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Removal of Radioactive Iodine Using Silver/Iron Oxide Composite Nanoadsorbents

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Removal of Radioactive Iodine Using Silver/Iron Oxide Composite Nanoadsorbents nanomaterials Communication Removal of Radioactive Iodine Using Silver/Iron Oxide Composite Nanoadsorbents Mah Rukh Zia 1,†, Muhammad Asim Raza 2,3,† , Sang Hyun Park 2,3 , Naseem Irfan 1, Rizwan Ahmed 1, Jung Eun Park 4, Jongho Jeon 4,* and Sajid Mushtaq 1,2,3,* 1 Department of Nuclear Engineering, Pakistan Institute of Engineering and Applied Sciences, P. O. Nilore, Islamabad 45650, Pakistan; [email protected] (M.R.Z.); [email protected] (N.I.); [email protected] (R.A.) 2 Advanced Radiation Technology Institute, Korea Atomic Energy Research Institute, Jeongeup 56212, Korea; [email protected] (M.A.R.); [email protected] (S.H.P.) 3 Radiation Science and Technology, University of Science and Technology, Daejeon 34113, Korea 4 Department of Applied Chemistry, College of Engineering, Kyungpook National University, Daegu 41566, Korea; [email protected] * Correspondence: [email protected] (J.J.); [email protected] (S.M.); Tel.: +82-53-950-5584 (J.J.); +92-51-9248611-3716 (S.M.) † These Authors contributed equally to this study. Abstract: Efficient and cost-effective removal of radioactive iodine (radioiodine) from radioactive contaminated water has become a crucial task, following nuclear power plant disasters. Several materials for removing radioiodine have been reported in the literature. However, most of these materials exhibit some limitations, such as high production cost, slow adsorption kinetics, and poor adsorption capacity. Herein, we present silver/iron oxide nanocomposites (Ag/Fe3O4) for the efficient and specific removal of iodine anions from contaminated water. The Ag/Fe3O4 were Citation: Zia, M.R.; Raza, M.A.; Park, synthesized using a modified method and characterized via scanning electron microscopy, transmis- S.H.; Irfan, N.; Ahmed, R.; Park, J.E.; Jeon, J.; Mushtaq, S. Removal of sion electron microscopy, and X-ray diffraction analyses. This adsorbent showed a high adsorption Radioactive Iodine Using Silver/Iron capacity for iodine anions (847 mg/g of the adsorbent) in pure water. Next, Ag/Fe3O4 was applied Oxide Composite Nanoadsorbents. to the removal of radioiodine, and high removal efficiencies were observed in water. In addition, Nanomaterials 2021, 11, 588. https:// its desalination capacity was retained in the presence of competitive ions and varied pH. After the doi.org/10.3390/nano11030588 adsorption process, Ag/Fe3O4 was easily removed from the water by applying an external magnetic field. Moreover, the same operation can be repeated several times without a significant decrease in Academic Editor: Christos the performance of Ag/Fe3O4. Therefore, it is expected that the findings presented in this study will A. Aggelopoulos offer a new method for desalinating radioiodine in various aqueous media. Received: 8 February 2021 Keywords: adsorbents; radioactive wastes; radioactive iodine; desalination; nanocomposites Accepted: 22 February 2021 Published: 26 February 2021 Publisher’s Note: MDPI stays neutral 1. Introduction with regard to jurisdictional claims in published maps and institutional affil- The safe and reliable treatment of radioactive waste is inevitably linked to the safe iations. production of nuclear energy [1,2]. Environmental damage caused by radioactive waste has attracted global attention. Radioisotopes, such as radioactive iodine (radioiodine), which exhibit a high degree of dispersion in water and air, are produced by nuclear fission. These can exert long-term adverse effects on human lives [3–5]. Notably, the global con- cern regarding nuclear waste leakage was kindled by the Fukushima accident in 2011 [6]. Copyright: © 2021 by the authors. Licensee MDPI, Basel, Switzerland. Further, the Chernobyl disaster in Ukraine occurred in 1986 wherein iodine radioisotopes This article is an open access article were a major component of the radioactive contamination [7]. Moreover, the continuous distributed under the terms and operation of nuclear power plants can produce and introduce trace amounts of radioiodine conditions of the Creative Commons into the environment [8]. Radioiodine has also been extensively used in the diagnosis Attribution (CC BY) license (https:// of diseases and treatment of thyroid cancer on the basis of the selective uptake of iodine creativecommons.org/licenses/by/ into the thyroid [9,10]. Consequently, the introduction of trace amounts of radioiodine 4.0/). from nuclear medicine research institutes also needs to be considered. For example, the Nanomaterials 2021, 11, 588. https://doi.org/10.3390/nano11030588 https://www.mdpi.com/journal/nanomaterials Nanomaterials 2021, 11, 588 2 of 12 Nanomaterials 2021, 11, 588 2 of 11 of iodine into the thyroid [9,10]. Consequently, the introduction of trace amounts of radi- oiodine from nuclear medicine research institutes also needs to be considered. For exam- ple, the medical applications of iodine-131 (131I; half-life: 8 days) and iodine-129 (129I; half- medical applications of iodine-131 (131I; half-life: 8 days) and iodine-129 (129I; half-life: 6 15.7life: ×15.710 ×6 years)10 years) are consideredare considered to be to thebe the main main generators generators of radioiodine of radioiodine waste waste [11 –[11–13]. The13]. The short-lived short-lived as well as well as long-livedas long-lived radioisotopes radioisotopes of of iodine iodine can can accumulate accumulate and and causecause serious damagedamage toto the the human human body. body. Therefore, Therefore, the the efficient efficient treatment treatment of radioactiveof radioactive iodine io- indine nuclear in nuclear wastes wastes and contaminated and contaminated water iswater an essential is an essential area of research.area of research. In past decades, In past variousdecades, adsorbents various adsorbents such as graphene-based such as graphene sorbents-based [14 sorbents,15], deep [14,15], eutectic deep solvents eutectic [16 ,17sol-], hydrogelatorsvents [16,17], hydrogelators [18], nanoporous [18], carbons nanoporous [19,20 carbons], polyacrylonitrile–chalcogel [19,20], polyacrylonitrile–chalcogel [21], microp- orous[21], microporous polymers [22 polymers–24], metal–organic [22–24], metal–organic frameworks frameworks (MOFs) [25,26 (MOFs)], and functionalized[25,26], and func- ze- olitestionalized [27,28 zeolites] were employed [27,28] we tore remove employed radioiodine to remove that radioiodine was dissolved that in was solutions dissolved and/or in gaseoussolutions radioiodine. and/or gaseous However, radioiodine. these materialsHowever, exhibitedthese materials several exhibited drawbacks, several including draw- lowbacks, removal including efficiency, low removal slow adsorption efficiency, kinetics, slow adsorption and high productionkinetics, and cost. high Furthermore, production layeredcost. Furthermore, bismuth–iodine–oxide layered bismuth–iodine–o [29], titanate nanolaminaxide [29], [30 titanate], Mg–Al(NO nanolamina3) layered [30], double Mg– hydroxideAl(NO3) layered (LDH) double [31], and hydroxide magnetite (LDH) composites [31], and [32, 33magnetite] have been composites employed [32,33] to remove have iodine.been employed However, to remove setbacks iodine. ranging However, from their setbacks poor reusabilityranging from to theirtheir lowpoor adsorption reusability capacitiesto their low have adsorption limited thecapacities application haveof limit theseed methods.the application In previous of these studies, methods. we reportedIn previ- thatous studies, gold nanoparticles we reported (AuNPs) that gold immobilized nanoparticles adsorbents (AuNPs) immobilized for the removal adsorbents of radioiodine for the anionsremoval in of aqueous radioiodine media anions [34–37 ].in The aqueous method me exhibiteddia [34–37]. efficient The method and ion-selective exhibited desalina-efficient tion;and ion-selective however, the desalination; high cost of AuNPs-basedhowever, the high systems cost hampered of AuNPs-based their large-scale systems hampered syntheses andtheir remediation large-scale syntheses applications. and remediation applications. Silver-based materials have also demonstrateddemonstrated aa greatgreat potentialpotential forfor removingremoving iodineiodine owing to the highhigh affinityaffinity ofof iodineiodine towardtoward silversilver [[3,38,39].3,38,39]. InIn aa typicaltypical procedureprocedure inin thethe previous studies,studies, silversilver nanoparticlesnanoparticles oror silver-basedsilver-based compositecomposite materialsmaterials werewere immersedimmersed inin the contaminated water to remove radioiodine.radioiodine. Thereafter, radioiodine containingcontaining solidsolid wastewaste waswas separatedseparated fromfrom thethe waterwater viavia filtrationfiltration oror centrifugation.centrifugation. However,However, mostmost ofof thesethese methodsmethods requirerequire furtherfurther stepssteps toto separateseparate solidsolid radioactiveradioactive wasteswastes fromfrom waterwater afterafter thethe desalinationdesalination procedure.procedure. Moreover, thethe separationseparation ofof nanosizednanosized adsorbentsadsorbents viavia thesethese methods is time-consuming and non-applicable at an industrial scale.scale. Thus, the develop- ment of additional cost-effective, efficientefficient remediationremediation proceduresprocedures forfor radioactiveradioactive wasteswastes isis still desired. desired. Here, Here, we we designed designed a stab a stablele and and efficient efficient silver/iron silver/iron oxide oxide (Ag/Fe (Ag/Fe3O4) nano-3O4) nanocomposite-basedcomposite-based desalination desalination system
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