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

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. A maximum toluene conversion of 58.5% and selectivity of 95.6% for the alkylated products are achieved when toluene is reacted with -heptane. -selective alkylation is achieved, due to the effect of the pore size of H-ZSM-5. The 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.

First observation of O

近藤 洋介*; Achouri, N. L.*; Al Falou, H.*; Atar, L.*; Aumann, T.*; 馬場 秀忠*; Boretzky, K.*; Caesar, C.*; Calvet, D.*; Chae, H.*; et al.

Nature, 620(7976), p.965 - 970, 2023/08

https://doi.org/10.1038/s41586-023-06352-6

非常に中性子が過剰な原子核Oは、陽子、中性子ともに魔法数であることから古くからその性質に興味が持たれていたが、酸素の最後の束縛核Oよりも中性子が4個も多いため、これまで観測されてこなかった。この論文では、理化学研究所RIBFにてFからの1陽子ノックアウト反応によってOを生成し、そこから放出される中性子を測定することによって初めてその観測に成功した。核構造の観点からは、Oでは二重閉殻が保たれているか興味が持たれていたが、実験で得られた分光学的因子が殻模型計算で予言されて程度の大きいことから、閉殻構造をもたない可能性が高いことがわかった。

Intruder configurations in Ne at the transition into the island of inversion; Detailed structure study of Ne

Wang, H.*; 安田 昌弘*; 近藤 洋介*; 中村 隆司*; Tostevin, J. A.*; 緒方 一介*; 大塚 孝治*; Poves, A.*; 清水 則孝*; 吉田 数貴; et al.

Physics Letters B, 843, p.138038_1 - 138038_9, 2023/08

https://doi.org/10.1016/j.physletb.2023.138038

Neからの1中性子除去反応を用いて、Neの詳細な線分光を行った。平行運動量分布の解析に基づき、Neの準位構造とスピンパリティを決定し、初めて負のパリティ状態を同定した。測定された断面積と運動量分布から、N=20とN=28のシェルギャップの消失の証拠となる有意なintruder p-wave強度が明らかになった。束縛状態については、弱いf-waveの可能性のある強度が観測された。いくつかの有効相互作用を用いた大規模殻模型計算では、実験的に観測された大きなp-wave強度と小さなf-wave強度は再現されず、Ne同位体に沿った反転の島への遷移の完全な理論的記述への挑戦が続いていることを示している。

Japanese Evaluated Nuclear Data Library version 5; JENDL-5

岩本 修; 岩本 信之; 国枝 賢; 湊 太志; 中山 梓介; 安部 豊*; 椿原 康介*; 奥村 森*; 石塚 知香子*; 吉田 正*; et al.

Journal of Nuclear Science and Technology, 60(1), p.1 - 60, 2023/01

https://doi.org/10.1080/00223131.2022.2141903

The fifth version of Japanese Evaluated Nuclear Data Library, JENDL-5, was developed. JENDL-5 aimed to meet a variety of needs not only from nuclear reactors but also from other applications such as accelerators. Most of the JENDL special purpose files published so far were integrated into JENDL-5 with revisions. JENDL-5 consists of 11 sublibraries: (1) Neutron, (2) Thermal scattering law, (3) Fission product yield, (4) Decay data, (5) Proton, (6) Deuteron, (7) Alpha-particle, (8) Photonuclear, (9) Photo-atomic, (10) Electro-atomic, and (11) Atomic relaxation. The neutron reaction data for a large number of nuclei in JENDL-4.0 were updated ranging from light to heavy ones, including major and minor actinides which affect nuclear reactor calculations. In addition, the number of nuclei of neutron reaction data stored in JENDL-5 was largely increased; the neutron data covered not only all of naturally existing nuclei but also their neighbor ones with half-lives longer than 1 day. JENDL-5 included the originally evaluated data of thermal scattering law and fission product yield for the first time. Light charged-particle and photon induced reaction data were also included for the first time as the JENDL general purpose file.

Extended neutron orbital and the shell closure in Ca

Enciu, M.*; Liu, H. N.*; Obertelli, A.*; Doornenbal, P.*; Nowacki, F.*; 緒方 一介*; Poves, A.*; 吉田 数貴; Achouri, N. L.*; 馬場 秀忠*; et al.

Physical Review Letters, 129(26), p.262501_1 - 262501_7, 2022/12

https://doi.org/10.1103/PhysRevLett.129.262501

230MeV/nucleonでのCaからの中性子ノックアウト反応が線分光と行われ、と軌道からの中性子ノックアウト反応の運動量分布が測定された。断面積はの閉殻と整合し、Ca同位体でのと閉殻と同程度に強い閉殻であることが確認された。運動量分布の分析からと軌道の平均二乗根半径の差は0.61(23)fmと決定され、これはmodified-shell-modelによる予言の0.7fmと整合した。これは、中性子過剰なCa同位体での軌道半径が大きいことが、中性子数にしたがって線形的に荷電半径が増える意外な現象の原因であることを示唆している。

Precise magnetization measurements down to 500 mK using a miniature He cryostat and a closed-cycle He gas handling system installed in a SQUID magnetometer without continuous-cooling functionality

島村 一利*; 輪島 裕樹*; 牧野 隼士*; 阿部 聡*; 芳賀 芳範; 佐藤 由昌*; 河江 達也*; 吉田 靖雄*

Japanese Journal of Applied Physics, 61(5), p.056502_1 - 056502_7, 2022/05

https://doi.org/10.35848/1347-4065/ac5bb0

We have conducted precise magnetization measurements down to 500 mK using a commercial magnetometer. The gas handling system contains two sorption pumps filled with granular charcoals. He gas is pressurized up to ambient pressure for liquification at 3 K and the vapor is pumped for cooling. We demonstrate the performance of the system by observing the Meissner effect of aluminum below the superconducting transition temperature.

