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論文

Organization of malonamides from the interface to the organic bulk phase

Micheau, C.; 上田 祐生; 元川 竜平; 阿久津 和宏*; 山田 悟史*; 山田 雅子*; Moussaoui, S. A.*; Makombe, E.*; Meyer, D.*; Berthon, L.*; et al.

Journal of Molecular Liquids, 401, p.124372_1 - 124372_12, 2024/05

https://doi.org/10.1016/j.molliq.2024.124372

Supramolecular organization of extractant molecules impacts metal ions separation behavior. Probing bulk and interfacial structures of the relevant systems is expected to provide key insights into the metal ion selectivity and kinetic aspects. The supramolecular features of two solvent extraction systems based on malonamide extractants, N,N,N′,N′-tetrahexylmalonamide (THMA) in toluene and N,N′-dimethyl-N,N′-dibutyl-2-tetradecylmalonamide (DBMA) in n-heptane, were studied using small-angle X-ray scattering for the organic bulk phases, as well as interfacial tension and neutron reflectivity measurements for the interfaces. In the bulk solution, THMA forms dimeric/trimeric associates but no aggregates in toluene, while DBMA forms large aggregates in n-heptane. On the other hand, THMA accumulates in a diffuse layer at the interface at high THMA concentration, whereas DBMA forms a compact but thinner layer. After Pd(II) extraction, the thickness of interfacial layers decreases in the case of THMA, and totally vanishes in the case of DBMA. Based on these new structural information, two mechanisms are proposed for Pd(II) and Nd(III) extraction with malonamides. In toluene, THMA associates slightly accumulate in the vicinity of the interface, then coordinate Pd(II) and diffuse into the organic bulk phase. In n-heptane, DBMA aggregates adsorb at the interface then pick up Nd(III) cations in their polar cores and finally diffuse into the bulk.

論文

Arsenic removal from contaminated water utilizing novel green composite ${it Chlorella vulgaris}$ and nano zero-valent iron

Islam, M. S.*; Maamoun, I.; Falyouna, O.*; Eljamal, O.*; Saha, B. B.*

Journal of Molecular Liquids, 370, p.121005_1 - 121005_11, 2023/01

https://doi.org/10.1016/j.molliq.2022.121005
 被引用回数：11 パーセンタイル：88.04(Chemistry, Physical)

Arsenic waste must be carefully managed because of the adverse effects of arsenic in wastewater on the ecosystem. In the present study, an environmentally friendly novel composite of ${it Chlorella vulgaris}$ microalgae and nano-zero valent iron (NZVI) was employed as an adsorbent to eliminate arsenic from the aqueous environment. Fourier Transform Infrared spectroscopy, X-ray diffraction, and scanning electron microscope images were used to characterize and analyze the CV/NZVI composites. Batch tests using initial arsenic concentrations ranging from 5 to 100 mg/L were conducted to evaluate removal efficiencies. According to kinetic analysis, the best model for fitting the experimental data was the pseudo first-order model, which had the lowest Akaike information criterion (AIC), and Bayesian information criterion (BIC) values of -23.878 and -7.902, respectively. Results alluded that physisorption is the primary mechanism influenced by As-removal by CV/NZVI composite. Due to the negative sign of the enthalpy and Gibbs free energy, the thermodynamic investigation revealed that the adsorption reaction was exothermic and spontaneous. The thermodynamic analysis also affirmed that the arsenic removal process involved primarily physisorption and slight chemisorption phenomena. Meanwhile, 1.5 g/L CV/NZVI dosage achieved 99% As(V) removal efficiency in synthetic groundwater systems, confirming the high potential of the composite in complex aqueous systems.

論文

Sustainable technologies for the removal of Chloramphenicol from pharmaceutical industries Effluent; A Critical review

Falyouna, O.*; Maamoun, I.; Ghosh, S.*; Malloum, A.*; Othmani, A.*; Eljamal, O.*; Amen, T. W. M.*; Oroke, A.*; Bornman, C.*; Ahmadi, S.*; et al.

