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Journal Articles

Development of cation and anion exchange membranes for saline water concentration using high-energy heavy-ion beams

Sawada, Shinichi*; Yasukawa, Masahiro*; Koshikawa, Hiroshi*; Kitamura, Akane; Higa, Mitsuru*; Yamaki, Tetsuya*

Nippon Kaisui Gakkai-Shi, 73(4), p.208 - 216, 2019/08

For applications to saline water concentration by electrodialysis, we prepared nano-structure-controlled cation and anion exchange membranes (CEMs and AEMs) by a so-called ion-track grafting technique. This new technique involves irradiation of a polymer substrate with an MeV-GeV heavy-ion beam to form the nano-sized cylindrical ion tracks and the graft polymerization only into the ion tracks for the creation of one-dimensional transport pathways. A 25-$$mu$$m-thick poly(ethylene-co-tetrafluoroethylene) film was irradiated with 560 MeV $$^{129}$$Xe or 310 MeV $$^{84}$$Kr. The irradiated films were immersed in grafting solutions of ethyl p-styrenesulfonate (EtSS) and chloromethylstyrene (CMS),and then subjected to the hydrolysis of EtSS units and quaternization of CMS units to prepare CEMs and AEMs, respectively. These CEMs and AEMs showed lower resistance than the commercially-available membranes even at the very low water uptake. This would be due to the signifcantly-effcient transport of ions through the unique one-dimensional highly-connected transport pathways. In the saline water concentration experiment, a pair of our CEM and a commercial AEM or vice versa led to a higher salt concentration in the concentration chamber than did a pair of the commercial membranes. This result demonstrated great applicability of our ion-track-grafted CEMs and AEMs for saline water concentration.

Journal Articles

Research and development on membrane IS process for hydrogen production using solar heat

Odtsetseg, M.; Iwatsuki, Jin; Tanaka, Nobuyuki; Noguchi, Hiroki; Kamiji, Yu; Ioka, Ikuo; Kubo, Shinji; Nomura, Mikihiro*; Yamaki, Tetsuya*; Sawada, Shinichi*; et al.

International Journal of Hydrogen Energy, 44(35), p.19141 - 19152, 2019/07

Journal Articles

FE-SEM observations of multiple nanohillocks on SrTiO$$_{3}$$ irradiated with swift heavy ions

Kitamura, Akane; Ishikawa, Norito; Kondo, Keietsu; Fujimura, Yuki; Yamamoto, Shunya*; Yamaki, Tetsuya*

Transactions of the Materials Research Society of Japan, 44(3), p.85 - 88, 2019/06

Swift heavy ions can create nanosized hillocks on the surfaces of various ceramics. When these materials are irradiated with swift heavy ions at normal incidence, each ion impact results in the formation of a single hillock on the surfaces. In contrast, irradiation at grazing incidence forms chains of multiple hillocks on the surface, for example, for strontium titanate (SrTiO$$_{3}$$). So far, chains of multiple hillocks have been investigated using atomic force microscopy (AFM). It should be noted that AFM measurements involve systematic errors of several nanometers due to the finite size of the probe tip. Consequently, it is possible that the image of one hillock may merge with that of a neighboring hillock even if the two hillocks are well separated. In contrast to AFM, field-emission scanning electron microscopy (FE-SEM) is a useful technique for obtaining higher-resolution images. In this study, we observed multiple nanohillocks on the surfaces of SrTiO$$_{3}$$ using FE-SEM. Crystals of SrTiO$$_{3}$$(100) and 0.05 wt% Nb-doped SrTiO$$_{3}$$(100) were irradiated with 350 MeV Xe ions, respectively, at grazing incidence, where the angle between the sample surface and the beam was less than 2$$^{circ}$$. On the SrTiO$$_{3}$$ surface, a chain of periodic nanohillocks is created along the ion path. In contrast, black lines accompanied by hillocks are observed on the Nb-doped SrTiO$$_{3}$$ surface.

