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Effective adsorption and collection of cesium from aqueous solution using graphene oxide grown on porous alumina

圓谷 志郎*; 本田 充紀; 下山 巖; Li, S.*; 楢本 洋*; 矢板 毅; 境 誠司*

Japanese Journal of Applied Physics, 57(4S), p.04FP04_1 - 04FP04_4, 2018/04

 被引用回数:3 パーセンタイル:24.63(Physics, Applied)

Graphene oxide (GO) with a large surface area was synthesized by the direct growth of GO on porous alumina using chemical vapor deposition to study the Cs adsorption mechanism in aqueous solutions. Electronic structure analysis employing in situ near-edge X-ray absorption fine structure spectroscopy and X-ray photoelectron spectroscopy measurements clarifies the Cs atoms bond via oxygen functional groups on GO in the aqueous solution. The Cs adsorption capacity was found to be as high as 650-850 mg g$$^{-1}$$, which indicates that the GO/porous alumina acts as an effective adsorbent with high adsorption efficiency for radioactive nuclides in aqueous solutions.



岩田 景子; 高見澤 悠; 河 侑成; 岡本 芳浩; 下山 巖; 本田 充紀; 塙 悟史; 西山 裕孝

Photon Factory Activity Report 2017, 2 Pages, 2018/00



Proposed cesium-free mineralization method for soil decontamination; Demonstration of cesium removal from weathered biotite

本田 充紀; 下山 巖; 小暮 敏博*; 馬場 祐治; 鈴木 伸一; 矢板 毅

ACS Omega (Internet), 2(12), p.8678 - 8681, 2017/12

 被引用回数:4 パーセンタイル:17.92(Chemistry, Multidisciplinary)

The possibility to remove sorbed cesium (Cs) from weathered biotite (WB), which is considered a major Cs-adsorbent in the soil of Fukushima, has been investigated by the addition of NaCl-CaCl$$_{2}$$ mixed salt and subsequent heat treatment in a low pressure. X-ray fluorescence analysis was employed to determine the Cs removal rate with elevated temperature. The structural changes and new phases formed were determined using powder X-ray diffraction, as well as electron diffraction and X-ray microanalysis in a transmission electron microscope. We found that Cs was completely removed from the specimen heated at 700 $$^{circ}$$C, when WB completely decomposed and augite with a pyroxene structure was formed. On the basis of this finding, we propose the cesium-free mineralization (CFM) method, a new soil decontamination process by means of transformation of Cs-sorbing minerals to those where Cs is impossible to be incorporated, by heating with certain additives.


福島の環境回復に向けた取り組み,4; 汚染土壌の除染、減容化および再生利用を目指した物理処理及び新しい熱処理法開発への試み

矢板 毅; 本田 充紀; 下山 巖; 伊藤 健一*; 万福 裕蔵*; 辻 卓也; 松村 大樹

日本原子力学会誌ATOMO$$Sigma$$, 59(8), p.483 - 487, 2017/08




下山 巖; 本田 充紀; 小暮 敏博*; 馬場 祐治; 平尾 法恵*; 岡本 芳浩; 矢板 毅; 鈴木 伸一

Photon Factory News, 35(1), p.17 - 22, 2017/05



Mechanism of Cs removal from Fukushima weathered biotite by heat treatment with a NaCl-CaCl$$_{2}$$ mixed salt

本田 充紀; 岡本 芳浩; 下山 巖; 塩飽 秀啓; 鈴木 伸一; 矢板 毅

ACS Omega (Internet), 2(2), p.721 - 727, 2017/02

 被引用回数:15 パーセンタイル:58.32(Chemistry, Multidisciplinary)

