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論文

Measurements of neutron capture cross-section for nuclides of interest in decommissioning (II); $$^{58}$$Fe(n,$$gamma$$)$$^{59}$$Fe

中村 詔司; 芝原 雄司*; 遠藤 駿典; Rovira Leveroni, G.; 木村 敦

Journal of Nuclear Science and Technology, 62(3), p.300 - 307, 2025/03

https://doi.org/10.1080/00223131.2024.2427244
 被引用回数：0 パーセンタイル：0.00(Nuclear Science & Technology)

As nuclear facilities are dismantled in decommissioning, large amount of various waste is generated. Even more inconveniently, waste is radioactive due to neutron activation. Thus, the neutron capture cross-sections of nuclides targeted in decommissioning are required to evaluate the radioactivity produced. In this work, $$^{58}$$Fe nuclide was selected among objective nuclides for decommissioning, and its thermal-neutron capture cross-section was measured by a neutron activation method at the graphite thermal column of Kyoto University Research Reactor in 5-MW operation. The thermal-neutron capture cross-section was derived using ${it Westcott'}$s convention. The present work obtained 1.36$$pm$$0.03 barns for the $$^{58}$$Fe(n,$$gamma$$)$$^{59}$$Fe reaction. The present result supports the JENDL-5 evaluation within 2$$sigma$$. If updated with currently recommended nuclear data, some of the reported past data would support the present result.

論文

Measurements of neutron capture cross-section for nuclides of interest in decommissioning (III); $$^{170}$$Er(n,$$gamma$$)$$^{171}$$Er and $$^{180}$$Hf(n,$$gamma$$)$$^{181}$$Hf reactions

中村 詔司; 芝原 雄司*; 遠藤 駿典; Rovira Leveroni, G.; 木村 敦

Journal of Nuclear Science and Technology, 14 Pages, 2025/00

https://doi.org/10.1080/00223131.2025.2457589
 被引用回数：0 パーセンタイル：0.00(Nuclear Science & Technology)

In the decommissioning of nuclear facilities, large amounts of radioactive waste are generated due to neutron activation. In that case, neutron capture cross-sections of nuclides targeted in decommissioning are required to evaluate their radioactivities produced. The present study selected two nuclides, $$^{171}$$Er and $$^{181}$$Hf, among objective ones for decommissioning, and thermal-neutron capture cross-sections for their parent nuclides were measured by the neutron activation method at the Kyoto University Research Reactor under 1-MW operation. The thermal-neutron capture cross-sections were derived on the basis of Westcott's convention. The present study obtained the results as follows: 8.19$$pm$$0.35 barns for the $$^{170}$$Er(n,$$gamma$$)$$^{171}$$Er reaction and 13.57$$pm$$0.14 barns for the $$^{180}$$Hf(n,$$gamma$$)$$^{181}$$Hf reaction. As a by-product, the measurements of the Hf sample also yielded 0.427$$pm$$0.006 barns for the $$^{179}$$Hf(n,$$gamma$$)$$^{180m}$$Hf reaction. This study revealed that some experimental and data evaluations differ from the present results by more than the experimental uncertainties.

論文

Pulsed muon facility of J-PARC MUSE

下村 浩一郎*; 幸田 章宏*; Pant, A. D.*; 砂川 光*; 藤森 寛*; 梅垣 いづみ*; 中村 惇平*; 藤原 理賀; 反保 元伸*; 河村 成肇*; et al.

Interactions (Internet), 245(1), p.31_1 - 31_6, 2024/12

https://doi.org/10.1007/s10751-024-01863-8

J-PARC Muon Facility: MUSE (Muon Science Establishment) is responsible for the inter-university user program and the operation, maintenance, and construction of the muon beamlines, namely D-line, S-line, U-line, and H-line, along with the muon source at J-PARC Materials and Life Science Facility (MLF). In this paper, recent developments are briefly presented.