Journal Articles

X-ray absorption study of platinum nanoparticles on an ion-irradiated carbon support

Kakitani, Kenta*; Kimata, Tetsuya*; Yamaki, Tetsuya*; Yamamoto, Shunya*; Matsumura, Daiju; Taguchi, Tomitsugu*; Terai, Takayuki*

Radiation Physics and Chemistry, 153, p.152 - 155, 2018/12

 Percentile:100(Chemistry, Physical)

Journal Articles

Fluoropolymer-based nanostructured membranes created by swift-heavy-ion irradiation and their energy and environmental applications

Yamaki, Tetsuya*; Nuryanthi, N.*; Kitamura, Akane; Koshikawa, Hiroshi*; Sawada, Shinichi*; Voss, K.-O.*; Severin, D.*; Tautmann, C.*

Nuclear Instruments and Methods in Physics Research B, 435, p.162 - 168, 2018/11

 Percentile:100(Instruments & Instrumentation)

We used individual single-ion tracks in fluoropolymers with diameters of tens to hundreds of nanometers; chemical etching and ion-track grafting enabled us to develop ion-track and proton-conductive membranes, respectively. In the ion-track membranes of PVDF, strongly-LET-dependent etching was found, so the pore shape as well as the size was exclusively controlled by the track structures. We performed the ion-track grafting of styrene into ETFE to develop nanostructure-controlled proton exchange membranes (PEMs) for applications in PEM fuel cells. Our ion beam technology to develop fluoropolymer-based nanostructures has the potential to apply in the field of filtration processes and fuel cell devices. This would make it possible to provide new microfiltration technology for water treatment, sterilization, petroleum refining and dairy processing.

Journal Articles

Development of ion-exchange membranes for the membrane Bunsen reaction in thermochemical hydrogen production by iodine-sulfur process

Nomura, Mikihiro*; Kodaira, Takahide*; Ikeda, Ayumi*; Naka, Yasuhito*; Nishijima, Haruyuki*; Imabayashi, Shinichiro*; Sawada, Shinichi*; Yamaki, Tetsuya*; Tanaka, Nobuyuki; Kubo, Shinji

Journal of Chemical Engineering of Japan, 51(9), p.726 - 731, 2018/09

 Percentile:100(Engineering, Chemical)

Thermochemical hydrogen production by the iodine-sulfur process decomposes water into hydrogen and oxygen by combining the chemical reactions of iodine and sulfur. Two types of acids are produced through the Bunsen reaction. To improve the performance of this reaction, ion-exchange membranes for the membrane Bunsen reaction should be developed. In the present study, a cation-exchange membrane was prepared by using a radiation-graft polymerization method. It was found that a divinylbenzene crosslinking procedure was very effective in reducing water permeation through the membrane, and the membrane Bunsen reaction was successfully carried out by using the developed crosslinked membrane. Therefore, the developed crosslinked membrane is a potential candidate for cation-exchange membranes for the membrane Bunsen reaction.

Journal Articles

Analysis of scintillation light intensity by microscopic radiation transport calculation and F$"{o}$rster quenching model

Ogawa, Tatsuhiko; Yamaki, Tetsuya*; Sato, Tatsuhiko

PLOS ONE (Internet), 13(8), p.e0202011_1 - e0202011_19, 2018/08

 Percentile:100(Multidisciplinary Sciences)

Scintillators are generally used to detect various kinds of particles such as electrons, gammas, protons and heavy ions. Scintillators emit photons according to the energy deposited to the crystal. It is also known that light yield is suppressed for particles depositing energy densely owing to quenching. Moreover, it is suggested that quenching is attributed to transfer of energy from excited fluorescent molecules to damaged molecules (F$"{o}$rster mechanism). In this study, energy deposition in a scintillator crystal by radiation was calculated using radiation transport codes to finally obtain excitation and damage of fluorescent molecules. Based on the calculation, spatial configuration of exited and damaged molecules. Then the probability that F$"{o}$rster mechanism takes place in excited molecules were estimated to obtain the number of fluorescent molecules that emit photons. As a result, light yield is proportionally increased with increase in the incident energy in case of electron incidence. On the other hand, light yield is increased non-linearly in case of proton incidence. This trend is in a good agreement with the experimental results.

