Gold-Nanoparticle-Immobilized Desalting Columns for Highly Efficient

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Gold nanoparticles immobilized desalting columns for highly efficient and specific removal of radioactive iodine in aqueous media Mi Hee Choi, Ha-Eun Shim, Seong-Jae Yun, Sang-Hyun Park, Dae Seong Choi, Beom-su Jang, Yong Jun Choi, and Jongho Jeon ACS Appl. Mater. Interfaces, Just Accepted Manuscript • DOI: 10.1021/acsami.6b11136 • Publication Date (Web): 19 Oct 2016 Downloaded from http://pubs.acs.org on October 20, 2016

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ACS Applied Materials & Interfaces

Gold Nanoparticles Immobilized Desalting Columns for Highly Efficient and Specific Removal of Radioactive Iodine in Aqueous Media

Mi Hee Choi,a,† Ha-Eun Shim,a,b,† Seong-Jae Yun,a Sang-Hyun Park,a,c Dae Seong Choi,a Beom-Su Jang,a,c Yong Jun Choi*d and Jongho Jeon*a,c a

Advanced Radiation Technology Institute, Korea Atomic Energy Research Institute,

Jeongeup, Republic of Korea b

c

Department of Chemistry, Kyungpook National University, Daegu, Republic of Korea

Department of Radiation Biotechnology and Applied Radioisotope Science, University of

Science and Technology, Daejeon, Republic of Korea d

School of Environmental Engineering, The University of Seoul, Seoul, Republic of Korea

†

These authors contributed equally to this work.

Corresponding Authors *

E-mail: [email protected] [email protected]

Keywords: gold nanoparticles, radioactive iodine, desalination, remediation, radioactivity

Abstract There have been worldwide attentions on the efficient removal of radioactive iodine, because it is commonly released in nuclear plant accidents. Increasing concerns on environmental problems due to the radioactive iodine are leading us to develop stable and sustainable technology for remediation of radioelement contaminants. In this work, we report a highly efficient chromatographic method for specific and rapid capture of radioactive iodine. The gold nanoparticles immobilized dextran gel columns showed excellent removal capabilities of

ACS Paragon Plus Environment


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radioactive iodine in various conditions. These results suggested that our platform technology can be a promising method for the desalination of radioactive iodines in water.

For several decades, radioactive and nuclear waste treatment has been an important issue because large amount of radioactive contaminants frequently caused serious environmental problems. For examples, massive amount of radioactive iodine (129I,

131

I), which is believed

to cause adverse effects on lives such as thyroid cancer and chronic disease, has been released into the environment resulting from the recent accident at Fukushima nuclear reactors.1,2 Moreover, the huge amount of radioactive iodine were discarded into our circumstance as its use of radiation therapy and biomedical studies. Therefore, a lot of desalination processes employing various inorganic and organic adsorbents have been reported to remove radioactive iodine from the contaminated environment. For examples, metallic complexes,3-6 zeolites,7-10 activated carbons,11,12 organometallic frameworks13-15 and ionic liquids16,17 were investigated to capture iodine dissolved in aqueous or organic solvent. However, these processes showed either slow adsorption dynamics or low removal efficiency and thus relatively long time or large quantities of adsorbents were necessary to achieve satisfactory removal capabilities. There have been previous reports described that silver oxide anchored inorganic nanomaterials were able to enhance the removal efficiency of radioactive iodine.1820

However, most of these methods will require additional steps to separate solid radioactive

wastes from the water after the desalination procedure was accomplished by using adsorbents. Moreover, several metal adsorbents including mercury, silver cations and silver nanoparticles are known to possess significant toxicity in aqueous media.21-22 Therefore, these intrinsic drawbacks should be considered for the development of novel strategy desalinating radioactive iodine.


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Previous report indicated that the iodine ion is spontaneously chemisorbed on the surface of gold nanoparticles (AuNPs) due to the excellent affinity between gold and iodine atom.23 We have previously demonstrated that radioactive iodine (125I) was rapidly adsorbed on the surface of AuNPs and the radiolabeled materials were applied to in vivo imaging studies.24 By using the same chemical property, AuNPs based optical sensors for the selective detection of iodide ions have been reported.25 These results indicated that AuNPs can be applied to the efficient removal of radioactive iodine in aqueous media. In the present study, we report an efficient and convenient chromatographic method for ion-specific capture of radioactive iodine by using gold nanoparticles immobilized with dextran gel complex. As metal adsorbents known to have ability to capture the radioelement were incarcerated by the solid supports, our method will be used as an affinity chromatography to remove the radioactivity in water. Among various radioisotopes of iodine,

125

I was selected as a target

radioelement in this study due to a low radiation dose of radioactive iodines including

