Bioresource Technology 160 (2014) 142–149
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Adsorption removal of cesium from drinking waters: A mini review on use of biosorbents and other adsorbents Xiang Liu a,c, Guan-Ru Chen a, Duu-Jong Lee a,b,⇑, Tohru Kawamoto d, Hisashi Tanaka d, Man-Li Chen e, Yu-Kuo Luo e a
Department of Chemical Engineering, National Taiwan University, Taipei 106, Taiwan Department of Chemical Engineering, National Taiwan University of Science and Technology, Taipei 106, Taiwan Department of Environmental Engineering, Fudan University, Shanghai, China d National Institute of Advanced Industrial Science and Technology (AIST), 1-1-1 Higashi, Tsukuba 305-8565, Japan e Taipei Water Department, Taipei City Government, Taipei 106, Taiwan b c
h i g h l i g h t s Studies on adsorption removal of cesium from water are reviewed. Minerals, biosorbents, and synthesized composites were used as adsorbents. Demonstration tests were reported to highlight the points raised. Feasibility of using Prussian blue (PB) for large scale application is discussed.
a r t i c l e
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Article history: Available online 11 January 2014 Keywords: Adsorption Cesium Biosorbents Prussian blue
a b s t r a c t Radiocesium (Cs) removal from waters becomes an emerging issue after the Fukushima Daiichi Nuclear Power Plant Disaster, during which a total of approximately 3.3 1016 Bq Cs was released to contaminate the environment. This mini-review provided a summary on literature works to develop efficient adsorbent for removing Cs from waters. Adsorbent made of raw and modified minerals, composites particles, and biosorbents that are highly specific to Cs in the presence of other alkali and alkali earth metals were summarized. Development of Prussian blue (PB) nanoparticles on Cs removal and its potential use in drinking waterworks was discussed. This review is a unique report for adsorption removal of Cs from contaminated waters. Ó 2014 Elsevier Ltd. All rights reserved.
1. Introduction Radionuclides are a major concern to human health if they enter the environment. The East Japan Earthquake yielded major damage of Fukushima Daiichi Nuclear Power Plant (NPP), which released 630,000–770,000 TBq (terabecquerels) of radioactive nuclides such as 90Sr, 131I, 134Cs and 137Cs, into environment, leaving the region with contaminated soil, air, and water (Hu et al., 2012; Namiki et al., 2012). The venting of radioactive gases, hydrogen explosions, and fires associated with spent fuel rods resulted in the preferential release of more volatile radionuclides, such as Cs, and gases to the atmosphere (Buesseler et al., 2012). Radioactive Cs (137Cs) is of special concern due to its high radioactivity and long
⇑ Corresponding author at: Department of Chemical Engineering, National Taiwan University, Taipei 106, Taiwan. Tel.: +886 2 2363 5632; fax: +886 2 2362 3040. E-mail address: [email protected] (D.-J. Lee). 0960-8524/$ - see front matter Ó 2014 Elsevier Ltd. All rights reserved. http://dx.doi.org/10.1016/j.biortech.2014.01.012
half-life (30.2 yrs), which is much longer than 131I (8 days) (Namiki et al., 2012; Thammawong et al., 2013). The 137Cs levels in Japan before 2011 ranged 1–2 Bq m 3 (Aoyama and Hirose, 2004). The potential exposure of radioactivity one year after the Fukushima accident was contributed by 134Cs at approximately 1.8 1016 Bq and by 137Cs at approximately 1.5 1016 Bq (Parajuli et al., 2013). The 137Cs releases of from Chernobyl accident (3.8 1016 Bq) was comparable to 137Cs released by atmospheric nuclear weapons testing (1.3 1016 Bq) (Buesseler et al., 1987). (Note: 1 Bq indicates there is one nucleus decays in the medium per second. 1 Ci (curie) = 3.7 1010 Bq. 1 rem (roentgen equivalent in man) is 100 erg/g.) The best available technologies (BATs) and the small system compliance technologies (SSCTs) by US EPA (Radionuclides Final Rule, Dec. 7, 2000) for radionuclide removal from surface water and groundwater include ionic exchange, reverse osmosis, softening, enhanced coagulation/sedimentation, sand filtration, co-precipitation with BaSO4, electrodialysis/electrodialysis reversal,
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preformed hydrous manganese oxide filtration, and use of activated alumina. Any other methods that can meet the maximum contaminant level are also applicable. 131I has short half-life of about 8 days. As Summers et al. (1989) stated, the aquatic humic substances could form complex with 131I which can be easily removed in drinking water production process via flocculation or activated carbon adsorption. Conversely, Cs is water-soluble and behaves similarly to potassium and sodium in terrestrial ecosystems; hence, a high dose of 137Cs can induce medullar dystrophy, disorders of the reproductive function, and adverse effects on liver and renal functions. Cs is difficult to be removed from contaminated water (Thammawong et al., 2013). This mini-review provided a summary on current progress made on Cs removal using adsorption. In particular, an effort using Prussian blue as the specific adsorbent for Cs removal was highlighted.