Journal Articles

Research on nanostructure-controlled functional membranes using high-energy ion beams; Fluoropolymer-based porous and ion-exchange membranes

Yamaki, Tetsuya*; Kitamura, Akane; Sawada, Shinichi*; Koshikawa, Hiroshi*

Nippon Kaisui Gakkai-Shi, 72(2), p.62 - 74, 2018/04

This review paper is devoted to two topics, i.e., fluoropolymer-based porous and ion-exchange membranes, both of which include the creation of nanostructure-controlled functional membranes with high-energy ion beams. Latent tracks of the MeV-GeV heavy ions in a polymer foil can sometimes be chemically etched out to form a membrane with micro- and nano-sized through-pores, the so-called ion-track membrane. Our focus is on ion-track membranes of poly (vinylidene fluoride) (PVDF) and cation- and anion-exchange membranes (CEMs and AEMs, respectively).

Journal Articles

Ion track etching of PVDF films irradiated with fast C$$_{60}$$$$^{+}$$ cluster ions

Kitamura, Akane; Yamaki, Tetsuya*; Chiba, Atsuya*; Usui, Aya

QST-M-8; QST Takasaki Annual Report 2016, P. 37, 2018/03

We investigated the track-etched surface of PVDF films irradiated with C$$_{60}$$$$^{+}$$ cluster ions, comparing the data with C$$^{+}$$ monoatomic ions. PVDF films were irradiated with 6 MeV C$$_{60}$$$$^{+}$$ cluster ions. The energy of the each carbon ion is 100 keV/atom; thus, for comparison, the PVDF films were also irradiated with 100 keV C$$^{+}$$ ions. SEM and AFM observation showed that the surface irradiated with C$$_{60}$$$$^{+}$$ cluster ions apparently possessed flat-bottomed pores with an average diameter and depth of approximately 400 and 250 nm, respectively. On the other hand, track-etched pores were also formed on the surface irradiated with C$$^{+}$$ ions, but their morphology was irregular or obscure. In the irradiation with the C$$_{60}$$$$^{+}$$ cluster ions, the surface diameter of track-etched pores increased with increasing the etching time. The tracks of the 100 keV C$$^{+}$$ ions seemed to be hardly developed by the etching when the time. In conclusion, the C$$_{60}$$$$^{+}$$ cluster ions irradiation caused a large size of etchable tracks on the PVDF surface. The result could represent the effect of local and simultaneous collision by the aggregated ions.

Journal Articles

Preparation of nano-structure controlled ion-exchange membranes by ion beams and their application to seawater concentration

Yamaki, Tetsuya*; Goto, Mitsuaki*; Sawada, Shinichi*; Koshikawa, Hiroshi*; Kitamura, Akane; Higa, Mitsuru*

QST-M-8; QST Takasaki Annual Report 2016, P. 35, 2018/03

We prepared ion exchange membranes by a heavy-ion-track grafting method, and then used them for seawater concentration process. Both the water uptake and resistance were lower for our ion-track grafted membranes than for the conventional $$gamma$$-ray-grafted membranes. The results would be because local and high-density energy deposition due to the ion beam enabled us to control the membrane structure in a nanometer scale. We demonstrate our membranes are suitable for this application.

Journal Articles

Reproduction of heavy-ion irradiation effect on organic polymers using radiation transport simulation code

