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Journal Articles

Weakened oxygen adsorbing the Pt-O bond of the Pt catalyst induced by vacancy introduction into carbon support

Okazaki, Hiroyuki*; Idesaki, Akira*; Koshikawa, Hiroshi*; Matsumura, Daiju; Ikeda, Takashi*; Yamamoto, Shunya*; Yamaki, Tetsuya*

Journal of Physical Chemistry C, 127(49), p.23628 - 23633, 2023/12

Journal Articles

Changes in electronic structure of carbon supports for Pt catalysts induced by vacancy formation due to Ar$$^{+}$$ irradiation

Okazaki, Hiroyuki*; Kakitani, Kenta*; Kimata, Tetsuya*; Idesaki, Akira*; Koshikawa, Hiroshi*; Matsumura, Daiju; Yamamoto, Shunya*; Yamaki, Tetsuya*

Journal of Chemical Physics, 152(12), p.124708_1 - 124708_5, 2020/03

 Times Cited Count:2 Percentile:26.72(Chemistry, Physical)

Journal Articles

Control of the size of etchable ion tracks in PVDF; Irradiation in an oxygen atmosphere and with fullerene C$$_{60}$$

Kitamura, Akane; Yamaki, Tetsuya*; Yuri, Yosuke*; Koshikawa, Hiroshi*; Sawada, Shinichi*; Yuyama, Takahiro*; Usui, Aya; Chiba, Atsuya*

Nuclear Instruments and Methods in Physics Research B, 460, p.254 - 258, 2019/12

 Times Cited Count:2 Percentile:23.44(Instruments & Instrumentation)

Poly(vinylidene-fluoride) (PVDF) film is suitable for investigation of the size of etchable ion tracks because we can clearly judge the finish of the track etching and the surrounding bulk area remains due to the high chemical stability. Thereby we can measure the radius of ion tracks of each ion. In this study, we focused on two irradiation conditions for controlling the size of etchable ion tracks of PVDF films. One was irradiation in an oxygen atmosphere and the other was a fullerene (C$$_{60}$$$$^{+}$$) cluster beam irradiation. SEM observation showed that the size of pores became larger by irradiation in an oxygen atmosphere. It was found that the oxidation of ion tracks widened the size of etchable ion tracks. The C$$_{60}$$$$^{+}$$ irradiation caused larger etchable tracks on the PVDF surface. The result could represent the effect of local and simultaneous collisions by the swift aggregated ions.

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*

Nihon 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

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

 Times Cited Count:8 Percentile:63.44(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

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*

Nihon 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

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

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

Poly(ether ether ketone) (PEEK)-based graft-type polymer electrolyte membranes having high crystallinity for high conducting and mechanical properties under various humidified conditions

Hamada, Takashi; Hasegawa, Shin; Fukasawa, Hideyuki*; Sawada, Shinichi; Koshikawa, Hiroshi; Miyashita, Atsumi; Maekawa, Yasunari

Journal of Materials Chemistry A, 3(42), p.20983 - 20991, 2015/11

 Times Cited Count:32 Percentile:70.95(Chemistry, Physical)

no abstracts in English

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

 Times Cited Count:9 Percentile:64.82(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

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:20 Percentile:59.91(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

Ion-track membranes of fluoropolymers; Toward controlling the pore size and shape

Yamaki, Tetsuya; Nuryanthi, N.*; Koshikawa, Hiroshi; Asano, Masaharu; Sawada, Shinichi; Hakoda, Teruyuki; Maekawa, Yasunari; Voss, K.-O.*; Severin, D.*; Seidl, T.*; et al.

Nuclear Instruments and Methods in Physics Research B, 314, p.77 - 81, 2013/11

 Times Cited Count:3 Percentile:26.8(Instruments & Instrumentation)

Ion-track membranes of poly(vinylidene fluoride) (PVDF), a type of fluoropolymer, could find wide applications due to its superior chemical and mechanical properties. In order to produce track-etched pores in PVDF films, we have independently employed much milder etching conditions without any oxidant additives in the alkaline etching solution. The goal of this work is to pursue the possibility of varying beam parameters and applying the effect of the etching pretreatment to control the pore size and shape. Ongoing in-situ/on-line analyses at the M-branch of the UNILAC would shed light on the detailed chemistry of not only ion-induced degradation but also the post-irradiation reactivity.