131

I. But the reactivity of

125

I compared to other

125

I is identical with other

iodine isotopes. First, we investigated the removal capability of AuNPs under several conditions including varying pH values and in the presence of competing anions. For this study, citrate stabilized AuNPs with mean diameter of 13 nm was modified with a polyethylene glycol thiol (PEG-SH, MW 5000) to retain the colloidal stability in high concentration of salt or extreme pH environments (See supporting information for detailed procedure on the surface modification of AuNPs). PEG coated AuNPs were mixed with increasing amount of [125I]NaI in pure water. The removal of radioactivity in aqueous solutions was highly depends on the ratio between AuNPs and radioactive iodine (Figure 1a). In the first 5 min, AuNPs could capture more than 94.0% of



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radioactivity in pure water containing up to 500-fold molar excess of

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125 -

I ions to

AuNPs (Table S1). The removal efficiency was increased up to 98.4% after 15 min as shown in Figure 1a, marked as red color. The maximum sorption capacity of PEG modified AuNPs for the uptake of

125 -

I ions was determined to be approximately 25

µmol/g at >68.4 nmol/L of the final concentration of

125 -

I ions (5 min contact time,

Figure S2). Specific radioactivity of [125I]NaI used in this study was 74 GBq/µmol. Theoretically, approximately 1850 GBq of [125I]NaI can be captured by 1 gram of PEG modified AuNPs. To investigate the desalination ability of AuNPs under the different conditions, we examined the specificity of AuNPs on

125 -

I ions using various pH solutions ([125I-

]/[AuNPs] = 500). As shown in Figure 1b, PEG coated AuNPs could adsorb more than 96% of

125 -

I ions in the acidic (pH = 1) solution, while the removal efficiency was

slightly decreased in the basic (pH = 13) solution (88.4%). It should be noted that most of 125I- ions were also rapidly adsorbed by AuNPs in 1.0 M NaCl and phosphate buffer saline (1 x PBS) solutions which contains high concentration of competing anions (Table S1 and Figure S2). However, the desalination activity of AuNPs was significantly inhibited in the presence of NaI because the surface of AuNPs was completely occupied by large amount of non-radioactive iodide ions. Based on these results, we can clearly demonstrate that AuNPs can efficiently and specifically capture 125 -

I ions in various conditions.

Next, the immobilization of AuNPs was studied by using several commercially available solid matrixes such as silica, alumina, C-18 silica cartridges. Unfortunately, citrate-stabilized AuNPs could not be trapped by using these columns or showed low colloidal stability during the experiments. On the other hand, a PD-10 column which contains cross-linked dextran gel could simply incarcerate the AuNPs by the following procedure. Citrate-stabilized AuNPs (10


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nM, 13 nm diameter) were slowly added to the column (Figure S4). After the AuNPs enter the packed bed completely, the resulting columns were washed with pure water to provide AuNPs immobilized desalting columns (Au-DC). We have prepared two columns, Au-DC10 and Au-DC30 using 10 mL and 30 mL of AuNPs, respectively (Figure 2a). AuNPs incarcerated in the desalting column did not elute nor undergoes aggregations by high concentration of salt solutions such as 1.0 M NaCl and PBS (1 x). Desalination studies were performed by adding a radioactive iodine solution (3.7 MBq of [125I]NaI in 50 mL pure water) to Au-DC (Figure 2b). The eluates from AuDC were collected and their radioactivities were measured by using a γ-counter. As shown in the table 1, 99.87% and 99.98% of

125 -

I in the eluent was removed by Au-

DC10 and Au-DC30, respectively. Even though small amount of radioactivity was detected in the PD-10 column, it seems to be the non-specific retention of iodine in the dextran gel matrix. The sustainability of

125 -

I -loaded Au-DC10 for radioactive iodine

adsorption was also examined. After 24 h of the desalination experiment,

125 -

I -loaded

Au-DC10 was washed with the same volume of water (50 mL). The amount of liberated radioactivity from the column was negligible, which showed nonreversibility of the adsorption process of Au-DC (data not shown). Desalination of [125I]NaI in several aqueous solutions have also been investigated using Au-DC10. Radioactive iodine (3.7 MBq) was dissolved in 50 mL of 1.0 M NaCl, phosphate buffer saline (1 x PBS, pH = 7.4), 1.0 M HCl and 0.1 M NaOH, and then each solution was applied to the column. As shown in Figure 3, over 99.5% of

125 -

I ions in the

presence of high concentration of salt and acidic solution were efficiently captured by Au-DC10 (Table S2). Notably, an excellent removal efficiency was still observed with 1.0 M NaCl solution which ratio of Cl- to

125 -

I anions ([Cl-]:[125I-]) was higher than

109:1. This result demonstrated that the distribution coefficient (Kd) was observed to