Ogawa, Tatsuhiko; Yamaki, Tetsuya*; Sato, Tatsuhiko

QST-M-2; QST Takasaki Annual Report 2015, P. 46, 2017/03

Modification of materials by irradiation, which is substantially important for radiation safety in facilities and industrial applications, is studied from various aspects. Material modification is induced by local energy deposition by incident radiation followed by the changes of chemical bonds in the spatial scale of nm to $$mu$$m. So far, absorbed dose was regarded as the best index of irradiation effects, however, it is also known that irradiation effects varies depending on the radiation species even under the same absorbed dose or LET. Radiation transport simulation code PHITS can calculate simulate energy deposition in nm to $$mu$$m scale to obtain LET and specific energy deposition (SED). By using SED calculation function, an attempt to reproduce radiation species dependence of material property change based on the theoretical prediction of chemical reactions induced by energy deposition in different irradiation conditions. Estimate on the decrease in Elongation at Break (EB) of poly-ether sulfone in three different irradiation conditions, 10 MeV protons, 50 MeV $$^4$$He and $$^{12}$$C showed that reduction of EB by carbon ions is twice as small as that by proton and that by helium for the same absorbed dose, which is in an agreement with experiment. Moreover, assuming that scission of polymer takes place at random and 100 eV energy deposition in the region result in loss of mechanical strength, saturating trend of EB reduction.

Journal Articles

Complex chemistry with complex compounds

Eichler, R.*; Asai, Masato; Brand, H.*; Chiera, N. M.*; Di Nitto, A.*; Dressler, R.*; D$"u$llmann, Ch. E.*; Even, J.*; Fangli, F.*; Goetz, M.*; et al.

EPJ Web of Conferences (Internet), 131, p.07005_1 - 07005_7, 2016/12


In recent years gas-phase chemical studies assisted by physical pre-separation allowed for the productions and investigations of fragile single molecular species of superheavy elements. The latest highlight is the formation of very volatile hexacarbonyl compound of element 106, Sg(CO)$$_{6}$$. Following this success, second-generation experiments were performed to measure the first bond dissociation energy between the central metal atom and the surrounding ligand. The method using a tubular decomposition reactor was developed and successfully applied to short-lived Mo(CO)$$_{6}$$, W(CO)$$_{6}$$, and Sg(CO)$$_{6}$$.

Journal Articles

Decomposition studies of group 6 hexacarbonyl complexes, 1; Production and decomposition of Mo(CO)$$_6$$ and W(CO)$$_6$$

Usoltsev, I.*; Eichler, R.*; Wang, Y.*; Even, J.*; Yakushev, A.*; Haba, Hiromitsu*; Asai, Masato; Brand, H.*; Di Nitto, A.*; D$"u$llmann, Ch. E.*; et al.

Radiochimica Acta, 104(3), p.141 - 151, 2016/03

 Times Cited Count:8 Percentile:10.94(Chemistry, Inorganic & Nuclear)

Conditions of the production and decomposition of hexacarbonyl complexes of short-lived Mo and W isotopes were investigated to study thermal stability of the heaviest group 6 hexacarbonyl complex Sg(CO)$$_6$$. A tubular flow reactor was tested to decompose the hexacarbonyl complexes and to extract the first bond dissociation energies. A silver was found to be the most appropriate reaction surface to study the decomposition of the group 6 hexacarbonyl. It was found that the surface temperature at which the decomposition occurred was correlated to the first bond dissociation energy of Mo(CO)$$_6$$ and W(CO)$$_6$$, indicating that the first bond dissociation energy of Sg(CO)$$_6$$ could be determined with this technique.

Journal Articles

Ion-track grafting of vinylbenzyl chloride into poly(ethylene-$$co$$-tetrafluoroethylene) films using different media

Nuryanthi, N.*; Yamaki, Tetsuya; Kitamura, Akane; Koshikawa, Hiroshi; Yoshimura, Kimio; Sawada, Shinichi; Hasegawa, Shin; Asano, Masaharu; Maekawa, Yasunari; Suzuki, Akihiro*; et al.

Transactions of the Materials Research Society of Japan, 40(4), p.359 - 362, 2015/12

The ion-track grafting of a vinylbenzyl chloride (VBC) into a poly(ethylene-co-tetrafluoroethylene) (ETFE) film is necessary for preparing nanostructured hydroxide-ion-conductive electrolyte membranes. A key for success here is to obtain as high graft levels as possible (for higher conductivity) in a smaller number of tracks (for improving the other membrane properties). To this end, therefore, the effect of the medium for the VBC grafting was investigated as part of our continuing effort to optimize the experimental conditions. A 25 $$mu$$m-thick ETFE film was irradiated in a vacuum chamber with 560 MeV $$^{129}$$Xe at different fluences, and then the grafting was performed by immersing the irradiated films in a 20vol% VBC monomer at 60$$^{circ}$$C. A medium was a mixture of water (H$$_{2}$$O) and isopropyl alcohol (iPrOH) at different volume ratios. The degree of grafting increased as the H$$_{2}$$O content became higher, and reached a maximum in pure H$$_{2}$$O. These results can be explained by considering the well-known Trommsdorff effect, in which poor solubility of the grafted polymer in polar media leads to an increased polymerization rate probably due to a lower termination rate.