Journal Articles

Applied-voltage dependence on conductometric track etching of poly(vinylidene fluoride) films

Nuryanthi, N.*; Yamaki, Tetsuya; Koshikawa, Hiroshi; Asano, Masaharu; Sawada, Shinichi; Hasegawa, Shin; Maekawa, Yasunari; Katsumura, Yosuke*

Nuclear Instruments and Methods in Physics Research B, 314, p.95 - 98, 2013/11

 Times Cited Count:3 Percentile:26.8(Instruments & Instrumentation)

Our efforts have been focused on ion-track etched membranes of poly(vinylidene fluoride) (PVDF). This study deals with the effect of the transmembrane potential applied during the conductometry in order to offer a higher degree of freedom to control the pore size. We can say that higher voltage application during the conductometry would accelerate the etching in the tracks. The electrophoretic migration of dissolved products occurring out of each pore might be one of the reasons for this enhanced pore evolution and growth.

Journal Articles

Counter-anion effect on the properties of anion-conducting polymer electrolyte membranes prepared by radiation-induced graft polymerization

Koshikawa, Hiroshi; Yoshimura, Kimio; Sinnananchi, W.; Yamaki, Tetsuya; Asano, Masaharu; Yamamoto, Kazuya*; Yamaguchi, Susumu*; Tanaka, Hirohisa*; Maekawa, Yasunari

Macromolecular Chemistry and Physics, 214(15), p.1756 - 1762, 2013/08

 Times Cited Count:14 Percentile:43.43(Polymer Science)

Graft-type anion-conducting polymer electrolyte membranes were prepared by the radiation-induced graft polymerization of chloromethylstyrene into poly(ethylene-co-tetrafluoroethylene) (ETFE) films and subsequent quaternization with trimethylamine to evaluate the counter anion effects on fuel cell properties. The hydroxide form was maintained in -saturated water to prevent the bicarbonate formation. The hydroxide form showed conductivity and water uptake four and two times higher than the chloride and bicarbonate forms. The hydroxide form is thermally and chemically less stable, resulting in the tendency to absorb water and to convert to the bicarbonate form.

Journal Articles

Ion-track membranes of poly(vinylidene fluoride); Etching characteristics during conductomeric analysis

Nuryanthi, N.*; Yamaki, Tetsuya; Koshikawa, Hiroshi; Asano, Masaharu; Sawada, Shinichi; Hasegawa, Shin; Maekawa, Yasunari; Katsumura, Yosuke*

Transactions of the Materials Research Society of Japan, 38(1), p.105 - 108, 2013/03

We report here how conditions of the conductometric analysis affected the etching characteristics of 25 $$mu$$m-thick poly(vinylidene fluoride) film irradiated with 450 MeV $$^{129}$$Xe ions. The etching was performed in a 9 mol dm$$^{-3}$$ aqueous potassium hydroxide solution at 80$$^{circ}$$C in a conductometric cell. According to the scanning electron microscope observations, the ion-track membrane obtained with an applied AC voltage of 1.0 V had the surface pores of 168$$pm$$20 nm in diameter. On the other hand, the etching without an applied voltage gave the approximately two-thirds smaller pores. The conductomeric etching would provide a higher degree of freedom for controlling the pore diameter.

Journal Articles

Alkaline durable anion exchange membranes based on graft-type fluoropolymer films for hydrazine hydrate fuel cell

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

ECS Transactions, 50(2), p.2075 - 2081, 2012/10

no abstracts in English

Journal Articles

Investigation of nanopore evolution in track-etched poly(vinylidene fluoride) membranes

Yamaki, Tetsuya; Nuryanthi, N.*; Koshikawa, Hiroshi; Asano, Masaharu; Sawada, Shinichi; Hasegawa, Shin; Maekawa, Yasunari; Voss, K.-O.*; Trautmann, C.*; Neumann, R.*

Transactions of the Materials Research Society of Japan, 37(2), p.223 - 226, 2012/06

The aim of this study is to investigate the formation of the poly(vinylidene fluoride) (PVDF) track membranes in detail by electrolytic conductometry. A PVDF film was irradiated with a 450 MeV $$^{129}$$Xe or 2.2 GeV $$^{197}$$Au ion beam, and then the latent tracks were etched in a 9 mol dm$$^{-3}$$ aqueous KOH solution at 80$$^{circ}$$C that had been poured into a conductometric cell. At the same time, the evolution of cylindrical nanopores was monitored by measuring the conductance through the membrane. The etching kinetics significantly depended on the deposited energy within each track, which is represented by the LET. Interestingly, applying a higher voltage to the cell promoted track etching up to the breakthrough probably because the electrophoretic migration of dissolved products occurred out of each pore.