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by activated carbon adsorption (30–40% removal). Conversely, the radiocesium in adsorbed form (on suspended particles) can be effectively removed by coagulation-sedimentation unit, however, the radiocesium ions cannot be removed by the waterworks. These authors mixed the cesium ions with sediments collected at sedimentation basin can improve Cs removal, likely owing to the adsorption occurring at the suspended particle surface. Brown et al. (2008) commented that the removal efficiencies of Cs in coagulation-sedimentation and sand filtration stage both ranged 10–40%. Apparently, when entering the waterworks, if the cesium is in bound form (with particles), conventional coagulation-sedimentation process can effectively remove the cesium from water. Conversely, if the cesium is in soluble form, conventional coagulation process has minimal removal to cesium.
3. Adsorption removal of cesium from waters 2. Removal of cesium in conventional waterworks Radioactive fallout can lead to contaminated surface water and/ or groundwater, eventually will enter drinking water production chain (Smith et al., 2001). The maximum contaminant levels for drinking water by U.S. EPA (2000) included uranium concentration < 30 lg l 1, combined activities of 226Ra and 228Ra < 5 pCi l 1, the gross alpha-particle activity K > NH4 > Na > Mg. Li et al. (2008) studied the use of vermiculite for Cs adsorption. At initial concentration of 30 lg l 1, addition of 20 g l 1 vermiculite removed 98% of Cs in 5 h testing (1.5 lg g 1). The presence of Na+, Ca2+ and NH4+ competes with the adsorption site with Cs. Bayulken et al. (2011) investigated the adsorption of Cs+ using Turkish clays, including bentonite, zeolite, sepiolite and kaolinite. These authors noted that bentonite and zeolite had higher Cs adsorption capacity than sepiolite and kaoline. Kim et al. (2013a) revealed that Yesan clay and zeolite could adsorb radioactive Cs at 1.865 and 9.055 lg g 1, respectively. Kim et al. (2013b) applied sericite to remove Cs and reached a maximum adsorption
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quantity of 6.68 mg g 1. Long et al. (2013) compared the Cs+ adsorption using ethylamine-modified montmorillonite (EthylMt) and calcium-saturated montmorillonite (Ca-Mt) and showed that Ethyl-Mt could be applied as an effective adsorbent for Cs+ removal due to its high adsorption capacity and adequate surface characteristics. Chitrakar et al. (2013) noted that the layered manganese oxide can adsorb Cs+ at 172 mg g 1 at pH 2–4 and 132 mg g 1 at pH 10. A montmorillonite-iron oxide composite (MIOC) was prepared to remove Cs+ from aqueous solution at maximum adsorption capacities of 52.6 mg g 1 and in a binary solution with Sr2+ with the corresponding maximum uptakes of Cs was 41.6 mg g 1 (Ararem et al., 2013). Du et al. (2013) prepared spherical PAN-based potassium nickel hexacyanoferrates (KNiCF) composite adsorbent for Cs removal. The PAN-KNiCF adsorbents had high selectivity for cesium removal and the distribution coefficients in the presence of co-ions followed Na+ > Mg2+ > Ca2+ > K+ > NH4+. Ding et al. (2013) compared the walnut shell only and the Nickel hexacyanoferrate (NiHCF)walnut shell on the removal of cesium from aqueous solution. The newly developed adsorbents had equilibrium cesium uptake of 0.5 mg g 1 and had overcame the difficulty of nanoparticle separation after use. Copper ferrocyanide (CuFC) was used as an adsorbent to remove cesium and reached better adsorption performance than the use of potassium zinc hexacyanoferrate (Han et al., 2012). Tasdelen et al. (2013) used N-isopropylacrylamide/itaconic acid (NIPAAm/IA) hydrogels as adsorbent for the removal of radioactive cesium in the aquatic system. Biosorbents were tested for Cs removal. Krishna et al. (2004a) applied Funaria hygrometrica to adsorb 90Sr and 137Cs from low strength radioactive waste. The NaOH pretreated biosorbent had adsorption capacities of 137Cs at 38 mg g 1. These authors revealed that the –COO group was corresponding to the radionuclide adsorption. Krishna et al. (2004b) fixed Funaria hygrometrica to polysilicates and then tested the adsorption of 90Sr and 137Cs under continuous flow mode. At pH 5–10 and contact time of 30 min, the adsorption quantity of 137Cs was 15 mg g 1. The biosorbent can be satisfactorily regenerated using 0.2 M nitric acid solution. Dahiya et al. (2008) applied pretreated betel nut shell to adsorb Pb2+, Cu2+, Co2+ and Cs+ from water, with the maximum adsorption quantities of 3.93 ± 0.11 mg g 1 for Cs+. Effects of pH, initial concentrations of metals, biosorbent quantities and contact time were discussed. Ofomaja et al. (2013) applied chemically treated pine