Journal Articles

Fabrication of hard-coated optical absorbers with microstructured surfaces using etched ion tracks; Toward broadband ultra-low reflectance

Amemiya, Kuniaki*; Koshikawa, Hiroshi; Yamaki, Tetsuya; Maekawa, Yasunari; Shitomi, Hiroshi*; Numata, Takayuki*; Kinoshita, Kenichi*; Tanabe, Minoru*; Fukuda, Daiji*

Nuclear Instruments and Methods in Physics Research B, 356-357, p.154 - 159, 2015/08

 Percentile:100(Instruments & Instrumentation)

Broadband low reflectance materials have various applications in the field of optical energy management; however, materials with ultra-low reflectance (below 0.1%) have been considered as mechanically delicate. We have developed a novel hard-surface optical absorber with microstructured, diamond-like carbon coated ion tracks on CR-39 plastic substrate. The spectral reflectance of the first prototype was below 2% for wavelengths ranging from 400 nm to 1400 nm; moreover, the optical absorber had mechanically hard surface and exhibited temporal durability. Choosing the appropriate design of the surface structure and coating layer is likely to reduce the reflectance to the order of 0.1%. This technique yields easy-to-handle broadband ultra-low reflectance absorbers.

Journal Articles

In situ synthesis of volatile carbonyl complexes with short-lived nuclides

Even, J.*; Ackermann, D.*; Asai, Masato; Block, M.*; Brand, H.*; Di Nitto, A.*; D$"u$llmann, Ch. E.*; Eichler, R.*; Fan, F.*; Haba, Hiromitsu*; et al.

Journal of Radioanalytical and Nuclear Chemistry, 303(3), p.2457 - 2466, 2015/03

 Times Cited Count:6 Percentile:28.02(Chemistry, Analytical)

Rapid In situ synthesis of metal carbonyl complexes has been demonstrated using short-lived isotopes produced in nuclear fission and fusion reactions. The short-lived isotopes with high recoil energy directly react with carbon-monoxides and form carbonyl complexes. Only highly volatile complexes were fast transported in a gas stream to counting and chemistry devices. Short-lived Mo, Tc, Ru, Rh, W, Re, Os, and Ir were found to form volatile carbonyl complexes, while no volataile complex of Hf and Ta were detected. This technique has been applied to a chemical investigation of the superheavy element Sg (atomic number 106), and will be applicable to various fields of nuclear science with short-lived transition metal isotopes.

Journal Articles

Synthesis and detection of a Seaborgium carbonyl complex

Even, J.*; Yakushev, A.*; D$"u$llmann, Ch. E.*; Haba, Hiromitsu*; Asai, Masato; Sato, Tetsuya; Brand, H.*; Di Nitto, A.*; Eichler, R.*; Fan, F. L.*; et al.

Science, 345(6203), p.1491 - 1493, 2014/09

 Times Cited Count:35 Percentile:17.05(Multidisciplinary Sciences)

A new superheavy element complex, a seaborgium carbonyl, has been successfully synthesized, and its adsorption property has been studied using a cryo-thermochromatography and $$alpha$$-detection apparatus COMPACT. Nuclear reaction products of short-lived $$^{265}$$Sg preseparated with a gas-filled recoil ion separator GARIS at RIKEN were directly injected into a gas cell filled with He/CO mixture gas, and chemical reaction products of volatile carbonyl complexes were trasported to COMPACT. The Sg carbonyl complex detected with COMPACT was found to be very volatile with adsorption enthalpy of $$-$$50 kJ/mol, from which we have concluded that this complex should be a Sg hexacarbonyl Sg(CO)$$_{6}$$. This is the first synthesis of organometallic compounds of transactinide elements for which only simple inorganic comounds have been synthesized so far.