Journal Articles

Development of grafted type poly(ether ether ketone) electrolyte membranes; Morphology of PEEK substrate and radiation-induced graft polymerization

Hasegawa, Shin; Chen, J.; Koshikawa, Hiroshi; Iwase, Hiroki*; Koizumi, Satoshi; Onuma, Masato*; Maekawa, Yasunari; Iwase, Hiroki*

Proceedings of 12th International Conference on Radiation Curing in Asia (RadTech Asia 2011) (Internet), p.238 - 239, 2011/06

Radiation-induced graft polymerization of sulfo-containing styrene derivatives into crystalline poly(ether ether ketone) (PEEK) substrates was carried out to prepare thermally and mechanically stable polymer electrolyte membranes based on an aromatic hydrocarbon polymer, so-called "super-engineering plastics". Graft polymerization of the sulfo-containing styrene, ethyl 4-styrenesulfonate (E4S) into PEEK substrates with degrees of crystallinity (DC) of 11 - 26% gradually progressed, achieving a grafting degree of more than 50% after 72 hours, whereas graft polymerization of the substrates with DC above 26% did not proceed. When morphological change in these films were measured by SAXS, PEEK films with DC larger than 26% showed a new peak at d=14 nm, corresponding to lamella structure. Thus, the suppression of graft polymerization of PEEK films with DC above 26% was due to obstruct of monomer diffusion by the formation of the oriented lamella structure.

Journal Articles

Graft-type polymer electrolyte membranes consisting of poly(ether ether ketone) prepared by radiation technique

Maekawa, Yasunari; Hasegawa, Shin; Koshikawa, Hiroshi; Chen, J.

Proceedings of 12th International Conference on Radiation Curing in Asia (RadTech Asia 2011) (Internet), p.104 - 105, 2011/06

We applied the radiation-induced grafting to poly(ether ether ketone) film, which was mechanically and thermally stable aromatic hydrocarbon polymers, so-called "super engineering plastics". The developed PEEK-based polymer electrolyte membrane (PEM) with 96 $$mu$$m thickness exhibited 1.5 times higher conductivity and 2.3 times higher mechanical strength, compared with conventional fluorinated PEM. The single fuel cell device maintained stable operation over 1000 hours under the operation at 95$$^{circ}$$C. According to the high mechanical strength of PEEK substrates, we could reduce the film thickness of PEEK-based PEM down to 10 $$mu$$m. The PEEK-based PEM with film thickness of 10 and 19 $$mu$$m showed higher cell voltages than that of Nafion at the current density in the range from 0.2 to 1.0 A/cm$$^{2}$$.

Journal Articles

Preparation of anion-exchange membranes for fuel cell applications by $$gamma$$-ray pre-irradiation grafting

Koshikawa, Hiroshi; Yamaki, Tetsuya; Asano, Masaharu; Maekawa, Yasunari; Yamaguchi, Susumu*; Yamamoto, Kazuya*; Asazawa, Koichiro*; Yamada, Koji*; Tanaka, Hirohisa*

Proceedings of 12th International Conference on Radiation Curing in Asia (RadTech Asia 2011) (Internet), p.240 - 241, 2011/06

The anion-exchange membranes (AEM) for fuel cells were prepared by the radiation-induced graft polymerization of chloromethylstyrene into poly(ethylene-co-tetrafluoroethylene) (ETFE) films and subsequent quaternization of the grafts with trimethylamine. When the AEM were treated in 1M-KOH and washed with N$$_{2}$$-saturated water, the membranes with chloride form can be converted quantitatively to hydroxide form. However, the hydroxide form was easily converted to the bicarbonate form by the treatment in non-bubbled (CO$$_{2}$$ dissolved) water. When we introduced the crosslinkers in polymer grafts, which is proved to be very effective in the proton conducting PEM having a poly(styrenesulfonic acid) grafts, the grafted AEM with both chloride and hydroxide forms showed only slight decrease of water uptake. It should be noted that AEM with hydroxide form showed very high tendency to absorb water.

139 (Records 1-20 displayed on this page)