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microphase separationIsozaki, Yuka*; Higashiharaguchi, Seiya*; Kaneko, Naoya*; Yamazaki, Shun*; Taniguchi, Tatsuo*; Karatsu, Takashi*; Ueda, Yuki; Motokawa, Ryuhei
Chemistry Letters, 51(6), p.625 - 628, 2022/06
Times Cited Count：2 Percentile：27.64(Chemistry, Multidisciplinary)Wang, X.*; Tang, X.*; Zhang, P.*; Wang, Y.*; Gao, D.*; Liu, J.*; Hui, K.*; Wang, Y.*; Dong, X.*; Hattori, Takanori; et al.
Journal of Physical Chemistry Letters (Internet), 12(50), p.12055 - 12061, 2021/12
Times Cited Count：6 Percentile：50.99(Chemistry, Physical)Substituted polyacetylene is expected to improve the chemical stability, physical properties, and additional functions of the polyacetylene backbones, but its diversity is very limited. Here, by applying external pressure on solid acetylenedicarboxylic acid, we report the first crystalline poly-dicarboxylacetylene with every carbon on the trans-polyacetylene backbone bonded to a carboxyl group, which is very hard to synthesize by traditional methods. This unique structure combines the extremely high content of carbonyl groups and high conductivity of a polyacetylene backbone, which exhibits a high specific capacity and excellent cycling/rate performance as a Li-ion battery (LIB) anode. We present a completely functionalized crystalline polyacetylene and provide a high-pressure solution for the synthesis of polymeric LIB materials and other polymeric materials with a high content of active groups.
Gao, D.*; Tang, X.*; Wang, X.*; Yang, X.*; Zhang, P.*; Che, G.*; Han, J.*; Hattori, Takanori; Wang, Y.*; Dong, X.*; et al.
Physical Chemistry Chemical Physics, 23(35), p.19503 - 19510, 2021/09
Times Cited Count：4 Percentile：35.04(Chemistry, Physical)Pressure-induced phase transition and polymerization of nitrogen-rich molecules are widely focused due to its extreme importance for the development of green high energy density materials. Here, we present a study of the phase transition and chemical reaction of 1H-tetrazole up to 100 GPa by using Raman, IR, X-ray diffraction, neutron diffraction techniques and theoretical calculation. A phase transition above 2.6 GPa was identified and the high-pressure structure was determined with one molecule in a unit cell. The 1H-tetrazole polymerizes reversibly below 100 GPa, probably through a carbon-nitrogen bonding instead of nitrogen-nitrogen bonding. Our studies updated the structure model of the high pressure phase of 1H-tetrazole, and presented the possible intermolecular bonding route for the first time, which gives new insights to understand the phase transition and chemical reaction of nitrogen-rich compounds, and benefit for designing new high energy density materials.
Shobu, Takahisa; Shiro, Ayumi*; Kono, Fumiaki*; Muramatsu, Toshiharu; Yamada, Tomonori; Naganuma, Masayuki; Ozawa, Takayuki
Quantum Beam Science (Internet), 5(2), p.17_1 - 17_9, 2021/06
The automotive industries employ laser beam welding because it realizes a high energy density without generating irradiation marks on the opposite side of the irradiated surface. Typical measurement techniques such as strain gauges and tube X-rays cannot assess the localized strain at a joint weld. Herein high-energy synchrotron radiation X-ray diffraction was used to study the internal strain distribution of laser lap joint PNC-FMS steels (2- and 5-mm thick) under loading at a high temperature. As the tensile load increased, the local tensile and compressive strains increased near the interface. These changes agreed well with the finite element analysis results. However, it is essential to complementarily utilize internal defect observations by X-ray transmission imaging because the results depend on the defects generated by laser processing.
Zhang, P.*; Tang, X.*; Wang, Y.*; Wang, X.*; Gao, D.*; Li, Y.*; Zheng, H.*; Wang, Y.*; Wang, X.*; Fu, R.*; et al.