cone and examined its adsorption capacity to Cs+. These authors noted that the diffusion-chemisorption model fit well the kinetic data, while the ions of Cs+, Na+ and Ca2+ were competing with the same site on the adsorbent. The authors also argued that since the ionic radii of Ca2+ (0.99 Å) and Na+ (1.02 Å) are smaller than Cs+ (1.67 Å), hence the addition of the former two would reduce the adsorption capacity of latter. Some studies suggested unfavorable adsorption tests using studied adsorbents. Caccin et al. (2013) investigate the adsorption of cesium onto coconut shell activated carbon but revealed poor affinity between cesium and the activated carbon with adsorption capacities 1.5 g l 1 montmorillonite can remove 90% of dosed, 30 ppb Cs+, yielding an adsorption capacity of 18 mg g 1. The reported results showed that the nature of species (kaolin or montmorillonite) and the dosage significantly affected the adsorption behavior of Cs+. Just with the very favorable adsorption with montmorillonite the adsorption quantity is still low. 100
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As discussed above, the adsorption of Cs using common adsorbents is low in adsorption capacity. Additionally, since alkali and alkali earth metals are shown to be capable of competing with Cs for the adsorption sites, Cs adsorbents that are highly specific to Cs rather than to other alkali and alkali earth metals are needed. In the next section, the use of an old dye, Prussian blue (PB) on Cs adsorption is discussed. 4. Use of Prussian blue on cesium removal 4.1. PB nanoparticles PB is a pigment of dark blue color with chemical formula Fe7(CN)18. PB has simple face-centered lattice structure with eight water molecules exist in the unit cell. The pharmaceutical-grade PB was used as adsorbent to remove Cs from patient body after the Chemobyl disaster in 1987. After the Fukushima Daiichi nuclear disaster, PB was used as adsorbent in decontamination of radioactive cesium because of its high selectivity of cesium. This observation correlated with the hydration radii of the cations in the order of Cs+ (3.25 Å), followed by K+ (3.3 Å), Na+ (3.6 Å), Ca2+ (4.1 Å), and Mg2+ (4.25 Å), with the hydrated ions of Cs just fit the cage size of PB lattice (Thammawong et al., 2013). Ishizaki et al. (2013) revealed that the synthesized PB nanoparticles (Fe4(Fe(CN)6)3 with many hydrophilic defect sites has supreme Cs adsorption capability and proposed that the Cs+ ions were adsorbed onto the defect sites of nanoparticles by proton-elimination reaction from the coordinated waters. This section highlighted the use of PB as a promising adsorbent for Cs from waters. Ideally, for a unit cell (2 2 2), the Cs:Fe ratio is 1:8 after adsorption. With infinitely large lattice (n n n) and assuming all cavities can intake Cs, the stoichiometry can reach Cs:Fe = 1:1 ((n 1)3/n3 at very large n). However, very large lattice definitely reduce adsorption rate. Hence, nano-size PB particles are preferred in drinking water production so adsorption can be achieved in a few tens of seconds. Gotoh et al. (2007) synthesized three kinds of nanoparticles of PB and its analogues with surface modification using aliphalic amines which can stay stably in dispersed state. The nanoparticles are water soluble to form transient suspension of the particles. Hara et al. (2007) dispersed the PB nanoparticles with alkyl-ligand covered surface in organic solvents to do thin film fabrication. Shiozaki et al. (2008) dispersed the surface modified nanoparticles of PB in aqueous solution then formed thin PB film of thickness of 40–430 nm on indium tin oxide glass by spin-coating technique. Omura et al. (2008) modified the PB nanoparticles by coating with ferrocyanide anions and dispersed them into water. The thin film can be then fabricated using these water-dispersed PB nanoparticles. With these techniques, the PB nanoparticles can be coated in the form of thin films for further applications. The small size of PB nanoparticles provides them very large specific surface area for enhancing adsorption capability. Nanocomposites based on functionalized silica or glass matrices containing 99.99% at 420 s contact time (Fig. 2a), with an adsorption capacity of 241 mg g 1, which was much higher than montmorillonite (Fig. 1) and vermiculite (Li et al., 2008) at the same initial Cs concentration. The effluent turbidity, pH and electric conductivity were not affected by the fabric filtration (Fig. 2b–d). The noted pressure drop was at superficial velocity of 1 m h 1 were all below 1 m H2O, suitable for practice for waterworks. This observation provides a great potential for using PB as Cs adsorbent for drinking water production (Table 1).