An in situ extended X-ray absorption fine structure (in situ EXAFS) spectroscopic analysis at high temperature was conducted to investigate the mechanism of Cs removal from weathered biotite (WB) from Fukushima, induced by heating with a mixed salt of NaCl and CaCl$$_{2}$$. This indicated that most Cs remained in WB during heating at 200-700$$^{circ}$$C. In addition, the in situ EXAFS spectra gradually changed on heating with the mixed salt and a completely different spectrum was observed for the sample after cooling from 700$$^{circ}$$C to room temperature. Ex situ EXAFS measurements and X-ray fluorescence analyses were also conducted on samples after heat treatment and removal of the mixed salt to clarify the temperature dependence of the Cs removal ratio. Based on the results of radial structure function analysis obtained from in situ EXAFS, we concluded that almost all Cs was removed from WB by heating at 700$$^{circ}$$C with the mixed salt, and that Cs formed CsCl bonds after cooling to room temperature from 700$$^{circ}$$C. In contrast, although more than half of the Cs present was removed from WB by heat treatment at 500$$^{circ}$$C, most Cs was surrounded by silica tetrahedrons, maintained by Cs-O bonds. On the basis of these results, different Cs removal processes are suggested for the high-temperature (600-700$$^{circ}$$C) and low-temperature (400-500$$^{circ}$$C) regions.


X-ray absorption fine structure at the cesium $$L$$3 absorption edge for cesium sorbed in clay minerals

本田 充紀; 下山 巖; 岡本 芳浩; 馬場 祐治; 鈴木 伸一; 矢板 毅

Journal of Physical Chemistry C, 120(10), p.5534 - 5538, 2016/03

 被引用回数:16 パーセンタイル:59.27(Chemistry, Physical)

We present the use of near-edge X-ray absorption fine structure (NEXAFS) to investigate local electronic structures of cesium ions sorbed in two types of clay minerals (vermiculite and kaolinite) with a different capacity to fix Cs. NEXAFS is element specific because X-ray absorption edges of different elements have different energies. However, the energy of the Cs $$L$$3 absorption edge is close to that of the $$K$$-edge of titanium generally contained in clay minerals. Therefore, Cs $$L$$3-edge NEXAFS measurements of Cs in clay minerals have not yet succeeded. In this study, we successfully measured pure Cs $$L$$3-edge NEXAFS spectra for cesium sorbed in clay minerals by completely separating Ti $$K alpha$$ and Cs $$L alpha$$ fluorescence X-rays using a fluorescence method. We confirmed the peak intensity between vermiculite and kaolinite in the NEXAFS spectra. To clarify the identification of NEXAFS spectra, theoretical calculations were performed using the discrete variational X$$alpha$$ molecular orbital method (DV-X$$alpha$$), and peak identification was achieved. The difference in peak intensity was explained by the difference in the electron density of unoccupied molecular orbitals. We studied the influence of water molecules and found a change in the electron densities of unoccupied molecular orbitals caused by the coordination of water molecules.


Development of fluorescence XAFS system in soft X-ray region toward operando conditions using polycapillary X-ray lens

本田 充紀; 下山 巖; 馬場 祐治; 鈴木 伸一; 岡本 芳浩; 矢板 毅

e-Journal of Surface Science and Nanotechnology (Internet), 14, p.35 - 38, 2016/02

We developed a fluorescence XAFS system toward operando conditions using soft X-ray radiation at KEK-PF BL-27A. X-ray adsorption fine structure (XAFS) analysis in the soft X-ray region is useful for elucidating molecular structures in both atmosphere and solutions. Particularly, light elements play an important role in many cases in this energy region. The attenuation of soft X-rays in a solution is large compared to that of hard X-rays. Thus, appropriate spectral statistics cannot be obtained in the soft X-ray region. Recently, using fluorescence XAFS measurement at the S K-edge (2.4 keV), we found that biological molecules containing sulfur atoms adopt specific molecular structures under different pH conditions in a solution. However, the diameter of the beam of this beam line at BL-27A was large, leading to difficulties in uniformly irradiating only the sample surface. Therefore, it was necessary to uniformly irradiate samples using a small-area X-ray beam. To collimate the beam and improve its intensity, we installed an X-ray focusing device. Herein, we introduce a light-collecting device that uses a polycapillary X-ray lens to focus soft X-rays. After installing this lens, we confirmed that focused X-rays and a higher-intensity beam were achieved. We conclude that focusing X-rays using a polycapillary lens in the soft X-ray region is an effective method for obtaining better spectral statistics in fluorescence XAFS measurements.