Journal of the American Chemical Society, 142(41), p.17662 - 17669, 2020/10
Times Cited Count：21 Percentile：73.83(Chemistry, Multidisciplinary)Solid-state topochemical polymerization (SSTP) is a promising method to construct functional crystalline polymeric materials, but in contrast to various reactions that happen in solution, only very limited types of SSTP reactions are reported. Diels-Alder (DA) and dehydro-DA (DDA) reactions are textbook reactions for preparing six-membered rings in solution but are scarcely seen in solid-state synthesis. Here, using multiple cutting-edge techniques, we demonstrate that the solid 1,4-diphenylbutadiyne (DPB) undergoes a DDA reaction under 10-20 GPa with the phenyl as the dienophile. The crystal structure at the critical pressure shows that this reaction is "distance-selected". The distance of 3.2
between the phenyl and the phenylethynyl facilitates the DDA reaction, while the distances for other DDA and 1,4-addition reactions are too large to allow the bonding. The obtained products are crystalline armchair graphitic nanoribbons, and hence our studies open a new route to construct the crystalline carbon materials with atomic-scale control.
Ohashi, Kunihide*; Hino, Takanori*; Kobayashi, Hiroshi*; Onodera, Naoyuki; Sakamoto, Nobuaki*
Journal of Marine Science and Technology, 24(3), p.884 - 901, 2019/09
Times Cited Count：17 Percentile：75.85(Engineering, Marine)An unsteady Reynolds averaged Navier-Stokes solver with a structured overset grid method has been developed. Velocity pressure coupling is achieved using an artificial compressibility approach, spatial discretization is based on a FVM. Body motions are considered using the grid deformation technique and grid velocities in the convective term. The full multigrid (FMG) method is applied to obtain fast convergence. The cell flag on a coarse grid level is determined using the cell flag on a fine grid level. In the coarse and fine grid level calculations at the FMG stage, the data are interpolated until the finest grid level is achieved at an overset update interval. Then, the data are updated based on the overset relations at the finest grid level and then transferred to a coarser grid level. The computations for flows around a hull form, including an unsteady simulation with regular waves, are demonstrated.
H - CF cocrystal towards graphane structureWang, Y.*; Dong, X.*; Tang, X.*; Zheng, H.*; Li, K.*; Lin, X.*; Fang, L.*; Sun, G.*; Chen, X.*; Xie, L.*; et al.
Angewandte Chemie; International Edition, 58(5), p.1468 - 1473, 2019/01
Times Cited Count：35 Percentile：80.32(Chemistry, Multidisciplinary)Pressure-induced polymerization (PIP) of aromatics is a novel method to construct sp
-carbon frameworks, and nanothreads with diamond-like structures were synthesized by compressing benzene and its derivatives. Here by compressing benzene-hexafluorobenzene cocrystal(CHCF), we identified H-F-substituted graphane with a layered structure in the PIP product. Based on the crystal structure determined from the in situ neutron diffraction and the intermediate products identified by the gas chromatography-mass spectrum, we found that at 20 GPa CHCF forms tilted columns with benzene and hexafluorobenzene stacked alternatively, which leads to a [4+2] polymer, and then transfers to short-range ordered hydrogenated-fluorinated graphane. The reaction process contains [4+2] Diels-Alder, retro-Diels-Alder, and 1-1' coupling, and the former is the key reaction in the PIP. Our studies confirmed the elemental reactions of the CHCF for the first time, which provides a novel insight into the PIP of aromatics.
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：62.29(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.
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 
-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.