In drinking production, the radiocesium removal should reach the highest level possible for not only minimizing adverse effects on human health but also providing psychological supports to residents. Conventional drinking water process can minimally remove radiocesium is a frustrating truth; while, owing to the completely soluble nature and low surface charge of cesium ions in water, most available adsorbents can not reach sufficient removal efficiencies via mechanisms such as hydrophobic interaction, electrostatic interaction, or surface complexation. The PB, on the contrary, adopting ion trapping mechanisms with the cage size just fits that of hydrated cesium ions, presents a very promising option as a cesium-adsorbent at low cost. Ways of maximizing the surface area of PB particles and the binding strength of PB particles to carrier medium are currently looked for. 5. Conclusion This mini-review summarized the literature works for developing highly selective Cs adsorbent, with focus on its use in drinking water production. Demonstration tests confirmed the incapability of conventional drinking waterworks for removing soluble Cs from water. The adsorbents including raw and modified minerals,
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. (a) Cs removal rarios versus contact
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X. Liu et al. / Bioresource Technology 160 (2014) 142–149 Table 1 Recent works for Cs absorbents considering maximum adsorption capacity. Adsorbent
Batch and continuous fixed-bed column adsorption of Cs+ and Sr2+ onto montmorillonite-iron oxide composite: Comparative and competitive study Adsorption of uranium, cesium and strontium onto coconut shell activated carbon Adsorption of cesium from aqueous solution using agricultural residue – Walnut shell: Equilibrium, kinetic and thermodynamic modeling studies Cesium removal from solution using PAN-based potassium nickel hexacyanoferrate (II) composite spheres Adsorption characteristics of sericite for cesium ions from an aqueous solution Evaluation of Cs+ removal from aqueous solution by adsorption on ethylamine-modified montmorillonite The adsorption behavior of cesium on poly(N-isopropylacrylamide/itaconic acid) copolymeric hydrogels Prussian blue-coated magnetic nanoparticles for removal of cesium from contaminated environment Prussian blue caged in alginate/calcium beads as adsorbents for removal of cesium ions from contaminated water
Montmorillonite-iron oxide composite (MIOC)
52.6
Ararem et al. (2013)
Coconut shell activated carbon
55.32
Caccin et al. (2013) Ding et al. (2013) Du et al. (2013) Kim et al. (2013b) Long et al. (2013) Tasdelen et al. (2013) Thammawong et al. (2013) Vipin et al. (2013)
Extraction of radioactive cesium using innovative functionalized porous materials Prussian blue caged in spongiform adsorbents using diatomite and carbon nanotubes for elimination of cesium Magnetic Separation of cesium ion using prussian blue modified magnetite Large Cs adsorption capability of nanostructured Prussian Blue particles with high accessible surface areas Adsorption of cesium (I) from aqueous solution using oxidized multiwall carbon nanotubes Removal of cobalt, strontium and cesium from radioactive laundry wastewater by ammonium molybdophosphate–polyacrylonitrile (AMP– PAN) Selective capture of cesium and thallium from natural waters and simulated wastes with copper ferrocyanide functionalized mesoporous silica Performance of phosphoric acid activated montmorillonite as buffer materials for radioactive waste repository Rubidium and cesium ion adsorption by an ammonium molybdophosphate– calcium alginate composite adsorbent Removal of Pb2+, Ag+, Cs+ and Sr2+ from aqueous solution by brewery’s waste biomass Biosorption of heavy metals and radionuclide from aqueous solutions by pre-treated arca shell biomass Biosorption of cesium-137 and strontium-90 by mucilaginous seeds of Ocimum basilicum Removal of 137Cs and 90Sr from actual low level radioactive waste solutions using moss as a phyto-sorbent.
Nickel hexacyanoferrate–walnut shell Polyacrylonitrile–potassium nickel hexacyanoferrates composite Sericite Ethylamine-modified montmorillonite N-isopropylacrylamide/itaconic acid (NIPAAm/IA) hydrogels Prussian blue-coated magnetic nanoparticles Prussian blue caged in alginate/calcium beads Prussian blue caged in alginate/calcium beads reinforced with carbon nanotubes Prussian blue analogues Co3[Fe(CN)6]2 H2O (CoFC) Prussian blue alone Prussian blue caged in spongiform Prussian-blue-modified magnetite (PB–Fe3O4) Hollow Prussian Blue nanoparticles with 190 nm in diameter Commercial PB particles Oxidized multiwall carbon nanotubes Ammonium molybdophosphate– polyacrylonitrile Copper ferrocyanide functionalized mesoporous silica Phosphoric acid activated montmorillonite Ammonium molybdophosphate–calcium alginate composite adsorbent Brewery’s waste biomass Pre-treated arca shell biomass Mucilaginous seeds of Ocimum basilicum Moss NaOH treated moss
composites particles, biosorbents were tested for Cs removal. Only PB analogues could reach 99.99% removal of Cs from waters. The potential application of PB-impregnated nonwoven fabric for Cs removal in waterworks was reported. Acknowledgements This work is financially supported by the Taipei Water Department, Taipei City Government. References Aksu, Z., 2005. Application of biosorption for the removal of organic pollutants: A review. Process Biochem. 40, 997–1026. Annadurai, G., Juang, R.S., Lee, D.J., 2002. Use of cellulose-based wastes for adsorption of dyes from aqueous solutions. J. Hazard. Mater. 92 (3), 263–274.
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17.1 (seawater, pH 7.7) 208.0 91.8 10.1 3.93 160 6 17
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Smith, J.T., Voitsekhovitch, O.V., Hakanson, L., Hilton, J., 2001. A critical review of measures of reduce radioactive doses from drinking water and consumption of freshwater foodstuffs. J. Environ. Radioact. 56, 11–32. Summers, R.S., Fuchs, F., Sontheimer, H., 1989. The fate and removal of radioactive iodine in the aquatic environment. Am. Chem. Soc., Symp. Series. ACS Publications. pp. 623–636. Suzuki, S., Ozawa, S., Ochi, K., Chikuma, T., Watanabe, Y., 2013. Approaches for cesium uptake by vermiculite. J. Chem. Technol. Biotechnol. 88, 1603– 1605. Tasdelen, B., Osmanlioglu, A.E., Kam, E., 2013. The adsorption behavior of cesium on poly (N-isopropylacrylamide/itaconic acid) copolymeric hydrogels. Polym. Bull. 70 (11), 3041–3053. Thammawong, C., Opaprakasit, P., Tangboriboonrat, P., Sreearunothai, P., 2013. Prussian blue-coated magnetic nanoparticles for removal of cesium from contaminated environment. J. Nanopart. Res. 15, 1689. Torad, N.L., Hu, M., Imura, M., Naito, M., Yamauchi, Y., 2012. Large Cs adsorption capability of nanostructured Prussian blue particles with high accessible surface areas. J. Mater. Chem. 22 (35), 18261–18267. Wang, J., Chen, C., 2009. Biosorbents for heavy metals removal and their future. Biotechnol. Adv. 27 (2), 195–226. U.S. Epa (United States Environmental Protection Agency), 2000. 40 CFR Parts 141 and 142. National Primary Drinking Water Regulations; Radionuclides; Notice of Data Availability. Fed. Reg. 65, 21576–21628. Vijayaraghavan, K., Yun, Y.S., 2008. Bacterial biosorbents and biosorption. Biotechnol. Adv. 26 (3), 266–291. Vipin, A.K., Hu, B., Fugetsu, B., 2013. Prussian blue caged in alginate/calcium beads as adsorbents for removal of cesium ions from contaminated water. J. Hazard. Mater. 258, 93–101.