Observation of oriented organic semiconductor using Photo-Electron Emission Microscope (PEEM) with polarized synchrotron

関口 哲弘; 馬場 祐治; 平尾 法恵; 本田 充紀; 和泉 寿範; 池浦 広美*

Molecular Crystals and Liquid Crystals, 622(1), p.44 - 49, 2015/12


 被引用回数:0 パーセンタイル:0.01(Chemistry, Multidisciplinary)

分子配向は有機半導体材料の様々な性能を制御する上で重要な因子の一つである。一般に薄膜材料は様々な方向を向く微小配向領域の混合状態となっている。したがって、各々の微小領域において配向方向を選別して顕微分光観測できる手法が望まれてきた。我々は、光電子顕微鏡(PEEM)法と直線偏光性をもつ放射光X線や真空紫外(VUV)光を組み合わせる装置の開発を行っている。ポリ(3-ヘキシルチオフェン)(P3HT)導電性ポリマー薄膜を溶液法により作製し、偏光放射光励起によるPEEM像の観測を行った。また様々な偏光角度のUV照射下におけるPEEM像を測定した。放射光励起実験において各微小領域の硫黄S 1s励起X線吸収スペクトルが得られ、微小領域におけるポリマー分子配向の情報を得ることができた。またUV励起実験においては、偏光角度に依存して異なる微結晶層を選択観測することに成功した。実験結果はポリマーの特定の分子軸へ向いた配向領域だけを選択的に顕微鏡観測できることを示唆する。


Integrated tokamak modelling with the fast-ion Fokker-Planck solver adapted for transient analyses

藤間 光徳; 濱松 清隆; 林 伸彦; 本多 充; 井手 俊介

Plasma Physics and Controlled Fusion, 57(9), p.095007_1 - 095007_9, 2015/09

 被引用回数:3 パーセンタイル:17.78(Physics, Fluids & Plasmas)



Advance in integrated modelling towards prediction and control of JT-60SA plasmas

林 伸彦; 本多 充; 白石 淳也; 宮田 良明; 若月 琢馬; 星野 一生; 藤間 光徳; 鈴木 隆博; 浦野 創; 清水 勝宏; et al.

Europhysics Conference Abstracts (Internet), 39E, p.P5.145_1 - P5.145_4, 2015/06

Towards prediction and control of JT-60SA plasmas, we are developing codes/models which can describe physics/engineering factors, and integrating them to one code TOPICS. Physics modelling: Coupling with MINERVA/RWMaC code showed that MHD equilibrium variation by centrifugal force largely affects RWM stability and the toroidal rotation shear stabilizes RWM. Coupling with OFMC code for NB torques, 3D MHD equilibrium code VMEC and drift-kinetic code FORTEC-3D for NTV torque, and toroidal momentum boundary model, predicted the core rotation of $$sim$$2% of Alfv$'e$n speed for a ITER hydrogen L-mode plasma. Coupling with core impurity transport code IMPACT showed the accumulation of Ar seeded to reduce the divertor heat load is so mild that plasma performance can be recovered by additional heating in JT-60SA steady-state (SS) scenario. Simulations coupled with MARG2D code showed that plasma current can be ramped-up to reach $$beta_N ge$$3 with MHD modes stabilized by ideal wall and with no additional flux consumption of central solenoid in JT-60SA. Engineering modelling: Coupling with integrated real-time controller showed that simultaneous control of $$beta_N$$ and $$V_{loop}$$ is possible at $$beta_N ge$$4 in JT-60SA SS scenarios. MHD equilibrium control simulator MECS demonstrated equilibrium control during heating phase and collapse induced events within power supply capability of PF coils in JT-60SA.


A Fluorescence XAFS measurement instrument in the Soft X-ray region toward observation under operando conditions

本田 充紀; 馬場 祐治; 下山 巖; 関口 哲弘

Review of Scientific Instruments, 86(3), p.035103_1 - 035103_5, 2015/03

 被引用回数:8 パーセンタイル:43.44(Instruments & Instrumentation)