Journal Articles

Imidazolium cation based anion-conducting electrolyte membranes prepared by radiation induced grafting for direct hydrazine hydrate fuel cells

Yoshimura, Kimio; Koshikawa, Hiroshi; Yamaki, Tetsuya; Shishitani, Hideyuki*; Yamamoto, Kazuya*; Yamaguchi, Susumu*; Tanaka, Hirohisa*; Maekawa, Yasunari

Journal of the Electrochemical Society, 161(9), p.F889 - F893, 2014/06

 Times Cited Count:14 Percentile:30.39(Electrochemistry)

Graft-type anion-conducting electrolyte membranes (AEMs) with imidazolium cations on graft polymers were synthesized through radiation-induced graft polymerization of ${it N}$-vinylimidazole (NVIm) on poly(ethylene-co-tetrafluoroethylene) (ETFE) films, followed by ${it N}$-propylation and ion-exchange reactions. The ${it N}$-propylation proceeded quantitatively, whereas the ion-exchange reactions in 1 M KOH at 60$$^{circ}$$C were accompanied by partial $$beta$$-elimination of the imidazolium cations(AEM2), which exhibited an ion-exchange capacity (IEC) of 0.85 mmol g$$^{-1}$$ and ionic conductivity of 10 mS cm$$^{-1}$$. AEM2 showed alkaline stability at 60$$^{circ}$$C but it gradually degraded at 80$$^{circ}$$C for ca. 150 h. The copolymer-type AEM (AEM3) with an IEC of 1.20 mmol g$$^{-1}$$ was prepared through the copolymerization of NVIm with styrene on ETFE films, followed by the same ${it N}$-propylation and ion-exchange reactions. AEM3 was shown higher alkaline durability in 1 M KOH at 80$$^{circ}$$C. As a result, it exhibited higher conductivity ($$>$$10 mS cm$$^{-1}$$) for 250 h. Therefore, alkylimidazolium cations in copolymer grafts are a promising anion conducting group for alkaline-durable AEMs. A maximum power density of 75 mW cm$$^{-2}$$ is obtained for AEM3 in a direct hydrazine hydrate fuel cell.

Journal Articles

Affinity of ion-exchange membranes for HI-I$$_{2}$$-H$$_{2}$$O mixture

Tanaka, Nobuyuki; Yamaki, Tetsuya; Asano, Masaharu; Terai, Takayuki*; Onuki, Kaoru

Journal of Membrane Science, 456, p.31 - 41, 2014/04

 Percentile:100(Engineering, Chemical)

Electro-electrodialysis (EED) has been applied to thermochemical water-splitting iodine-sulfur process for hydrogen production in order to enhance the HI uptake from a HI-I$$_{2}$$-H$$_{2}$$O mixture (HIx solution). In this paper, the constitution of the HIx solution absorbed in grafted membranes and in Nafion 212 is evaluated. The affinity of the membranes for the HIx solution is discussed based on the measurement results. The behavior of each component in the membrane was as follows: The strong affinity of the ETFE-St membrane for I$$_{2}$$ was shown because of the formation of a charge-transfer complex with electron-donating aromatic groups, whereas I$$_{2}$$ absorption by Nafion 212 was minimal. The difference of affinity for the ions can be attributed to the formation of the I$$_{3}$$- complex from I- and I$$_{2}$$ absorbed in the grafted membranes, which was precluded in Nafion 212.

Journal Articles

Microscopic evaluation of the absolute fluence distribution of a large-area uniform ion beam using the track-etching technique

Kitamura, Akane; Yamaki, Tetsuya; Yuri, Yosuke; Sawada, Shinichi; Yuyama, Takahiro

Nuclear Instruments and Methods in Physics Research B, 314, p.47 - 50, 2013/11

 Percentile:100(Instruments & Instrumentation)

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