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Adsorption removal of cesium from drinking waters: A mini review on use of biosorbents and other adsorbents Xiang Liu a,c, Guan-Ru Chen a, Duu-Jong Lee a,b,⇑, Tohru Kawamoto d, Hisashi Tanaka d, Man-Li Chen e, Yu-Kuo Luo e a
Department of Chemical Engineering, National Taiwan University, Taipei 106, Taiwan Department of Chemical Engineering, National Taiwan University of Science and Technology, Taipei 106, Taiwan Department of Environmental Engineering, Fudan University, Shanghai, China d National Institute of Advanced Industrial Science and Technology (AIST), 1-1-1 Higashi, Tsukuba 305-8565, Japan e Taipei Water Department, Taipei City Government, Taipei 106, Taiwan b c
h i g h l i g h t s Studies on adsorption removal of cesium from water are reviewed. Minerals, biosorbents, and synthesized composites were used as adsorbents. Demonstration tests were reported to highlight the points raised. Feasibility of using Prussian blue (PB) for large scale application is discussed.
a r t i c l e
i n f o
Article history: Available online 11 January 2014 Keywords: Adsorption Cesium Biosorbents Prussian blue
a b s t r a c t Radiocesium (Cs) removal from waters becomes an emerging issue after the Fukushima Daiichi Nuclear Power Plant Disaster, during which a total of approximately 3.3 1016 Bq Cs was released to contaminate the environment. This mini-review provided a summary on literature works to develop efficient adsorbent for removing Cs from waters. Adsorbent made of raw and modified minerals, composites particles, and biosorbents that are highly specific to Cs in the presence of other alkali and alkali earth metals were summarized. Development of Prussian blue (PB) nanoparticles on Cs removal and its potential use in drinking waterworks was discussed. This review is a unique report for adsorption removal of Cs from contaminated waters. Ó 2014 Elsevier Ltd. All rights reserved.
1. Introduction Radionuclides are a major concern to human health if they enter the environment. The East Japan Earthquake yielded major damage of Fukushima Daiichi Nuclear Power Plant (NPP), which released 630,000–770,000 TBq (terabecquerels) of radioactive nuclides such as 90Sr, 131I, 134Cs and 137Cs, into environment, leaving the region with contaminated soil, air, and water (Hu et al., 2012; Namiki et al., 2012). The venting of radioactive gases, hydrogen explosions, and fires associated with spent fuel rods resulted in the preferential release of more volatile radionuclides, such as Cs, and gases to the atmosphere (Buesseler et al., 2012). Radioactive Cs (137Cs) is of special concern due to its high radioactivity and long
⇑ Corresponding author at: Department of Chemical Engineering, National Taiwan University, Taipei 106, Taiwan. Tel.: +886 2 2363 5632; fax: +886 2 2362 3040. E-mail address: [email protected] (D.-J. Lee). 0960-8524/$ - see front matter Ó 2014 Elsevier Ltd. All rights reserved. http://dx.doi.org/10.1016/j.biortech.2014.01.012
half-life (30.2 yrs), which is much longer than 131I (8 days) (Namiki et al., 2012; Thammawong et al., 2013). The 137Cs levels in Japan before 2011 ranged 1–2 Bq m 3 (Aoyama and Hirose, 2004). The potential exposure of radioactivity one year after the Fukushima accident was contributed by 134Cs at approximately 1.8 1016 Bq and by 137Cs at approximately 1.5 1016 Bq (Parajuli et al., 2013). The 137Cs releases of from Chernobyl accident (3.8 1016 Bq) was comparable to 137Cs released by atmospheric nuclear weapons testing (1.3 1016 Bq) (Buesseler et al., 1987). (Note: 1 Bq indicates there is one nucleus decays in the medium per second. 1 Ci (curie) = 3.7 1010 Bq. 1 rem (roentgen equivalent in man) is 100 erg/g.) The best available technologies (BATs) and the small system compliance technologies (SSCTs) by US EPA (Radionuclides Final Rule, Dec. 7, 2000) for radionuclide removal from surface water and groundwater include ionic exchange, reverse osmosis, softening, enhanced coagulation/sedimentation, sand filtration, co-precipitation with BaSO4, electrodialysis/electrodialysis reversal,
X. Liu et al. / Bioresource Technology 160 (2014) 142–149
preformed hydrous manganese oxide filtration, and use of activated alumina. Any other methods that can meet the maximum contaminant level are also applicable. 131I has short half-life of about 8 days. As Summers et al. (1989) stated, the aquatic humic substances could form complex with 131I which can be easily removed in drinking water production process via flocculation or activated carbon adsorption. Conversely, Cs is water-soluble and behaves similarly to potassium and sodium in terrestrial ecosystems; hence, a high dose of 137Cs can induce medullar dystrophy, disorders of the reproductive function, and adverse effects on liver and renal functions. Cs is difficult to be removed from contaminated water (Thammawong et al., 2013). This mini-review provided a summary on current progress made on Cs removal using adsorption. In particular, an effort using Prussian blue as the specific adsorbent for Cs removal was highlighted.