Saito, Kyoichi*; Asai, Shiho
Bunseki Kagaku, 66(11), p.771 - 782, 2017/11
Times Cited Count：1 Percentile：3.39(Chemistry, Analytical)Recovery and purification of rare metals, which are essential ingredients for highly functional materials, generally comes with operational difficulty. In this study, we have developed polymer adsorbents specially designed for highly-efficient adsorption of rare metal ions and exhibited their practical adsorption performances. Radiation-induced graft polymerization, one of the effective modification techniques for polymers, was employed for preparing the proposed adsorbents. Among such adsorbents, a 6-nylon fiber with nucleic-acid base, adenine, on the surface of the fiber demonstrated specific adsorption of ruthenium and palladium ions. In addition, a 6-nylon fiber with an extractant HDEHP (bis (2-ethylhexyl) phophoric acid) that has high affinity for lanthanides, achieved higher separation speed than a commercially available HDEHP-impregnated resin.
Asai, Shiho; Saito, Kyoichi*
Biomedical Research on Trace Elements, 28(1), p.1 - 10, 2017/04
Radionuclides are commonly determined with radiometry and mass spectrometry. For -emitting nuclides, the activities can be measured without chemical separation due to the strong penetration ability. In contrast, the measurements of alpha and beta-emitting nuclides are generally associated with tedious and time-consuming chemical separation procedures to remove concomitants. Thus, an adsorbent that achieves rapid separation is desirable to reduce separation time and workload. Our research team has developed compact cartridge-type solid phase extraction materials which enable to facilitate separation procedures. In this review, basic separation performances of the developed cartridges were overviewed along with two application examples to radionuclide-containing samples.
Saito, Kyoichi*; Kojima, Takashi*; Asai, Shiho
Bunseki Kagaku, 66(4), p.233 - 242, 2017/04
Times Cited Count：1 Percentile：3.39(Chemistry, Analytical)Insoluble cobalt ferrocyanide and sodium titanate specifically capture cesium and strontium ions, respectively, in water contaminated with radionuclides which is found in Fukushima Daiichi NPP. The inorganic compounds used in this study were formed as precipitates in the polymer chain grafted onto a commercially available 6-nylon fiber using radiation-induced graft polymerization. An impregnation structure with the precipitates entangled by the grafted polymer chain through an electrostatic interaction via multipoints was indicated. The resultant insoluble cobalt ferrocyanide- or sodium titanate-impregnated fiber exhibited a higher adsorption rate and adsorption capacity per gram of the inorganic compound for cesium or strontium ions in seawater than conventional granular adsorbents.
H-CF cocrystal under extreme conditionsWang, Y.*; Wang, L.*; Zheng, H.*; Li, K.*; Andrzejewski, M.*; Hattori, Takanori; Sano, Asami; Katrusiak, A.*; Meng, Y.*; Liao, F.*; et al.
Journal of Physical Chemistry C, 120(51), p.29510 - 29519, 2016/12
Times Cited Count：23 Percentile：60.41(Chemistry, Physical)Pressure-induced polymerization (PIP) of aromatic molecules can generate saturated carbon nanostructures. As a strongly interacted 
- stacking unit, the CH-CF adduct is widely applied in supramolecular chemistry, and it provides a good preorganization for the PIP. Here we investigated the structural variation of CH-CF cocrystal and the subsequent PIP process under high pressure. Four new molecular-complex phases V, VI, VII, and VIII have been identified and characterized by the in situ Raman, IR, synchrotron X-ray, and neutron diffraction. The phase V is different from the phases observed at low temperature, which has a tilted column structure. Phases VI and VII have a structure similar to phase V. Phase VIII polymerizes irreversibly upon compression above 25 GPa without any catalyst, producing sp(CH/F)
materials. The - interaction is still dominant below 0.5 GPa but is most likely to be overstepped under further compression, which is important for discussing the supramolecular phase transition and the polymerization process.
-tetrafluoroethylene) films using different mediaNuryanthi, 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 
m-thick ETFE film was irradiated in a vacuum chamber with 560 MeV 
Xe at different fluences, and then the grafting was performed by immersing the irradiated films in a 20vol% VBC monomer at 60
C. A medium was a mixture of water (H
O) and isopropyl alcohol (iPrOH) at different volume ratios. The degree of grafting increased as the HO content became higher, and reached a maximum in pure HO. 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.
