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報告書

高レベル放射性物質研究施設における放射性廃液の安定化処理

小木 浩通*; 荒井 陽一; 粟飯原 はるか; 渡部 創; 柴田 淳広; 野村 和則

JAEA-Technology 2021-007, 27 Pages, 2021/06

JAEA-Technology-2021-007.pdf:2.43MB

放射性物質取扱施設である高レベル放射性物質研究施設(CPF: Chemical Processing Facility)では、過去の試験や分析で発生した多種の廃液をホットセル及びグローブボックス内で保管してきた。2015年7月より、保管されている放射性廃液について、管理方法の適正化を図るべく、実廃液の安定化処理を進めている。また、分析廃液等の多種多様な試薬が混在する廃液については安定化処理が非常に困難であるため、大学等と共同でSTRAD(Systematic Treatments of Radioactive liquid wastes for Decommissioning)プロジェクトを発足させ、処理技術の研究開発を進めている。これらの実績は、他の放射性物質取り扱い施設においても保管する廃液の処理をより効率的かつ安全に進められることが期待できる。本書は、CPFで安定化処理を実施した実廃液の処理方法及び処理状況に関して報告するものである。

論文

Coexistence of two components in magnetic excitations of La$$_{2-x}$$Sr$$_{x}$$CuO$$_{4}$$ ($$x$$ = 0.10 and 0.16)

佐藤 研太朗*; 池内 和彦*; 梶本 亮一; 脇本 秀一; 新井 正敏*; 藤田 全基*

Journal of the Physical Society of Japan, 89(11), p.114703_1 - 114703_7, 2020/11

 被引用回数:1 パーセンタイル:34.55(Physics, Multidisciplinary)

To elucidate the spin dynamics of La$$_{2-x}$$Sr$$_{x}$$CuO$$_{4}$$, which couples with the charge degree of freedom, the spin excitations spanning the characteristic energy ($$E_mathrm{cross}$$ $$sim$$ 35-40 meV) are investigated for underdoped $$x$$ = 0.10 and optimally doped (OP) $$x$$ = 0.16 through inelastic neutron scattering measurements. Analysis based on a two-component picture of high-quality data clarified the possible coexistence of upright standing incommensurate (IC) excitations with gapless commensurate (C) excitations in the energy-momentum space. The IC component weakens the intensity toward $$E_mathrm{cross}$$ with increasing energy transfer ($$hbaromega$$), whereas the C component strengthens at high-$$hbaromega$$ regions. The analysis results imply that the superposition of two components with a particular intensity balance forms an hourglass-shaped excitation in appearance. Furthermore, the temperature dependence of the intensity of each component exhibits different behaviors; the IC component disappears near the pseudo-gap temperature ($$T^*$$) upon warming, whereas the C component is robust against temperature. These results suggest the itinerant electron spin nature and the localized magnetism of the parent La$$_{2}$$CuO$$_{4}$$ in IC and C excitations, respectively, similar to the spin excitations in the OP YBa$$_{2}$$Cu$$_{3}$$O$$_{6+delta}$$ and HgBa$$_{2}$$CuO$$_{4+delta}$$ with higher superconducting-transition temperatures.

論文

Microscopic analyses on Zr adsorbed IDA chelating resin by PIXE and EXAFS

荒井 陽一; 渡部 創; 大野 真平; 野村 和則; 中村 文也*; 新井 剛*; 瀬古 典明*; 保科 宏行*; 羽倉 尚人*; 久保田 俊夫*

Nuclear Instruments and Methods in Physics Research B, 477, p.54 - 59, 2020/08

 被引用回数:0 パーセンタイル:0.02(Instruments & Instrumentation)

Used PUREX process solvent generated from reprocessing process of spent nuclear fuel contains a small amount of U and Pu complexed with tributyl phosphate (TBP) or dibutyl phosphate (DBP). The radioactive nuclides should be removed from the solvent for safety storage or disposal. The iminodiacetic acid (IDA) type chelating resin was proposed as promising procedures for efficient recovery of the trapped cations in the solvent. In order to reveal the distribution and amount of Zr in the particle and local structure of Zr complex formed in the adsorbent, PIXE and EXAFS analyses on the Zr adsorbed chelating resin were carried out. Micro-PIXE analysis proved that it is an effectual method for quantitative analysis of trace adsorbed elements. Moreover, some of the adsorption sites were possibly occupied by the molecules. On the other hand, Zr-K edge EXAFS analysis suggested that extraction mechanism of Zr from the aqueous solution and the solvent was different.