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by activated carbon adsorption (30–40% removal). Conversely, the radiocesium in adsorbed form (on suspended particles) can be effectively removed by coagulation-sedimentation unit, however, the radiocesium ions cannot be removed by the waterworks. These authors mixed the cesium ions with sediments collected at sedimentation basin can improve Cs removal, likely owing to the adsorption occurring at the suspended particle surface. Brown et al. (2008) commented that the removal efficiencies of Cs in coagulation-sedimentation and sand filtration stage both ranged 10–40%. Apparently, when entering the waterworks, if the cesium is in bound form (with particles), conventional coagulation-sedimentation process can effectively remove the cesium from water. Conversely, if the cesium is in soluble form, conventional coagulation process has minimal removal to cesium.
3. Adsorption removal of cesium from waters 2. Removal of cesium in conventional waterworks Radioactive fallout can lead to contaminated surface water and/ or groundwater, eventually will enter drinking water production chain (Smith et al., 2001). The maximum contaminant levels for drinking water by U.S. EPA (2000) included uranium concentration < 30 lg l 1, combined activities of 226Ra and 228Ra < 5 pCi l 1, the gross alpha-particle activity K > NH4 > Na > Mg. Li et al. (2008) studied the use of vermiculite for Cs adsorption. At initial concentration of 30 lg l 1, addition of 20 g l 1 vermiculite removed 98% of Cs in 5 h testing (1.5 lg g 1). The presence of Na+, Ca2+ and NH4+ competes with the adsorption site with Cs. Bayulken et al. (2011) investigated the adsorption of Cs+ using Turkish clays, including bentonite, zeolite, sepiolite and kaolinite. These authors noted that bentonite and zeolite had higher Cs adsorption capacity than sepiolite and kaoline. Kim et al. (2013a) revealed that Yesan clay and zeolite could adsorb radioactive Cs at 1.865 and 9.055 lg g 1, respectively. Kim et al. (2013b) applied sericite to remove Cs and reached a maximum adsorption
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quantity of 6.68 mg g 1. Long et al. (2013) compared the Cs+ adsorption using ethylamine-modified montmorillonite (EthylMt) and calcium-saturated montmorillonite (Ca-Mt) and showed that Ethyl-Mt could be applied as an effective adsorbent for Cs+ removal due to its high adsorption capacity and adequate surface characteristics. Chitrakar et al. (2013) noted that the layered manganese oxide can adsorb Cs+ at 172 mg g 1 at pH 2–4 and 132 mg g 1 at pH 10. A montmorillonite-iron oxide composite (MIOC) was prepared to remove Cs+ from aqueous solution at maximum adsorption capacities of 52.6 mg g 1 and in a binary solution with Sr2+ with the corresponding maximum uptakes of Cs was 41.6 mg g 1 (Ararem et al., 2013). Du et al. (2013) prepared spherical PAN-based potassium nickel hexacyanoferrates (KNiCF) composite adsorbent for Cs removal. The PAN-KNiCF adsorbents had high selectivity for cesium removal and the distribution coefficients in the presence of co-ions followed Na+ > Mg2+ > Ca2+ > K+ > NH4+. Ding et al. (2013) compared the walnut shell only and the Nickel hexacyanoferrate (NiHCF)walnut shell on the removal of cesium from aqueous solution. The newly developed adsorbents had equilibrium cesium uptake of 0.5 mg g 1 and had overcame the difficulty of nanoparticle separation after use. Copper ferrocyanide (CuFC) was used as an adsorbent to remove cesium and reached better adsorption performance than the use of potassium zinc hexacyanoferrate (Han et al., 2012). Tasdelen et al. (2013) used N-isopropylacrylamide/itaconic acid (NIPAAm/IA) hydrogels as adsorbent for the removal of radioactive cesium in the aquatic system. Biosorbents were tested for Cs removal. Krishna et al. (2004a) applied Funaria hygrometrica to adsorb 90Sr and 137Cs from low strength radioactive waste. The NaOH pretreated biosorbent had adsorption capacities of 137Cs at 38 mg g 1. These authors revealed that the –COO group was corresponding to the radionuclide adsorption. Krishna et al. (2004b) fixed Funaria hygrometrica to polysilicates and then tested the adsorption of 90Sr and 137Cs under continuous flow mode. At pH 5–10 and contact time of 30 min, the adsorption quantity of 137Cs was 15 mg g 1. The biosorbent can be satisfactorily regenerated using 0.2 M nitric acid solution. Dahiya et al. (2008) applied pretreated betel nut shell to adsorb Pb2+, Cu2+, Co2+ and Cs+ from water, with the maximum adsorption quantities of 3.93 ± 0.11 mg g 1 for Cs+. Effects of pH, initial concentrations of metals, biosorbent quantities and contact time were discussed. Ofomaja et al. (2013) applied chemically treated pine
cone and examined its adsorption capacity to Cs+. These authors noted that the diffusion-chemisorption model fit well the kinetic data, while the ions of Cs+, Na+ and Ca2+ were competing with the same site on the adsorbent. The authors also argued that since the ionic radii of Ca2+ (0.99 Å) and Na+ (1.02 Å) are smaller than Cs+ (1.67 Å), hence the addition of the former two would reduce the adsorption capacity of latter. Some studies suggested unfavorable adsorption tests using studied adsorbents. Caccin et al. (2013) investigate the adsorption of cesium onto coconut shell activated carbon but revealed poor affinity between cesium and the activated carbon with adsorption capacities 1.5 g l 1 montmorillonite can remove 90% of dosed, 30 ppb Cs+, yielding an adsorption capacity of 18 mg g 1. The reported results showed that the nature of species (kaolin or montmorillonite) and the dosage significantly affected the adsorption behavior of Cs+. Just with the very favorable adsorption with montmorillonite the adsorption quantity is still low. 100