論文

Imaging Josephson vortices on curved junctions

藤澤 唯太*; Krishnadas, A*; Nakamura, Tomonori*; Hsu, C.-H.*; Smith, B. R. M.*; Pardo-Almanza, M*; Hiyane, Hoshu*; 永井 佑紀; 町田 理*; 岡田 佳憲*

Physical Review B, 110(22), p.224511_1 - 224511_5, 2024/12

https://doi.org/10.1103/PhysRevB.110.224511
 被引用回数：0 パーセンタイル：0.00(Materials Science, Multidisciplinary)

エキゾチックな超伝導体の超伝導磁束の振る舞いを明らかにすることは、今後のデバイス開発にとって重要である。超伝導体LiTi$$_{2}$$O$$_{4}$$(111)の薄膜を作製し、磁場中での電子状態を走査型トンネル顕微鏡によって観測した。その際、接合部分の曲率に応じて超伝導磁束の状態が大きく変化することがわかった。そして、その変化は理論計算によっても確かめられた。この結果は、Josephson磁束を実験的な構造変化によってコントロールできる可能性を示唆しており、今後の新たなデバイス開発において重要な結果となるだろう。

論文

Measurements of neutron capture cross-sections for nuclides of interest in decommissioning; $$^{45}$$Sc, $$^{63}$$Cu, $$^{64}$$Zn, $$^{109}$$Ag, and $$^{113}$$In

中村 詔司; 芝原 雄司*; 遠藤 駿典; Rovira Leveroni, G.; 木村 敦

Journal of Nuclear Science and Technology, 61(11), p.1415 - 1430, 2024/11

https://doi.org/10.1080/00223131.2024.2346347
 被引用回数：1 パーセンタイル：62.55(Nuclear Science & Technology)

廃止措置においては、生成放射能の評価に資する核データとして、中性子捕獲断面積を整備する必要がある。本研究では、整備すべき対象核種のうち$$^{45}$$Sc, $$^{63}$$Cu, $$^{65}$$Zn, $$^{109}$$Ag及び$$^{113}$$Inを選定し、KURのTC-Pnを用いてそれらの熱中性子捕獲断面積測定を行った。その結果、熱中性子捕獲断面積の結果が、以下のとおり得られた:$$^{45}$$Sc(n, $$gamma$$)$$^{46}$$Sc反応は27.18$$pm$$0.28 barn、$$^{63}$$Cu(n, $$gamma$$)$$^{64}$$Cu反応は4.34$$pm$$0.06 barn、$$^{64}$$Zn(n, $$gamma$$)$$^{65}$$Zn反応は0.719$$pm$$0.011 barn、$$^{109}$$Ag(n, $$gamma$$)$$^{rm 110m}$$Ag反応は4.05$$pm$$0.05 barn、そして$$^{113}$$In(n, $$gamma$$) $$^{114}$$In$$^{m1+m2}$$反応は8.53$$pm$$0.27 barn。ScとZnの結果は、これまでに報告されている評価値を誤差範囲で支持するが、一方、他の核種については評価値と異なる結果となった。得られた結果は、生成量評価にはもちろん、これらの核種を中性束モニタとして利用する場合に用いることが考えられる。

論文

Circular polarization measurement for individual gamma rays in capture reactions with intense pulsed neutrons

遠藤 駿典; 安部 亮太*; 藤岡 宏之*; 猪野 隆*; 岩本 修; 岩本 信之; 河村 しほり*; 木村 敦; 北口 雅暁*; 小林 龍珠*; et al.