Single-crystal structure analysis of non-deuterated triglycine sulfate by neutron diffraction at 20 and 298 K; A New disorder model for the 298 K structure

寺澤 有果菜*; 大原 高志; 佐藤 宗太*; 吉田 知史*; 朝日 透*

Acta Crystallographica Section E; Crystallographic Communications (Internet), 78(3), p.306 - 312, 2022/03

https://doi.org/10.1107/S2056989022000858

Precise single-crystal structure analyses of the title compound, nondeuterated triglycine sulfate (HTGS) at 20 K and 298 K were undertaken using time-of-flight neutron diffraction data. At 20 K for the O-H...O hydrogen bond between the glycinium cation and the zwitterionic, unprotonated glycine molecule that is associated with the ferroelectric behaviour of HTGS. Two reasonable structures for the same three atoms were refined for the 298 K dataset. One is a single-minimum potential-energy model, having the H atom with a large ellipticity along the bond path between the O atoms. The other is a double-minimum potential-energy model having two H atom sites with occupancies of 0.876 and 0.124.

Pairing forces govern population of doubly magic Ca from direct reactions

Browne, F.*; Chen, S.*; Doornenbal, P.*; Obertelli, A.*; 緒方 一介*; 宇都野 穣; 吉田 数貴; Achouri, N. L.*; 馬場 秀忠*; Calvet, D.*; et al.

Physical Review Letters, 126(25), p.252501_1 - 252501_7, 2021/06

https://doi.org/10.1103/PhysRevLett.126.252501

理化学研究所RIビームファクトリーにて、中性子過剰核Scからの1陽子ノックアウト反応によってCaを生成し、そのエネルギー準位と反応断面積をガンマ線分光および不変質量分光によって得た。その結果を歪曲波インパルス近似による核反応計算と大規模殻模型による核構造計算を組み合わせた理論値と比較した。実験の準位と断面積は理論計算によってよく再現された。Caの正パリティ状態については、基底状態の生成断面積が励起状態のものに比べて圧倒的に大きいという結果が得られた。これは、Scでは中性子魔法数34が消滅しCaではその魔法数が存在するというこれまでの知見と一見矛盾するが、対相関による分光学的因子のコヒーレンスから理解することができる。

First spectroscopic study of Ar by the (,2) reaction

Juhsz, M. M.*; Elekes, Z.*; Sohler, D.*; 宇都野 穣; 吉田 数貴; 大塚 孝治*; 緒方 一介*; Doornenbal, P.*; Obertelli, A.*; 馬場 秀忠*; et al.

Physics Letters B, 814, p.136108_1 - 136108_8, 2021/03

AA2020-0747.pdf:0.83MB

https://doi.org/10.1016/j.physletb.2021.136108

(,)反応と線分光を用いてArの束縛状態と非束縛状態の核構造研究を行った。実験結果と殻模型計算を比較することで、2つの束縛状態と6つの非束縛状態を決定した。Arの束縛状態を生成する反応断面積が小さいことから、これは中性子数32, 34の顕著なsub-shell closureが存在している確かな証拠と解釈できる。

Evaluation of fission product yields and associated covariance matrices

椿原 康介*; 奥村 森*; 石塚 知香子*; 吉田 正*; 湊 太志; 千葉 敏*

Journal of Nuclear Science and Technology, 58(2), p.151 - 165, 2021/02

AA2020-0468.pdf:2.37MB

https://doi.org/10.1080/00223131.2020.1813643

The independent and cumulative fission product yields (FPYs) and their covariance matrices were newly evaluated for thermal- and fast-neutron induced fission and spontaneous fission. We principally evaluated the independent isobaric charge distributions by taking account of available experimental data, especially putting emphasis on the shell and even-odd staggering in the fission yields by applying a Boltzmann factor including the shell and the pairing correction energies for the mass of fission products. Furthermore, the isomeric ratios of FPY were obtained by a systematic calculation based on the Hauser-Feshbach theory. Normalization of the FPY and associated covariance matrices of independent FPY were determined based on the generalised least-square method to make them consistent with important physical constraints. Especially, the FPYs were normalized to be consistent with the mass chain yield of England and Rider. The cumulative FPYs were calculated by following the relevant -decay chain by using the decay data from JENDL/DDF-2015. Finally, we verified the FPYs evaluated presently by considering experimental decay heats, delayed neutron yields, aggregate antineutrino spectra and results from post-irradiation examination. All the results have shown that the present set of FPYs were consistent with these data, and free from trivial problems present in JENDL/FPY-2011.