HF-LPE requires higher volumes of donor phase for the operation and there are more potential leakage points that can cause accidental release of radioactive material.  Acknowledgment We acknowledge the support to this work provided by the Ministry of Education and Science of Serbia through project Physics and Chemistry with Ion Beams, No. III 45006. References: [1] S. Banerjee et al., Nucl. Med. Biol., 2004, 31, 753-759. [2] K. Kumrić et al., Sep. Purif. Techn., 2006, 51, 310-317. [3] T. Trtić-Petrović et al., J. Sep. Sci., 2010, 33, 2002-2009. 

Comparison of static and continuous hollow fibre liquid-phase extraction of lutetium

This work is a comparative study of the efficiency of the lutetium (III) extraction in
membrane-assisted liquid-phase extraction (LPE) carried out under static and
continuous operation mode using di(2-ethylhexyl)phosphoric acid (DEHPA) as a
carrier. The removal of Lu(III) from the donor solution and its recovery into the
acceptor phase were compared for the two operation modes investigated.
Additionally, the applicability of both systems for purification of 177Luradiopharmaceutical was discussedPhysical chemistry 2012 : 11th international conference on fundamental and applied aspects of physical chemistry; Belgrade (Serbia); 24-28 September 201

Kumrić, Ksenija

Trtić-Petrović, Tatjana M.

Vladisavljević, G.T.

Repository of the Vinča Nuclear Institute (VinaR)