European Physical Journal A, 60(8), p.166_1 - 166_10, 2024/08

https://doi.org/10.1140/epja/s10050-024-01392-6
 被引用回数：2 パーセンタイル：0.00(Physics, Nuclear)

Measurements of $$gamma$$-ray circular polarization emitted from neutron capture reactions provide valuable information for nuclear physics studies. The spin and parity of excited states can be determined by measuring the circular polarization from polarized neutron capture reactions. Furthermore, the $$gamma$$-ray circular polarization in a neutron capture resonance is crucial for studying the enhancement effect of parity nonconservation in compound nuclei. The $$gamma$$-ray circular polarization can be measured using a polarimeter based on magnetic Compton scattering. A polarimeter was constructed, and its performance indicators were evaluated using a circularly polarized $$gamma$$-ray beam. Furthermore, as a demonstration, the $$gamma$$-ray circular polarization was measured in $$^{32}$$S(n,$$gamma$$)$$^{33}$$S reactions with polarized neutrons.

論文

Quantification of bulk elemental composition for C-type asteroid Ryugu samples with nondestructive elemental analysis using muon beam

二宮 和彦*; 大澤 崇人; 寺田 健太郎*; 和田 大雅*; 長澤 俊作*; Chiu, I.-H.; 中村 智樹*; 他40名*

Meteoritics & Planetary Science, 59(8), p.2044 - 2057, 2024/08

https://doi.org/10.1111/maps.14135
 被引用回数：1 パーセンタイル：52.52(Geochemistry & Geophysics)

小惑星探査機「はやぶさ」2が持ち帰った小惑星リュウグウのサンプルは、太陽系の起源と進化を調べる上で重要である。ここでは、非破壊ミュオン元素分析法を用いて測定した123mgのリュウグウ試料の元素組成を報告する。3種類の炭素質コンドライトを用いたミュオンX線スペクトルから、元素組成とミュオンX線強度の関係を各元素について求めた。検量線は直線性を示し、リュウグウの元素組成は定量的に決定された。リュウグウの元素組成は、サンプル数が多いため、小惑星リュウグウの平均的なバルク元素組成を反映している。リュウグウの元素組成はオルグイユ(CI1)と類似しており、CI1に分類されるべきである。しかし、リュウグウのO/Si比はオルグイユのO/Si比より25%低く、オルグイユが地球に落下した後、地球物質によって深刻に汚染された可能性を示している。これらの結果は、リュウグウ試料が太陽系の固体物質としてCIコンドライトよりも代表的であることを示している。

論文

Holocene paleolimnological changes in Rundv${aa}$shetta lakes in the Soya Coast region and their paleoenvironmental significance with glacial isostatic adjustment in East Antarctica

井上 源喜*; 本田 英介*; 伊東 敬祐*; Kang, I.*; 瀬戸 浩二*; 谷 幸則*; 渡邊 隆広; 鹿島 薫*; 大谷 修司*; 山中 寿朗*; et al.

Quaternary Science Reviews, 338, p.108822_1 - 108822_18, 2024/08

https://doi.org/10.1016/j.quascirev.2024.108822
 被引用回数：0 パーセンタイル：0.00(Geography, Physical)

本研究では、南極宗谷海岸のルンドボークスヘッタ湖沼(丸湾南池,丸湾大池)の湖底堆積物の地質学的解析、有機成分分析、藻類等の顕微鏡観察及び放射性炭素年代測定を行い、完新世における本地域の環境変動と古陸水学的変遷を推測した。

論文

Neutron capture cross-section measurements at TC-Pn in KUR for nuclides of concern in decommissioning

中村 詔司; 遠藤 駿典; Rovira Leveroni, G.; 木村 敦; 芝原 雄司*

KURNS Progress Report 2023, P. 46, 2024/07

本研究は、生成放射能を評価するために、廃止措置で問題となる核種について熱中性子捕獲断面積を測定するものである。本件では、対象核種の中から$$^{58}$$Fe、$$^{170}$$Erおよび$$^{180}$$Hfを選定し、京大原子炉にて放射化法によりそれらの熱中性子捕獲断面積を測定した。今回、$$^{58}$$Fe(n,$$gamma$$)$$^{59}$$Fe反応について1.23$$pm$$0.03 barn、$$^{170}$$Er(n,$$gamma$$)$$^{171}$$Er反応について8.19$$pm$$0.35 barnを、そして$$^{180}$$Hf(n,$$gamma$$)$$^{181}$$Hf反応について13.57$$pm$$0.14 barnを得た。また、Hf試料の測定において副産物として、$$^{179}$$Hf(n,$$gamma$$)$$^{180m}$$Hf反応について0.427$$pm$$0.006 barnを得た。評価済みデータライブラリに採用されているデータは、今回得られた結果の不確かさ以上に違うことを明らかにした。