Tamada, Masao
Hoshasen Kagaku (Internet), (100), P. 16, 2015/10
Collection of a rare metal form hot spring water attracted medias and had a public response by reports of numerous newspapers and television programs in my 35 years' research and development of radiation processing technologies and its technology management. Collection experiments of the rare metal were carried out in Kusatsu Onsen, Gunma prefecture, where discharge of hot spring water is the largest in Japan. We were on standby 6 am there when morning live broadcast started from 8 am. The invention of emersion grafting solved the problems in the cost reduction of adsorbent production owing to its high grafting yield and led the way for technology transfer of filter for the removal of metal ions in ppb level from semiconductor cleaning liquid and adsorbent for radio-active cesium.
Seko, Noriaki; Shibata, Takuya; Kasai, Noboru; Ueki, Yuji; Saiki, Seiichi; Hoshina, Hiroyuki
Hoshasen To Sangyo, (138), p.9 - 12, 2015/06
no abstracts in English
Someya, Takaaki*; Asai, Shiho; Fujiwara, Kunio*; Sugo, Takanobu*; Umeno, Daisuke*; Saito, Kyoichi*
Nihon Kaisui Gakkai-Shi, 69(1), p.42 - 48, 2015/02
A large amount of seriously contaminated sea water with radioactive Cs has been reserved in semi-enclosed coastal sea area which is separated by silt fences and embankments. Insoluble cobalt ferrocyanide (Co-FC) microparticles-impregnated fiber was developed for removing Cs from the contaminated sea water. The resultant Co-FC-impregnated fiber was immersed in either nonradioactive or radioactive Cs solution. The adsorption isotherm well correlated with a Langmuir-type equation. In addition, mass-transfer capacity coefficients were determined by fitting the experimental data of the rate of Cs adsorption onto the Co-FC-impregnated fiber to theoretical adsorption curves based on the Cs concentration difference between the bulk and the interface in seawater as a driving force of the overall adsorption rate. Decontamination factors as functions of fiber weight and the contact time required for the removal of cesium ions from the contaminated seawater in a closed area were estimated.
Saiki, Seiichi; Shibata, Takuya; Hoshina, Hiroyuki; Ueki, Yuji; Kasai, Noboru; Seko, Noriaki
Nihon Ion Kokan Gakkai-Shi, 25(4), p.170 - 175, 2014/11
Hayashi, Natsuki*; Hoshina, Hiroyuki; Amada, Haruyo; Yamanobe, Takeshi*; Seko, Noriaki
Nihon Ion Kokan Gakkai-Shi, 25(4), p.105 - 108, 2014/11
Ueki, Yuji; Saiki, Seiichi; Shibata, Takuya; Hoshina, Hiroyuki; Kasai, Noboru; Seko, Noriaki
International Journal of Organic Chemistry, 4(2), p.91 - 105, 2014/06
Grafted fibrous polymer with quaternary amine groups could function as a highly-efficient catalyst for biodiesel fuel (BDF) production. In this study, the optimization of grafted fibrous polymer (catalyst) and transesterification conditions for the effective BDF production was attempted through a batch-wise transesterification of triglyceride (TG) with ethanol (EtOH) in the presence of a cosolvent. Trimethylamine was the optimal quaternary amine group for the grafted fibrous catalyst. The optimal degree of grafting of the grafted fibrous catalyst was 170%. The optimal transesterification conditions were as follows: The molar quantity of quaternary amine groups, transesterification temperature, molar ratio of TG and EtOH, and primary alkyl alcohol were 0.8 mmol, 80C, 1:200, and 1-pentanol, respectively. The grafted fibrous catalyst could be applied to BDF production using natural oils. Furthermore, the grafted fibrous catalyst could be used repeatedly after regeneration involving three sequential processes, i.e., organic acid, alkali, and alcohol treatments, without any significant loss of catalytic activity.