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As discussed above, the adsorption of Cs using common adsorbents is low in adsorption capacity. Additionally, since alkali and alkali earth metals are shown to be capable of competing with Cs for the adsorption sites, Cs adsorbents that are highly specific to Cs rather than to other alkali and alkali earth metals are needed. In the next section, the use of an old dye, Prussian blue (PB) on Cs adsorption is discussed. 4. Use of Prussian blue on cesium removal 4.1. PB nanoparticles PB is a pigment of dark blue color with chemical formula Fe7(CN)18. PB has simple face-centered lattice structure with eight water molecules exist in the unit cell. The pharmaceutical-grade PB was used as adsorbent to remove Cs from patient body after the Chemobyl disaster in 1987. After the Fukushima Daiichi nuclear disaster, PB was used as adsorbent in decontamination of radioactive cesium because of its high selectivity of cesium. This observation correlated with the hydration radii of the cations in the order of Cs+ (3.25 Å), followed by K+ (3.3 Å), Na+ (3.6 Å), Ca2+ (4.1 Å), and Mg2+ (4.25 Å), with the hydrated ions of Cs just fit the cage size of PB lattice (Thammawong et al., 2013). Ishizaki et al. (2013) revealed that the synthesized PB nanoparticles (Fe4(Fe(CN)6)3 with many hydrophilic defect sites has supreme Cs adsorption capability and proposed that the Cs+ ions were adsorbed onto the defect sites of nanoparticles by proton-elimination reaction from the coordinated waters. This section highlighted the use of PB as a promising adsorbent for Cs from waters. Ideally, for a unit cell (2 2 2), the Cs:Fe ratio is 1:8 after adsorption. With infinitely large lattice (n n n) and assuming all cavities can intake Cs, the stoichiometry can reach Cs:Fe = 1:1 ((n 1)3/n3 at very large n). However, very large lattice definitely reduce adsorption rate. Hence, nano-size PB particles are preferred in drinking water production so adsorption can be achieved in a few tens of seconds. Gotoh et al. (2007) synthesized three kinds of nanoparticles of PB and its analogues with surface modification using aliphalic amines which can stay stably in dispersed state. The nanoparticles are water soluble to form transient suspension of the particles. Hara et al. (2007) dispersed the PB nanoparticles with alkyl-ligand covered surface in organic solvents to do thin film fabrication. Shiozaki et al. (2008) dispersed the surface modified nanoparticles of PB in aqueous solution then formed thin PB film of thickness of 40–430 nm on indium tin oxide glass by spin-coating technique. Omura et al. (2008) modified the PB nanoparticles by coating with ferrocyanide anions and dispersed them into water. The thin film can be then fabricated using these water-dispersed PB nanoparticles. With these techniques, the PB nanoparticles can be coated in the form of thin films for further applications. The small size of PB nanoparticles provides them very large specific surface area for enhancing adsorption capability. Nanocomposites based on functionalized silica or glass matrices containing 99.99% at 420 s contact time (Fig. 2a), with an adsorption capacity of 241 mg g 1, which was much higher than montmorillonite (Fig. 1) and vermiculite (Li et al., 2008) at the same initial Cs concentration. The effluent turbidity, pH and electric conductivity were not affected by the fabric filtration (Fig. 2b–d). The noted pressure drop was at superficial velocity of 1 m h 1 were all below 1 m H2O, suitable for practice for waterworks. This observation provides a great potential for using PB as Cs adsorbent for drinking water production (Table 1).
In drinking production, the radiocesium removal should reach the highest level possible for not only minimizing adverse effects on human health but also providing psychological supports to residents. Conventional drinking water process can minimally remove radiocesium is a frustrating truth; while, owing to the completely soluble nature and low surface charge of cesium ions in water, most available adsorbents can not reach sufficient removal efficiencies via mechanisms such as hydrophobic interaction, electrostatic interaction, or surface complexation. The PB, on the contrary, adopting ion trapping mechanisms with the cage size just fits that of hydrated cesium ions, presents a very promising option as a cesium-adsorbent at low cost. Ways of maximizing the surface area of PB particles and the binding strength of PB particles to carrier medium are currently looked for. 5. Conclusion This mini-review summarized the literature works for developing highly selective Cs adsorbent, with focus on its use in drinking water production. Demonstration tests confirmed the incapability of conventional drinking waterworks for removing soluble Cs from water. The adsorbents including raw and modified minerals,
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Fig. 2. Adsorption test using PB-impregnated nonwoven fabric. Feed: 30 ppb Cs, 0.4 NTU turbidity, pH 7.0, conductivity 102 lS cm time; (b) effluent turbidity versus contact time; (c) effluent pH versus contact time; (d) effluent conductivity versus contact time.