論文

Neutron capture cross section measurement of $$^{129}$$I and $$^{127}$$I using the NaI(Tl) spectrometer of the ANNRI beamline at J-PARC

Rovira Leveroni, G.; 木村 敦; 中村 詔司; 遠藤 駿典; 岩本 修; 岩本 信之; 藤 暢輔; 瀬川 麻里子; 前田 亮; 片渕 竜也*

European Physical Journal A, 60(5), p.120_1 - 120_14, 2024/05

https://doi.org/10.1140/epja/s10050-024-01333-3
 被引用回数：0 パーセンタイル：0.00(Physics, Nuclear)

The neutron capture cross section of $$^{129}$$I and $$^{127}$$I were measured from the thermal to the keV energy region with the NaI(Tl) spectrometer of the Accurate Neutron-Nucleus Reaction Measurement Instrument beamline in the Materials and Life Science Experimental Facility of the Japan Proton Accelerator Research Complex. The neutron capture yield was determined by means of the total energy detection principle with the pulse-height weighting technique. The present cross section results for $$^{127}$$I were normalized using the saturated resonance method with a thick-enough $$^{197}$$Au and provide good agreement with JENDL-5 from thermal to about 500 keV. A resonance analysis with the REFIT code was performed and the resonance parameters for $$^{127}$$I below 310 eV are presented in this work. In the case of $$^{129}$$I, the three largest resonances of $$^{127}$$I were employed for the cross section normalization. The present results for $$^{129}$$I are the first experimental data for the neutron region between thermal and 20 eV. The present data display a different energy dependence than that in the JENDL-5 and JEFF-3.3 and much similar to that in ENDF/B-VIII.0. Notwithstanding, good agreement was found at the thermal region between the present measurement of 31.6 $$pm$$ 1.3 b and both evaluated and most experimental data.

論文

A Science-based mixed oxide property model for developing advanced oxide nuclear fuels

加藤 正人; 沖 拓海; 渡部 雅; 廣岡 瞬; Vauchy, R.; 小澤 隆之; 上羽 智之; 生澤 佳久; 中村 博樹; 町田 昌彦

Journal of the American Ceramic Society, 107(5), p.2998 - 3011, 2024/05

https://doi.org/10.1111/jace.19609
 被引用回数：3 パーセンタイル：23.89(Materials Science, Ceramics)

Herein, a science-based uranium and plutonium mixed oxide (MOX) property model (Sci-M Pro) is derived for determining properties of MOX fuel and analyzing their performance as functions of Pu content, minor-actinide content, oxygen-to-metal ratio, and temperature. The property model is constructed by evaluating the effect of phonons and electronic defects on heat capacity and thermal conductivity of MOX fuels. The effect of phonons was evaluated based on experimental datasets related to lattice parameter, thermal expansion, and sound speeds. Moreover, the effect of electronic defects was determined by analyzing oxygen-potential data based on defect chemistry. Furthermore, the model evaluated the effect of the Bredig transition on the thermal properties of MOX fuel by analyzing the irradiation test results. The derived property model is applied to the performance code to analyze fast reactor fuel pins.