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be more than 4.7

x

106 (Table S2). Evidently, Au-DC showed excellent removal

efficiencies over a wide range of pH values and in high concentration of anions. Finally, the reusability and adsorption capability of Au-DC has been examined to evaluate its potential application for nuclear waste treatment. Because radioactive iodine has often been detected in the urinal excretion of thyroid cancer patient and in the ocean, radioactive iodine solutions were prepared by using a synthetic urine26 and commercially available sea water. Each solution (50 mL) containing 3.7 MBq of [125I]NaI were added to Au-DC10 and Au-DC30. The removal efficiencies were calculated by measuring the remaining radioactivity of the eluates. The same procedure was repeated for seven times at 24 h intervals. The results shown in Figure 4 demonstrated that less than 1% of removal efficiency was decreased during 7 days. Interestingly,

125 -

I anions adsorbed by AuNPs were not released from the column by

repetitive additions of sea water or synthetic urine. The observed removal efficiencies of Au-DC30 were slightly better than those of Au-DC10, however the capability of AuDC10 was high enough to separate most of radioelements from both aqueous solutions (Figure 4). There have been several previous reports described various adsorbents such as inorganic nanomaterials and metal-loaded zeolites. However these materials should be immersed into the contaminated water for removal of radioactive iodine. Compared to the previous studies, the method developed here could offer simpler and more efficient method to capture radioactivity in various aqueous solutions. By a single elution of [125I]NaI solution to a Au-DC, more than 99% of radioactivity was specifically captured by AuNPs and the whole desalination procedure of 50 mL aqueous solutions could be finished within 25 min. Because a large scale synthesis and nanocharacterization of the citrate stabilized AuNPs was well-established, a lot of Au-DC


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could be easily prepared in a short time. Additionally, AuNPs is known to show lower toxic effects than other metal adsorbents such as silver and mercury which have frequently been used for removal of I- anions.27 These advantages strongly demonstrated that the affinity chromatography using Au-DC will be potentially useful for efficient treatment of radioactive iodine wastes. To date, AuNPs have been employed in a wide range of applications for specific purposes including biosensor, catalyst, drug delivery and in vivo imaging/therapy due to their unique physical and chemical properties.28-30 To the best of our knowledge, this is the first report on applying AuNPs to the remediation of radioelement in contaminated water. In summary, we have successfully developed a new desalination method for efficient removal of radioactive iodine. Au-DC was easily prepared by using citrate-stabilized AuNPs and a commercially available desalting column. Au-DC could provide excellent removal capabilities and specificity under the various conditions such as varying pH values and the presence of competing ions. Therefore, we can conclude that Au-DC will be a promising adsorbent system worth investigating for industrial radioactive iodine removal process. Further optimization and validation of this process, and scale-up studies will be carried out to apply Au-DC to the remediation of various radioactive wastes.

Associated Content Supporting information



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Detailed experimental procedure for removal of radioactive iodine in aqueous solutions; Characterization of AuNPs using UV spectrum, TEM image, dynamic light scattering, and zeta potential analysis (Figure S1); Removal efficiency of radioactive iodine (125I) using PEG modified AuNPs (Table S1); Isotherm for

125 -

I ion uptake by

PEG modified AuNPs (Figure S2); Representative radio-TLC results (Figure S3); Schematic illustration for the preparation of Au-DC (Figure S4); Removal efficiency of radioactive iodine (125I) using Au-DC (Table S2). This material is available free of charge via the Internet at http://pubs.acs.org.

Acknowledgements This work was supported by the National Research Foundation of Korea grant funded by the Korea government (Grant nos. 2012M2B2B1055245 and 2012M2A2A6011335) and Korea Atomic Energy Research Institute.

Notes The authors declare no competing financial interest.

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Figures and table

Figure 1. Removal efficiency of [125I]NaI using PEG coated AuNPs a) pure water and b) various solutions.


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Figure 2. a) Desalting columns: PD-10 (left), Au-DC10 (middle), and Au-DC30 (right); b) Schematic illustration of the desalination procedure using Au-DC.

Figure 3. Removal efficiency of [125I]NaI in various solutions using Au-DC10.



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Figure 4. Removal efficiency of [125I]NaI using Au-DC10 and Au-DC30 a) synthetic urine and b) sea water.

Table 1 Removal efficiency of [125I]NaI in pure water using desalting columns Column

AuNPs (mol)

Removal efficiency (%)

Kd (mL g-1)

PD-10

0

< 3.00

-

Au-DC10

1.0 x 10-10

99.87

1.83 x 107

Au-DC30

3.0 x 10-10

99.98

3.97 x 107


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Graphic for manuscript (TOC graphic)


Gold-Nanoparticle-Immobilized Desalting Columns for Highly Efficient

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