X-ray absorption fine structure (XAFS) measurements are widely used for the analysis of electronic structure. Generally, XAFS in the soft X-ray region is measured under vacuum, but chemical structures under vacuum are typically different from those under operando conditions, where chemical species exhibit their function. Here we developed an XAFS measurement instrument, as a step toward operando fluorescent yield XAFS measurement using synchrotron radiation in the soft X-ray region. We applied this method to analyze the local electronic structure of the sulfur atoms in L-cysteine in different pH solution. Our results show that this instrument aimed toward operando fluorescence XAFS measurements in the soft X-ray region is useful for structural analysis of sulfur atoms in organic molecules in air and in solution. The instrument will be applied to the structural analysis of materials containing elements that have absorption edges in soft X-ray region, such as phosphorus and alkali metals (potassium and cesium). It will be also particularly useful for the analysis of samples that are difficult to handle under vacuum and materials that have specific functions in solution.


Investigation of the influence of coadsorbent dye upon the interfacial structure of dye-sensitized solar cells

本田 充紀; 柳田 真利*; Han, L.*; 宮野 健次郎*

Journal of Chemical Physics, 141(17), p.174709_1 - 174709_7, 2014/11


 被引用回数:7 パーセンタイル:26.71(Chemistry, Physical)

The interface between Ru(tcterpy)(NCS)$$_{3}$$TBA$$_{2}$$ [black dye (BD); tcterpy = 4,4',4''-tricarboxy-2,2':6',2''-terpyridine, TBA = tetrabutylammonium cation] and nanocrystalline TiO$$_{2}$$, as found in dye-sensitized solar cells, is investigated by soft-X-ray synchrotron radiation and compared with the adsorption structure of $$cis$$-Ru(Hdcbpy)$$_{2}$$(NCS)$$_{2}$$TBA$$_{2}$$ (N719; dcbpy = 4,4'-dicarboxy-2,2'-bipyridine) on TiO$$_{2}$$ to elucidate the relationship between the adsorption mode of BD and the photocurrent with and without coadsorbed indoline dye D131. The depth profile is characterized with X-ray photoelectron spectroscopy and S $$K$$-edge X-ray absorption fine structure using synchrotron radiation. Both datasets indicate that one of the isothiocyanate groups of BD interacts with TiO$$_{2}$$ via its S atom when the dye is adsorbed from a single-component solution. In contrast, the interaction is slightly suppressed when D131 is coadsorbed, indicated by the fact that the presence of D131 changes the adsorption mode of BD. Based upon these results, the number of BD dye molecules interacting with the substrate is shown to decrease by 10% when D131 is coadsorbed, and the dissociation is shown to be related to the short-circuit photocurrent in the 600-800 nm region. The design of a procedure to promote the preferential adsorption of D131 therefore leads to an improvement of the short-circuit current and conversion efficiency.


Electrochemical immobilization of biomolecules on gold surface modified with monolayered L-cysteine

本田 充紀; 馬場 祐治; 関口 哲弘; 下山 巖; 平尾 法恵

Thin Solid Films, 556, p.307 - 310, 2014/04

 被引用回数:5 パーセンタイル:27.7(Materials Science, Multidisciplinary)

Immobilization of organic molecules on the top of a metal surface is not easy because of lattice mismatch between organic and metal crystals. Herein, we suggested that a monolayer of L-cysteine deposited on a gold surface can act as a buffer layer to immobilize biomolecules on the metal surface. We selected lactic acid as the immobilized biomolecule because it is one of the simplest carboxyl-containing biomolecules. The immobilization of lactic acid on the metal surface was carried out by an electrochemical method in an aqueous environment. The surface chemical states before and after the electrochemical reaction were characterized using X-ray photoelectron spectroscopy (XPS). The N 1s and C 1s XPS spectra showed that the L-cysteine-modified gold surface can immobilize lactic acid via peptide bonds. This technique might enable the immobilization of large organic molecules and biomolecules.