論文

Total and double differential scattering cross-section measurements of isotropic graphite

木村 敦; 遠藤 駿典; 中村 詔司

EPJ Web of Conferences, 294, p.01002_1 - 01002_7, 2024/04

https://doi.org/10.1051/epjconf/202429401002

The total and double differential scattering cross sections (DDSCS) of graphite have been measured in the Materials and Life Science Experimental Facility (MLF) in the J-PARC. The DDSCS were measured using the Beam Line No.14 (AMATERAS) in the MLF. The data were normalized using those of vanadium as a standard. Small angle scattering and Bragg edges were observed, and their intensities varied among the samples. The neutron total cross sections in the energy region from 1 to 100 meV were measured using Beam Line No.04 (ANNRI) in the MLF. In the epithermal range (over 40 meV), all samples tended to have values close to the free atom cross-section of graphite. However, at the first Bragg edge, the deduced total cross sections by those samples started to separate from each other. The difference became more significant with decreasing the neutron energy, and the value tended to increase with the grain size of the sample. The results of these measurements suggest that the discrepancies between the derived total cross sections in the low-energy region are due to small-angle scattering caused by grains of graphite with uniform size.

論文

$$^{241}$$Am neutron capture cross section measurement using the NaI(Tl) spectrometer of the ANNRI beamline of J-PARC

Rovira Leveroni, G.; 木村 敦; 中村 詔司; 遠藤 駿典; 岩本 修; 岩本 信之; 片渕 竜也*; 児玉 有*; 中野 秀仁*; 佐藤 八起*

Journal of Nuclear Science and Technology, 61(4), p.459 - 477, 2024/04

https://doi.org/10.1080/00223131.2023.2239885
 被引用回数：1 パーセンタイル：27.70(Nuclear Science & Technology)

The neutron capture cross-section of $$^{241}$$Am was measured from 10 meV to about 1 MeV using the NaI(Tl) spectrometer of the Accurate Neutron-Nucleus Reaction Measurement Instrument (ANNRI) beamline in the Materials and Life Science (MLF) facility of the Japan Proton Accelerator Research Complex (J-PARC). The total energy detection principle was applied in conjunction with the pulse-height weighting technique to derive the neutron capture yield. The present cross-section results were normalized using a $$^{197}$$Au sample measurement by applying the saturated resonance method. The thermal cross section was measured to be 708 $$pm$$ 22 b, in agreement within uncertainties to the present evaluation in JENDL-5 of 709 b. Moreover, the results of a shape resonance analysis of the resolved resonance region are also provided in the present dissertation.

論文

Measurements of the neutron total and capture cross sections and derivation of the resonance parameters of $$^{181}$$Ta

遠藤 駿典; 木村 敦; 中村 詔司; 岩本 修; 岩本 信之; Rovira Leveroni, G.; 藤 暢輔; 瀬川 麻里子; 前田 亮

Nuclear Science and Engineering, 198(4), p.786 - 803, 2024/04

https://doi.org/10.1080/00295639.2023.2227826
 被引用回数：1 パーセンタイル：27.70(Nuclear Science & Technology)

The neutron transmission ratio and capture yield for $$^{181}$$Ta were measured in J-PARC MLF ANNRI to improve the accuracy of resonance parameters. The total cross section was determined from the transmission ratio in the energy range from 0.2 to 150 eV. The capture cross section was obtained from the capture yield using the pulse height weighting technique (PHWT) in the energy range from thermal to 150 eV. The obtained transmission ratio and capture cross-section were fitted by the resonance analysis code, REFIT, and the resonance parameters were determined below 150 eV. It was also discussed the correlations caused by fitting based on statistical uncertainty and correlations for systematic uncertainty based on sample thickness in the transmission measurements.