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. (a) Cs removal rarios versus contact
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X. Liu et al. / Bioresource Technology 160 (2014) 142–149 Table 1 Recent works for Cs absorbents considering maximum adsorption capacity. Adsorbent
Batch and continuous fixed-bed column adsorption of Cs+ and Sr2+ onto montmorillonite-iron oxide composite: Comparative and competitive study Adsorption of uranium, cesium and strontium onto coconut shell activated carbon Adsorption of cesium from aqueous solution using agricultural residue – Walnut shell: Equilibrium, kinetic and thermodynamic modeling studies Cesium removal from solution using PAN-based potassium nickel hexacyanoferrate (II) composite spheres Adsorption characteristics of sericite for cesium ions from an aqueous solution Evaluation of Cs+ removal from aqueous solution by adsorption on ethylamine-modified montmorillonite The adsorption behavior of cesium on poly(N-isopropylacrylamide/itaconic acid) copolymeric hydrogels Prussian blue-coated magnetic nanoparticles for removal of cesium from contaminated environment Prussian blue caged in alginate/calcium beads as adsorbents for removal of cesium ions from contaminated water
Montmorillonite-iron oxide composite (MIOC)
52.6
Ararem et al. (2013)
Coconut shell activated carbon
55.32
Caccin et al. (2013) Ding et al. (2013) Du et al. (2013) Kim et al. (2013b) Long et al. (2013) Tasdelen et al. (2013) Thammawong et al. (2013) Vipin et al. (2013)
Extraction of radioactive cesium using innovative functionalized porous materials Prussian blue caged in spongiform adsorbents using diatomite and carbon nanotubes for elimination of cesium Magnetic Separation of cesium ion using prussian blue modified magnetite Large Cs adsorption capability of nanostructured Prussian Blue particles with high accessible surface areas Adsorption of cesium (I) from aqueous solution using oxidized multiwall carbon nanotubes Removal of cobalt, strontium and cesium from radioactive laundry wastewater by ammonium molybdophosphate–polyacrylonitrile (AMP– PAN) Selective capture of cesium and thallium from natural waters and simulated wastes with copper ferrocyanide functionalized mesoporous silica Performance of phosphoric acid activated montmorillonite as buffer materials for radioactive waste repository Rubidium and cesium ion adsorption by an ammonium molybdophosphate– calcium alginate composite adsorbent Removal of Pb2+, Ag+, Cs+ and Sr2+ from aqueous solution by brewery’s waste biomass Biosorption of heavy metals and radionuclide from aqueous solutions by pre-treated arca shell biomass Biosorption of cesium-137 and strontium-90 by mucilaginous seeds of Ocimum basilicum Removal of 137Cs and 90Sr from actual low level radioactive waste solutions using moss as a phyto-sorbent.
Nickel hexacyanoferrate–walnut shell Polyacrylonitrile–potassium nickel hexacyanoferrates composite Sericite Ethylamine-modified montmorillonite N-isopropylacrylamide/itaconic acid (NIPAAm/IA) hydrogels Prussian blue-coated magnetic nanoparticles Prussian blue caged in alginate/calcium beads Prussian blue caged in alginate/calcium beads reinforced with carbon nanotubes Prussian blue analogues Co3[Fe(CN)6]2 H2O (CoFC) Prussian blue alone Prussian blue caged in spongiform Prussian-blue-modified magnetite (PB–Fe3O4) Hollow Prussian Blue nanoparticles with 190 nm in diameter Commercial PB particles Oxidized multiwall carbon nanotubes Ammonium molybdophosphate– polyacrylonitrile Copper ferrocyanide functionalized mesoporous silica Phosphoric acid activated montmorillonite Ammonium molybdophosphate–calcium alginate composite adsorbent Brewery’s waste biomass Pre-treated arca shell biomass Mucilaginous seeds of Ocimum basilicum Moss NaOH treated moss
composites particles, biosorbents were tested for Cs removal. Only PB analogues could reach 99.99% removal of Cs from waters. The potential application of PB-impregnated nonwoven fabric for Cs removal in waterworks was reported. Acknowledgements This work is financially supported by the Taipei Water Department, Taipei City Government. References Aksu, Z., 2005. Application of biosorption for the removal of organic pollutants: A review. Process Biochem. 40, 997–1026. Annadurai, G., Juang, R.S., Lee, D.J., 2002. Use of cellulose-based wastes for adsorption of dyes from aqueous solutions. J. Hazard. Mater. 92 (3), 263–274.
Maximum adsorption capacity (mg Cs/g adsorbent)
References
Title
4.94 157.7 6.68 80.27
96 131.57 142.85 53.2 158 167 16.2 262 29.3 12.75 81.3
17.1 (seawater, pH 7.7) 208.0 91.8 10.1 3.93 160 6 17
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