論文

Quantitative analysis of Zr adsorbed on IDA chelating resin using Micro-PIXE

荒井 陽一; 渡部 創; 大野 真平; 野村 和則; 中村 文也*; 新井 剛*; 瀬古 典明*; 保科 宏行*; 久保田 俊夫*

QST-M-23; QST Takasaki Annual Report 2018, P. 59, 2020/03

Radioactive spent solvent waste contains U and Pu is generated from reprocessing process of spent nuclear fuel. The nuclear materials should be removed from the solvent for safety storage or disposal. We are focusing on the nuclear materials recovery from spent solvent using imino diacetic acid (IDA) type chelating resin as a promising method. In order to reveal adsorbed amount of Zr, which is simulated of Pu, Micro-Particle Induced X-ray Emission (PIXE) was carried out. Micro-PIXE analysis succeeded in quantitative analysis on trace amount of adsorbed Zr from simulated spent solvent.

論文

STRAD project for systematic treatments of radioactive liquid wastes generated in nuclear facilities

渡部 創; 小木 浩通*; 荒井 陽一; 粟飯原 はるか; 高畠 容子; 柴田 淳広; 野村 和則; 神谷 裕一*; 浅沼 徳子*; 松浦 治明*; et al.

Progress in Nuclear Energy, 117, p.103090_1 - 103090_8, 2019/11

 被引用回数:5 パーセンタイル:58.77(Nuclear Science & Technology)

A new collaborative research project for systematic treatments of radioactive liquid wastes containing various reagents generating in nuclear facilities was started from 2018 initiated by Japan Atomic Energy Agency. The project was named as STRAD (Systematic Treatments of RAdioactive liquid wastes for Decommissioning) project. Tentative targets to be studied under the project are aqueous and organic liquid wastes which have been generated by experiments and analyses in a reprocessing experimental laboratory of JAEA. Currently fundamental studies for treatments of the liquid wastes with complicated compositions are underway. In the STRAD project, process flow for treatment of ammonium ion involved in aqueous waste was designed though the inactive experiments, and decomposition of ammonium ion using catalysis will be carried out soon. Adsorbents for recovery of U and Pu from spent solvent were also developed. Demonstration experiments on genuine spent solvent is under planning.

論文

Q dependence of magnetic resonance mode on FeTe$$_{0.5}$$Se$$_{0.5}$$ studied by inelastic neutron scattering

石角 元志*; 樹神 克明; 梶本 亮一; 中村 充孝; 稲村 泰弘; 池内 和彦*; Ji, S.*; 新井 正敏*; 社本 真一

Condensed Matter (Internet), 4(3), p.69_1 - 69_10, 2019/09

中性子非弾性散乱により観測された磁気共鳴モードのQ依存性という初めての手法で、FeTe$$_{0.5}$$Se$$_{0.5}$$の超伝導対称性がs$$pm$$波であることを実験的に示した。

論文

Stabilization processing of hazardous and radioactive liquid wastes derived from advanced aqueous separation experiments for safety handling and management of waste

中原 将海; 渡部 創; 小木 浩通*; 荒井 陽一; 粟飯原 はるか; 本山 李沙; 柴田 淳広; 野村 和則; 梶並 昭彦*

Proceedings of International Nuclear Fuel Cycle Conference / Light Water Reactor Fuel Performance Conference (Global/Top Fuel 2019) (USB Flash Drive), p.66 - 70, 2019/09

高レベル放射性物質研究施設では、先進湿式分離試験に由来する多種多様な有害性及び放射性液体廃棄物が発生する。そのため、これらを安全に取り扱い及び管理するために安定化処理を行う必要がある。今回は、これらの溶液に含まれる有害物質の沈殿処理若しくは酸化処理、核物質回収のための溶媒抽出による分離、フリーズドライ法を用いた濃縮処理について報告する。

論文

Characterization of the insoluble sludge from the dissolution of irradiated fast breeder reactor fuel

粟飯原 はるか; 荒井 陽一; 柴田 淳広; 野村 和則; 竹内 正行

Procedia Chemistry, 21, p.279 - 284, 2016/12

BB2015-3214.pdf:0.31MB

 被引用回数:3 パーセンタイル:92.31

Insoluble sludge is generated in reprocessing process. Actual sludge data, which had been obtained from the dissolution experiments of irradiated fuel of fast reactor "Joyo" were reevaluated especially from the view point of the characterization of sludge. The yields of sludge were calculated from the weight and there were less than 1%. Element concentrations of sludge were analyzed after decomposing by alkaline fusion. As the results, molybdenum, technetium, ruthenium, rhodium and palladium accounted for mostly of the sludge. From their chemical compositions and structure analyzed by XRD show good agree that main component of sludge is Mo$$_{4}$$Ru$$_{4}$$RhPdTc regardless of the experimental condition. At the condition of reprocessing fast breeder fuel, it is indicated that molybdenum and zirconium in dissolved solution is low, therefore zirconium molybdate hydrate may not produce abundant amount in the process.