論文

Neutron capture cross section measurement of $$^{129}$$I and $$^{127}$$I using ANNRI at MLF/J-PARC

Rovira Leveroni, G.; 木村 敦; 中村 詔司; 遠藤 駿典; 岩本 修; 岩本 信之; 藤 暢輔; 瀬川 麻里子; 前田 亮; 片渕 竜也*

JAEA-Conf 2023-001, p.74 - 79, 2024/02

https://doi.org/10.11484/jaea-conf-2023-001

Measurements to measure the neutron capture cross section of $$^{129}$$I and $$^{127}$$I were performed in the Accurate Neutron Nucleus Reaction Measurement Instrument (ANNRI) at the Materials and Life Science Facility (MLF) of the Japan Proton Accelerator Research Complex (J-PARC). The time-of-flight (TOF) methodology was employed to determine the neutron capture cross section from thermal to about 100 keV. The results from $$^{127}$$I were used to normalize the $$^{129}$$I cross section. Preliminary results of a resonance analysis below 100 eV for $$^{129}$$I are also presented.

論文

Tuning of spin-orbit coupling in chiral molecule-incorporated two-dimensional organic-inorganic hybrid perovskite copper halides with ferromagnetic exchange interactions

谷口 耕治*; Huang, P.-J.*; 佐賀山 基*; 鬼柳 亮嗣; 大石 一城*; 鬼頭 俊介*; 中村 唯我*; 宮坂 等*

Physical Review Materials (Internet), 8(2), p.024409_1 - 024409_10, 2024/02

https://doi.org/10.1103/PhysRevMaterials.8.024409
 被引用回数：2 パーセンタイル：62.00(Materials Science, Multidisciplinary)

Leveraging the flexible material designability of organic-inorganic hybrid systems, spatial inversion symmetry breaking and spin-orbit coupling (SOC) were simultaneously controlled in a series of two-dimensional organic-inorganic hybrid perovskite (2D-OIHP) copper halides with ferromagnetic exchange interaction (FMI). In chiral molecule-incorporated 2D-OIHP copper halides, an increase in Br component over Cl component at halogen sites leads to systematic variations in magnetic phase diagrams owing to the competition between the FMI and Dzyaloshinskii-Moriya interaction induced by the SOC. The crucial role of noncentrosymmetry in the competition for the magnetic interactions was confirmed by comparing the magnetic phase diagrams of chiral and achiral 2D-OIHP copper bromides.

論文

Uranium-plutonium-americium cation interdiffusion in polycrystalline (U,Pu,Am)O$$_{2 pm x}$$ mixed oxides

Vauchy, R.; 松本 卓; 廣岡 瞬; 宇野 弘樹*; 田村 哲也*; 有馬 立身*; 稲垣 八穂広*; 出光 一哉*; 中村 博樹; 町田 昌彦; et al.

Journal of Nuclear Materials, 588, p.154786_1 - 154786_13, 2024/01

https://doi.org/10.1016/j.jnucmat.2023.154786
 被引用回数：6 パーセンタイル：87.16(Materials Science, Multidisciplinary)

Diffusion couples made of dense polycrystalline (U,Pu,Am)O$$_{2 pm x}$$ oxides were annealed in various thermodynamic conditions (temperature, oxygen partial pressure), and for different durations. The associated actinide redistribution was quantified using Electron Probe Micro-Analysis (EPMA). Average diffusion profiles were obtained from elemental U, Pu, and Am X-ray maps and the resulting interdiffusion coefficients were calculated, then analyzed at the light of our model of point defect chemistry.

論文

Measurements of neutron total and capture cross sections of $$^{139}$$La and evaluation of resonance parameters

遠藤 駿典; 河村 しほり*; 奥平 琢也*; 吉川 大幹*; Rovira Leveroni, G.; 木村 敦; 中村 詔司; 岩本 修; 岩本 信之

European Physical Journal A, 59(12), p.288_1 - 288_12, 2023/12

https://doi.org/10.1140/epja/s10050-023-01203-4
 被引用回数：2 パーセンタイル：28.72(Physics, Nuclear)

ランタン(La)-139の断面積と共鳴パラメータは、原子力分野への応用や基礎核物理の研究にとって重要である。本論文では、大強度陽子加速器施設(J-PARC)のANNRIにてLaの中性子全断面積と捕獲断面積を測定した。Negative共鳴を含む4つの共鳴の共鳴パラメータを、共鳴解析コードREFITを用いて求めた。その結果いくつかの共鳴パラメータにおいて、評価済み核データライブラリとの不一致が見られた。さらに全断面積を再現するために、スピン依存する散乱半径もフィットした。得られた散乱半径は、評価済み核データライブラリで記録されたものよりも大きいことがわかった。