Labeling co-sensitizer dye for XPS quantification in coadsorption dye-sensitized solar cells

本田 充紀; 柳田 真利*; Han, L.*; 宮野 健次郎*

e-Journal of Surface Science and Nanotechnology (Internet), 12, p.63 - 67, 2014/02

Quantifying the coadsorption of dye molecules on nanoporous TiO$$_{2}$$ is difficult because of the complex adsorption structure between the dye and TiO$$_{2}$$ surface. D131 dye absorbs strongly in the ultraviolet region and is a common co-sensitizer for dye-sensitized solar cells. In this study, we showed that Cl-terminated D131 dye coadsorbed with a Ru complex on nanoporous TiO$$_{2}$$ can be used as a labeling compound to quantify coadsorption systems by X-ray photoelectron spectroscopy (XPS). Cl-terminated D131 alone and Cl-terminated D131 and N719 coadsorbed on nanoporous TiO$$_{2}$$ were measured with XPS. The Cl atoms were quantified by the peak intensity ratio of the Cl 1s and Ti 2p peaks. In the Cl-terminated D131 + N719 coadsorption system, the amount of Cl-terminated D131 dye adsorbed decreased by about 44% for the 1:1 mixture. Our technique could also be used to quantify other dyes in co-sensitizer systems, such as black dye and N3 dye.


Orientation effect of organic semiconducting polymer revealed using Photo-Electron Emission Microscope (PEEM)

関口 哲弘; 馬場 祐治; 下山 巖; 平尾 法恵; 本田 充紀; 和泉 寿範; 池浦 広美*

Photon Factory Activity Report 2013, Part B, P. 546, 2014/00

分子配向性は有機半導体材料の様々な性能を制御する上で重要である。一般に薄膜材料は様々な方向を向いた微小配向領域の混合状態である。したがって、各微小領域の配向方向を選択して顕微分光観測できる手法の開発が望まれている。我々は、光電子顕微鏡(PEEM)法と直線偏光性をもつ放射光X線や真空紫外(VUV)光を組み合わせる装置の開発を行っている。ポリ(3-ヘキシルチオフェン)(P3HT)導電性ポリマー薄膜を溶液法により作製した。偏光放射光励起により特定方向を向くポリマー分子鎖領域のPEEM像の観測を行うことができた。各微小領域の硫黄S 1s励起X線吸収スペクトルが得られ、微小領域におけるポリマー分子配向の情報を得ることに成功した。


高圧力下で形成される岩塩構造ランタン1水素化物; 放射光X線と中性子の利用による新しい希土類金属水素化物の発見

町田 晃彦; 本田 充紀*; 服部 高典; 佐野 亜沙美; 綿貫 徹; 片山 芳則; 青木 勝敏; 大下 英敏*; 池田 一貴*; 大友 季哉*

波紋, 23(2), p.131 - 136, 2013/05



Orientation of silicon phthalocyanine thin films revealed using polarized X-ray absorption spectroscopy

関口 哲弘; 馬場 祐治; 下山 巖; 平尾 法恵; 本田 充紀; Deng, J.*

Photon Factory Activity Report 2012, Part B, P. 68, 2013/00

有機半導体の表面分子配向は電子デバイスの性能向上の上で不可欠である。スピンコート法によりシリコンフタロシアニン二塩化物(SiPcCl$$_{2}$$)薄膜をグラファイト上に作製し、大気圧下で加熱(350度)を行った。角度分解X線吸収端微細構造(NEXAFS)法とXPS法により生成物薄膜の分子配向と組成を調べた。Si 1s吸収端のNEXAFSスペクトルは角度依存を示し、表面反応生成物が分子配向していることを示した。ab initio分子軌道法計算との比較により生成物は水和重合生成物(SiPcO)nに類似した構造であると推察した。


Formation of NaCl-type monodeuteride LaD by the disproportionation reaction of LaD$$_{2}$$

町田 晃彦; 本田 充紀*; 服部 高典; 佐野 亜沙美; 綿貫 徹; 片山 芳則; 青木 勝敏; 小松 一生*; 有馬 寛*; 大下 英敏*; et al.

Physical Review Letters, 108(20), p.205501_1 - 205501_5, 2012/05

 被引用回数:10 パーセンタイル:58.4(Physics, Multidisciplinary)



Microscopic observation of lateral diffusion at Si-SiO$$_{2}$$ interface by photoelectron emission microscopy using synchrotron radiation

平尾 法恵; 馬場 祐治; 関口 哲弘; 下山 巖; 本田 充紀*

Applied Surface Science, 258(3), p.987 - 990, 2011/11

 被引用回数:3 パーセンタイル:17.85(Chemistry, Physical)


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