論文

MAGIC chopper; Basic concept and experimental evaluation

中村 充孝; 池内 和彦*; 梶本 亮一; 神原 理; Krist, T.*; 篠原 武尚; 新井 正敏; 飯田 一樹*; 蒲沢 和也*; 稲村 泰弘; et al.

JAEA-Conf 2015-002, p.339 - 348, 2016/02

チョッパー分光分光器におけるMulti-Ei法において、すべての入射エネルギーに対して実験条件を最適化できる新規チョッパー(マジックチョッパー)を開発した。本研究では、マジックチョッパーの基本概念に加えて、モンテカルロシミュレーションや中性子透過実験で評価されたマジックチョッパーの性能について紹介する。

論文

Recent progress in the chopper spectrometer 4SEASONS at J-PARC

梶本 亮一; 中村 充孝; 稲村 泰弘; 蒲沢 和也*; 池内 和彦*; 飯田 一樹*; 石角 元志*; 中島 健次; 河村 聖子; 中谷 健; et al.

JAEA-Conf 2015-002, p.319 - 329, 2016/02

4SEASONS ($textit{SIKI}$) is one of the three chopper spectrometers operating in MLF at J-PARC, and covers thermal neutron region ($$10^0$$ - $$10^2$$ meV) with relaxed resolution and high flux. The repetition rate multiplication by the Fermi chopper on this short length (18 m between the source and the sample) spectrometer enables wide-band multiple-incident-energy (multi-$$E_mathrm{i}$$) measurements, which proved to be useful in observing hierarchical structures in excitations over a large energy scale. On the other hand, the upgrading work of the spectrometer has been continued since the first inelastic scattering experiment in 2009. For examples, we took several measures to suppress background, installed new detectors recently, and are developing a new Fermi chopper now. In the presentation, we show examples of scientific outputs from the spectrometer which benefit from the multi-$$E_mathrm{i}$$ measurements, and recent or planned upgrades of the instrument.

論文

Background caused by continuously emitted high-energy neutrons at the chopper spectrometer 4SEASONS

梶本 亮一; 中村 充孝; 稲村 泰弘; 蒲沢 和也*; 池内 和彦*; 飯田 一樹*; 石角 元志*; 中島 健次; 原田 正英; 新井 正敏

JPS Conference Proceedings (Internet), 8, p.036001_1 - 036001_6, 2015/09

The background that appears in spectra acquired by the chopper spectrometer 4SEASONS at J-PARC was investigated. A continuous background that oscillates in synch with the rotation of the Fermi chopper was observed even when neutrons should be suppressed. The characteristics of the background strongly suggest that high-energy delayed neutrons continuously emitted from the mercury target are its cause.

論文

Neutron scattering study of spin fluctuations in La$$_{2-x}$$Sr$$_{x}$$CuO$$_{4}$$ by four-dimensional mapping of neutron cross-sections using the 4SEASONS chopper spectrometer

脇本 秀一; 池内 和彦*; 新井 正敏; 藤田 全基*; 梶本 亮一; 川村 奨*; 松浦 直人*; 中島 健次; 山田 和芳*

JPS Conference Proceedings (Internet), 8, p.034013_1 - 034013_6, 2015/09

Previous neutron results of La$$_{2-x}$$Sr$$_{x}$$CuO$$_{4}$$ (LSCO) by TOF measurements revealed that magnetic dynamical structure factor has a maximum at $$sim$$ 18 meV. To clarify the origin of the maximum, we carried out 4 dimensional mapping of dynamical structure factor $$S(Q, omega)$$ to see details of both magnons and phonons. We found that $$x$$ = 0 shows ordinary spin waves while $$x$$ = 0.08 shows a maximum at $$sim$$ 18 meV where $$Q$$-independent phonon branch crosses. This imply that in superconducting compositions phonon may also indirectly related to the superconductivity.