論文

Measurements of capture cross-section of $$^{93}$$Nb by activation method and half-life of $$^{94}$$Nb by mass analysis

中村 詔司; 芝原 雄司*; 遠藤 駿典; 木村 敦

Journal of Nuclear Science and Technology, 60(11), p.1361 - 1371, 2023/11

https://doi.org/10.1080/00223131.2023.2198526
 被引用回数：3 パーセンタイル：65.16(Nuclear Science & Technology)

廃止措置の対象核種の中から$$^{93}$$Nbについて、熱中性子捕獲断面積($$sigma$$$$_{0}$$)および共鳴積分(I$$_{0}$$)を放射化法により測定した。また、$$^{94}$$Nbの半減期を質量分析により測定した。ニオブ93試料は、京都大学複合原子力科学研究所の研究炉に整備されている水圧輸送艦を用いて照射した。金-アルミ合金線、およびコバルト-アルミ合金線を用いて、照射位置における中性子束成分を測定した。厚さ25$$mu$$mのガドリニウム箔を用いた照射も行って、熱および熱外中性子による反応率の寄与をより分けた。ガドリニウムの厚さから、カットオフ・エネルギーは0.133eVに設定した。ニオブ試料中に含まれている不純物により生成される$$^{182}$$Taの放射能を減衰させるために、約2年間ニオブ試料を冷却した。$$gamma$$線スペクトロスコピーにより照射されたニオブ試料およびモニタの生成放射能を測定した。Westcottコンベンションに基づいて解析を行い、$$sigma$$$$_{0}$$およびI$$_{0}$$を、それぞれ1.11$$pm$$0.04barnおよび10.5$$pm$$0.6barnと導出することができた。$$gamma$$線測定の後に、ニオブ試料の質量分析を行い、反応率を導出した。$$gamma$$線スペクトロスコピーと質量分析で得られたデータを組み合わせることにより、$$^{94}$$Nbの半減期を、(2.00$$pm$$0.15)$$times$$10$$^{4}$$年と導出することができた。

論文

Pd nanoparticles on the outer surface of microporous aluminosilicates for the direct alkylation of benzenes using alkanes

美崎 慧*; 三輪 寛子*; 伊藤 孝; 吉田 健文*; 長谷川 慎吾*; 中村 由紀奈*; 徳竹 駿太*; 高畠 萌*; 下村 浩一郎*; Chun, W.-J.*; et al.

ACS Catalysis, 13(18), p.12281 - 12287, 2023/09

https://doi.org/10.1021/acscatal.3c02309
 被引用回数：6 パーセンタイル：50.66(Chemistry, Physical)

The direct alkylation of benzenes with simple alkanes is one of the ideal processes for the production of alkylbenzenes. We demonstrated that Pd nanoparticles on the outer surface of H-ZSM-5 are efficient catalysts for direct alkylation. The reaction proceeds through the activation of an alkane on the acid sites present inside the zeolite pores. This process is followed by the nucleophilic addition of an arene to the activated alkane. The spillover of the abstracted hydrogen atoms from the acid sites to the Pd nanoparticles on the outer surface accelerates recombination to H$$_2$$. A maximum toluene conversion of 58.5% and selectivity of 95.6% for the alkylated products are achieved when toluene is reacted with $$n$$-heptane. ${it Para}$-selective alkylation is achieved, due to the effect of the pore size of H-ZSM-5. The $$mu^+$$SR study of muonium, a pseudo-isotope of hydrogen, in aluminosilicates suggested that the formation of atomic hydrogen is possible and its lifetime is in the sub-microsecond range or longer, which is long enough for chemical reactions.

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