        Pon HYSICAL11th InterFundamentPhyUnder UnivePThe ConfProfesSeptemBe CHEMISnational Coal and Appsical Chem the auspicersity of Beroceeding      erence is desor  Ivan Dr        ber 24-28lgrade, Ser  TRY 2012nference lied Aspectistry s of the lgrade s dicated to aganić , 2012  bia   s of       ISBN 978-86-82475-27-9 Volume 1 ISBN 978-86-82475-28-6 Volume II  Title: PHYSICAL CHEMISTRY 2012 (Proceedings) Editors: S. Anić and Ž. Čupić Published by: Society of Physical Chemists of Serbia, Studenski trg 12-16, 11158, Belgrade, Serbia Publisher: Society of Physical Chemists of Serbia For Publisher: S. Anić, President of Society of Physical Chemists of Serbia Printed by: “Jovan” Priting and Publishing Company; 200 Copies; Number of pages: 6+ 497; Format: B5; Printing finished in September 2012.  Text and Layout: “Jovan”  200- Coppy printing  III CONTENTS  Volume 1 Organizers V Committees VI Sponsors VIII Professor Ivan Draganić IX Plenary lectures 1 Chemical Thermodynamics 35 Spectroscopy, Molecular Structure,  Physical Chemistry of Plasma 65 Kinetics, Catalysis  137 Nonlinear Dynamics  225 Electrochemistry  301 Biophysical Chemistry, Photochemistry,  Radiation Chemistry  337 Radiochemistry, Nuclear Chemistry  Material Science 415  Volume II Solid State Physical Chemistry 505 Macromolecular Physical Chemistry  515 Environmental Protection  Forensic Sciences Pharmaceutical Physical Chemistry 557 Phase Boundaries 667 Complex Compounds 681 General Physical Chemistry 707 Geophysical Chemistry 719 Education, History 731 Food Physical Chemistry 743 Free Topic 783 Index 791  K-06-P 579 COMPARISON OF STATIC AND CONTINUOUS HOLLOW FIBRE LIQUID-PHASE EXTRACTION OF LUTETIUM  K R. Kumrić1, T M. Trtić-Petrović1, G T. Vladisavljević2  1Laboratory of Physics, Vinča Institute of Nuclear Sciences, University of Belgrade, P.O. Box 522, Belgrade, Serbia, 2Loughborough University, Department of Chemical Engineering, Leicestershire LE11 3TU UK  Abstract This work is a comparative study of the efficiency of the lutetium (III) extraction in membrane-assisted liquid-phase extraction (LPE) carried out under static and continuous operation mode using di(2-ethylhexyl)phosphoric acid (DEHPA) as a carrier. The removal of Lu(III) from the donor solution and its recovery into the acceptor phase were compared for the two operation modes investigated. Additionally, the applicability of both systems for purification of 177Lu-radiopharmaceutical was discussed. Introduction Radionuclide 177Lu possesses favorable radiophysical characteristics for therapeutic application in nuclear medicine [1]. One of the main steps in the production process of 177Lu-radiopharmaceutical is the separation of bound from unbound radionuclide. Membrane-assisted LPE offers the possibility of purification of the 177Lu-radiopharmaceuticals, after the labeling procedure [2, 3]. Membrane-assisted LPE operates in a three-phase system and involves simultaneous extraction and re-extraction. The pores of a microporous hydrophobic membrane are filled with the organic phase (extractant) held by the action of capillary forces, while the feed (donor) and the stripping (acceptor) solutions are placed on each side of the membrane. Membrane-assisted LPE can be performed in a miniaturized system under static or continuous mode of operation. The aim of the present study was to compare the removal efficiency and re-extraction of Lu(III) achieved in a static and continuous flow membrane-assisted LPE system. The systems were investigated with regard to the potential application in purification of 177Lu-radiopharmaceutical. Results and Discussion Lutetium was extracted using two different membrane-assisted LPE systems: (i) static, hollow fibre LPE system (HF-LPE) in the absence of flow of any phase, and (ii) dynamic, HF-LPE system with recirculation of the aqueous donor and acceptor phases. Microporous polypropylene hollow fibre membrane, ACCUREL 50/280 (Membrana GmbH, Wuppertal, Germany) was used in the experiments. The extraction was performed under predetermined optimum experimental conditions [3]: the donor phase of 2 mg dm-3 Lu(III) in 0.2 M sodium acetate buffer at pH 3.5, the organic phase composed of 5% DEHPA in di-hexyl ether and the acceptor K-06-P 580 phase of 2 M HCl. The membrane wall was impregnated with the organic phase, the acceptor phase was in the lumen of HF, and the donor phase was outside the HF. The efficiency of mass transfer of Lu(III) through the liquid membrane was evaluated using the following parameters: the removal efficiency (R) that represents the fraction of Lu(III) removed from the donor phase, the extraction efficiency (E ) that represents a fraction of Lu(III) initially present in the donor phase that was found in the acceptor after extraction and the memory effect (M ) that is the fraction of Lu(III) captured in the organic phase. 0 50 100 150 200 250051060708090100R, E or M, %Time, min Figure 1. Time dependence of the efficiency parameters R (■), E (●) and M (○) in the static three phase HF-LPE system. Fig. 1 shows the time-dependent parameters of Lu(III) transfer in HF-LPE under stagnant mode of operation with a volume of acceptor of 0.01 cm3. As can be seen, the stagnant system was efficient in terms of the removal of Lu(III) from the donor phase, but poorly efficient in terms of Lu(III) recovery from the organic into the acceptor phase. As the acceptor volume increased from 0.01 to 0.06 cm3 as a result of increased HF length, the extraction efficiency improved from 5 to 15 % but even at the highest acceptor volume, 85% of the extracted amount of Lu(III) remained in the membrane. A further increase of the acceptor volume beyond 0.06 cm3 was impractical. Continuous HF-LPE of Lu(III) was carried out in the self-designed membrane contactor containing a single HF membrane. This configuration enables recirculation of both aqueous phases. Fig. 2 shows the time-dependent efficiency parameters in HF-LPE under recirculation of the acceptor phase (3 cm3) through the lumen of the fibre and donor phase (20 cm3) outside the fibre. As can be seen from Fig. 2, continuous HF-LPE system enables not only efficient removal of Lu(III) from the donor to the organic phase, but also its recovery from the organic to the acceptor phase. The accumulation of Lu(III) in the membrane was less than 5%, meaning that re-extraction of Lu(III) was almost complete. K-06-P 581 0 50 100 150 200 250020406080100R, E or M, %Time, min  Figure 2. Time dependence of the efficiency parameters R (■), E (●) and M (○) in the HF-LPE system with the recirculation of aqueous phases (donor flow rate: 5.3 cm3 min-1, acceptor flow rate: 0.4 cm3 min-1). Conclusion The removal efficiency of Lu(III) from the aqueous donor solution was very high when both static and continuous HF-LPE were applied, which is of prime importance with regard to the potential application in purification of 177Lu-based radiopharmaceuticals. The main advantage of continuous over static system is almost complete re-extraction of Lu(III) into the acceptor phase. Considering practical aspects, static HF-LPE is easier to operate, which is very important when working with radioactive material, and more suitable for low volume production, as is often the case in radiopharmaceutical production. Continuous HF-LPE requires higher volumes of donor phase for the operation and there are more potential leakage points that can cause accidental release of radioactive material.  Acknowledgment We acknowledge the support to this work provided by the Ministry of Education and Science of Serbia through project Physics and Chemistry with Ion Beams, No. III 45006. References [1] S. Banerjee et al., Nucl. Med. Biol., 2004, 31, 753-759. [2] K. Kumrić et al., Sep. Purif. Techn., 2006, 51, 310-317. [3] T. Trtić-Petrović et al., J. Sep. Sci., 2010, 33, 2002-2009. CIP Volime II  CIP - Каталогизација у публикацији Народна библиотека Србије, Београд  544(082) 621.35(082) 66.017/.018(082)  MEĐUNARODNA konferencija iz fundamentalne i  primenjene fizičke hemije (11 ; 2012 ;        Beograd)    Physical Chemistry 2012 : proceedings.     #Vol. #2 / 11th International Conference on   Fundamental and Applied Aspects of Physical   Chemistry, September 24-28, 2012, Belgrade ;  [editors S.[Slobodan] Anić and Ž.[Željko]     Čupić ; organized by Society of Physical      Chemists of Serbia ... et al.]. - Belgrade :  Society of Physical Chemists of Serbia, 2012  (Belgrade : Jovan). - VI str., 499-782 str. : ilustr. ; 24 cm  "The Conference is dedicated to Professor     Ivan Draganić" --> nasl. str. - Tiraž 200. - Bibliografija uz svaki rad. - Registar.  ISBN 978-86-82475-28-6 1. Društvo fizikohemičara Srbije (Beograd) a) Физичка хемија - Зборници b)             Електрохемијско инжењерство - Зборници c)  Наука о материјалима - Зборници COBISS.SR-ID 193433356 

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Comparison of static and continuous hollow fibre liquid-phase extraction of lutetium

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