論文

Basic study on radiation degradation of potassium nickel ferrocyanide

荒井 陽一; 渡部 創; 高畠 容子; 中村 雅弘; 中島 靖雄

Proceedings of 2014 Nuclear Plant Chemistry Conference (NPC 2014) (USB Flash Drive), 8 Pages, 2014/10

放射性廃液からの放射性セシウムの除去は放射性廃棄物低減化に対して有効な手段であることから、その放射性セシウムの選択的除去のためにフェロシアン化物を用いた研究が行われている。フェロシアン化物の廃棄物は水を含んだスラリー状であり、フェロシアン化物の存在により放射線照射による水の分解に起因する水素の生成に影響を与える可能性が考えられる。また、フェロシアン化物は、その構造にシアンを含むことから、分解によりシアンが放出される可能性がある。そこで、水に浸漬させた状態でフェロシアン化ニッケルカリウム(KNiFC)に$$^{60}$$Coによる$$gamma$$線を照射し、水素やシアンの発生量を測定し、KNiFCの放射線分解について調査した。本試験の結果、KNiFCの存在により水素のG値が増大することを確認した。よって、KNiFCを貯槽等で保管する場合には掃気により水素濃度を減少させることが必要である。なお、Csの吸着の有無は水素の発生に影響しないことについても確認した。また、6MGyの照射により、溶液中にシアンが検出されたものの、その生成量は1.3mg/Lと十分に低い濃度であり、ガス化したシアン化水素は検出されなかった。

論文

Temperature dependence of spin fluctuations in underdoped La$$_{1.90}$$Sr$$_{0.10}$$CuO$$_4$$

佐藤 研太朗*; 松浦 直人*; 藤田 全基*; 梶本 亮一; Ji, S.*; 池内 和彦*; 中村 充孝; 稲村 泰弘; 新井 正敏; 榎木 勝徳*; et al.

JPS Conference Proceedings (Internet), 3, p.017010_1 - 017010_6, 2014/06

We studied the temperature dependence of spin excitation in the underdoped La$$_{1.90}$$Sr$$_{0.10}$$CuO$$_{4}$$ in a wide energy range. At low temperature, a clear magnetic signal emerging from incommensurate (IC) (0.5$$pm$$0.09, 0.5) positions was observed. The low-energy ($$sim$$10 meV) IC signal was confirmed at 200K, while the IC signal gradually merges upon warming and turns into a single commensurate peak centered at (0.5, 0.5) at 300 K. The overall spectral shape above $$sim$$60 meV measured at 5 K and 350 K was almost the same, meaning the weak thermal effect on the high-energy dispersion relation. This weak change in the high-energy dispersion is consistent with the localized spin picture, whereas the robust IC structure against the temperature would be difficult to explain within a simple stripe model.

論文

Energy- and $$Q$$-resolution investigations of a chopper spectrometer 4SEASONS at J-PARC

飯田 一樹*; 池内 和彦*; 石角 元志*; 鈴木 淳市; 梶本 亮一; 中村 充孝; 稲村 泰弘; 新井 正敏

JPS Conference Proceedings (Internet), 1, p.014016_1 - 014016_4, 2014/03

4SEASONS is one of the inelastic neutron scattering instruments in the pulsed neutron facility in J-PARC. It utilizes a Fermi chopper to monochromate the neutron beam generated incident on a sample and a large-area detector system to detect the scattered neutrons as functions of position and time, and analyzes the momentums and energies of excitations in the sample with the time-of-flight technique. The instrument has been developed to perform high-efficiency measurements of weak inelastic signals on novel spin and lattice dynamics in the energy region of 10$$^0$$ - 10$$^{2}$$ meV. The ability to utilize multiple incident-energies simultaneously, in addition to the recent improvement in the signal-to-noise ratio, has made 4SEASONS one of the best chopper spectrometers in the world. In the presentation, we will show the recent scientific outputs and upgrades of the instrument.

論文

Feasibility demonstration of a new Fermi chopper with supermirror-coated slit package

中村 充孝; 神原 理; Krist, T.*; 篠原 武尚; 池内 和彦*; 新井 正敏; 梶本 亮一; 中島 健次; 田中 浩道; 鈴木 淳市*; et al.

Nuclear Instruments and Methods in Physics Research A, 737, p.142 - 147, 2014/02

 被引用回数:3 パーセンタイル:30.24(Instruments & Instrumentation)

チョッパー分光器における非弾性中性子散乱実験の効率は、複数の入射エネルギーを同時利用することで劇的に向上しうる。しかしながら、通常のチョッパーでは全ての入射エネルギーに対して実験条件を最適化することは絶対的に不可能である。我々は、この問題点を克服すべく中性子スーパーミラーを貼付したスリットパッケージを有する新型フェルミチョッパーを開発し、複数の入射エネルギーそれぞれに対して実験条件を最適化しうることを実験的に実証した。

論文

Temperature dependence of spin excitations in the frustrated spin chain system CuGeO$$_3$$

藤田 全基*; Frost, C. D.*; Bennington, S. M.*; 梶本 亮一; 中村 充孝; 稲村 泰弘; 水野 文夫*; 池内 和彦*; 新井 正敏

Journal of the Physical Society of Japan, 82(8), p.084708_1 - 084708_5, 2013/08

 被引用回数:1 パーセンタイル:12.76(Physics, Multidisciplinary)

We studied the temperature dependence of the spin excitation spectrum in the frustrated spin chain system CuGeO$$_3$$ by a time-of-flight neutron scattering measurement. The intensity hump along the upper boundary (UB) of the continuum excitation, which is a robust feature for significant competition between next-nearest-neighbor (NNN) and nearest-neighbor (NN) exchange interactions, was shown to degrade upon warming. The hump disappears above $$sim$$90 K, whereas the outline of the two-spin on continuum excitation remains even at 180 K. The decrease in intensity at the UB suggests that the contribution of NNN interaction to form the thermodynamic equilibrium state becomes negligible as a result of the thermal perturbation. The intensity of the lowest excited mode at the magnetic zone center weakens concomitantly with that at the UB. This intensity reduction leads a change of the static structure factor from a single Lorentzian shape to a two peaked structure in the temperature range between 50 and 75 K. These results can be explained through the degradation of the spin dimer by thermal disturbance with remaining large NNN couplings at high temperature.

論文

Recent developments of instruments in a spallation neutron source at J-PARC and those prospects in the future

新井 正敏; 梶本 亮一; 中村 充孝; 稲村 泰弘; 中島 健次; 柴田 薫; 高橋 伸明; 鈴木 淳市*; 高田 慎一; 山田 武*; et al.

Journal of the Physical Society of Japan, 82(Suppl.A), p.SA024_1 - SA024_14, 2013/01

 被引用回数:6 パーセンタイル:47.28(Physics, Multidisciplinary)

J-PARC中性子散乱施設(1MW, 25Hzの短パルス中性子源)での実験装置の開発について記述したものである。大強度の結合型減速材を利用し、パルス整形チョッパーの利用により、新たな概念をもとにして高分解能装置の開発を行った。また、イベント・レコーディングによるデータ集積系の開発により、多重入射エネルギー法の実現も行った。さらに、回折計の高度化についても述べている。

論文

Optimization of a Fermi chopper for an inelastic neutron spectrometer with focusing guide

池内 和彦*; 中村 充孝; 梶本 亮一; 新井 正敏

Journal of the Physical Society of Japan, 82(Suppl.A), p.SA038_1 - SA038_5, 2013/01

 被引用回数:4 パーセンタイル:37.08(Physics, Multidisciplinary)

In order to evaluate an optimum condition of a Fermi chopper, especially for the multiple-incident-energy (multi-$$E_i$$) method, we demonstrated a numerical simulation by Monte Carlo method and analytical calculation. In a calculation using the actual optical design of the Fermi chopper spectrometer 4SEASONS installed at Japan Proton Accelerator Research Complex (J-PARC), a peak width of a beam monochromated by the chopper becomes wider as the energy decreases. The energy dependence is found to be caused by the critical-reflection-angle of the neutron supermirror utilized for the ellipsoidal guide tubes. We argue that the energy dependence should be advantageous to realize the optimum condition for every monochromated beam in the multi-$$E_i$$ measurement by making it follow the energy dependence of the moderator pulse width.

論文

Dynamical spin susceptibility studied by inelastic neutron scattering on LaFeAsO$$_{1-x}$$F$$_{x}$$

社本 真一; 石角 元志; 脇本 秀一; 樹神 克明; 梶本 亮一; 新井 正敏

Journal of Physics; Conference Series, 340, p.012075_1 - 012075_6, 2012/02

 被引用回数:1 パーセンタイル:47.1

Low-energy spin excitations on polycrystalline LaFeAsO$$_{1-x}$$F$$_{x}$$ samples have been studied by inelastic neutron scattering. The $$Q$$-integrated dynamical spin susceptibility $$chi$$"($$omega$$) at 11 meV decreases with increasing fluorine content $$x$$ across the phase transition from antiferromagnetic to superconducting phases. For superconducting samples, a peak in $$chi$$"($$omega$$) develops at $$omega$$ = $$E$$$$_{rm res}$$ below $$T$$$$_{rm c}$$, accompanied by its reduction below $$E$$$$_{rm res}$$. Fe 3$$d$$ orbital contribution on the dynamical spin susceptibility and the electron scattering between $$Gamma$$and $$M$$ Fermi surfaces are discussed.

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