Journal of Molecular Liquids, 368, Part B, p.120726_1 - 120726_25, 2022/12

https://doi.org/10.1016/j.molliq.2022.120726
 被引用回数：5 パーセンタイル：38.46(Chemistry, Physical)

Despite the carcinogenic and other adverse health effects ofchloramphenicol (CAP), it is frequently detected in different water sources (e.g., groundwater, surface water, wastewater effluents, etc.) due to ongoing, illegal, and abusive application of CAP in veterinary medicine. Although extensive research has been carried out to develop effective treatment technologies to remove the persistent CAP from aqueous mediums, yet there is no critical review of these studies to the best of our reach This review will be the first in the literature to comprehensively summarize the state-of-the-art treatment techniques for CAP removal from water. We report the removal of CAP by adsorption, biodegradation, nanoscale zerovalent iron technology (nZVI), and advanced oxidation processes (AOPs). The result shows that carbon-based adsorbents have more q$$_{rm max}$$ equal 892.86 mg/g for Porous carbon material from $$Enteromorpha prolifera$$. The Langmuir- Freundlich isotherm and pseudo-second order kinetics model were reported to best describe the isotherm and kinetic model respectively. Removing the CAP via biodegradation would achieve the advantages of low operating costs, and environmental friendliness. The process of AOPs among the various treatment options can be a promising method for CAP degradation in water. This review comprehensively summarizes the state-of-the-art treatment techniques for CAP removal from water. Particularly, serving as an inclusive reference for future researchers to easily define the research gabs in the literature and plan for their future work in developing novel treatment methods to decontaminate CA-contaminated waters.

論文

Neutron scattering on an aqueous sodium chloride solution in the gigapascal pressure range

山口 敏男*; 吉田 亨次*; 町田 真一*; 服部 高典

Journal of Molecular Liquids, 365, p.120181_1 - 120181_10, 2022/11

https://doi.org/10.1016/j.molliq.2022.120181
 被引用回数：1 パーセンタイル：16.81(Chemistry, Physical)

3mol/kg NaCl重水溶液を0.1MPa/298K, 1GPa/298K, 1GPa/523K, 4GPa/523Kの温度圧力条件において中性子散乱測定した。また、得られたデータにEmpirical potential structure refinement法を適用し、対相関関数,配位数分布,角度分布(配向相関),空間密度関数(3次元構造)を抽出した。それらの結果から、イオンの溶媒和と会合、溶媒水構造の圧力と温度依存性を議論した。

論文

The Translational, rotational, and phonon dynamics of water in ZrO$$_{2}$$/water nanofluid

吉田 亨次*; 真田 雄介*; 山口 敏男*; 松浦 直人*; 玉造 博夢; 内山 裕士*

Journal of Molecular Liquids, 366, p.120218_1 - 120218_9, 2022/11

https://doi.org/10.1016/j.molliq.2022.120218
 被引用回数：1 パーセンタイル：16.81(Chemistry, Physical)

The translational, rotational, and phonon dynamics of water in zirconium oxide (ZrO$$_{2}$$) nanofluid were investigated by quasi-elastic neutron scattering, $$^{17}$$O NMR relaxation, and inelastic X-ray scattering, respectively. The particle size of ZrO$$_{2}$$ is 3 $$sim$$ 100 nm, and the concentration of ZrO$$_{2}$$ nanoparticles is 5, 10, 20, and 30 wt%. The translational and rotational motions of water molecules become retarded with increasing the concentration of ZrO$$_{2}$$. This indicates that there is an attractive interaction between water molecules and the surface of the nanoparticles. The high-frequency sound velocity of the nanofluid obtained from phonon dynamics measurements is slightly larger than that of pure water although it is not much difference compared to the case of the translation and rotation. These findings indicate that water dynamics in the nanofluid is different from that of the bulk. It might be reasons for the enhancement of the thermal conductivity of the nanofluid.

論文

Promotion of ciprofloxacin adsorption from contaminated solutions by oxalate modified nanoscale zerovalent iron particles

Falyouna, O.*; Idham, M. F.*; Maamoun, I.; Bensaida, K.*; Ashik, U. P. M.*; 杉原 裕司*; Eljamal, O.*

Journal of Molecular Liquids, 359, p.119323_1 - 119323_20, 2022/08

https://doi.org/10.1016/j.molliq.2022.119323
 被引用回数：36 パーセンタイル：99.45(Chemistry, Physical)

Water contamination by ciprofloxacin (CIP) is a global and emerging issue because it increases the risk of infection by antimicrobial resistant bacteria. CIP removal from water by iron nanoparticles (Fe$$^{0}$$) with the presence of oxalate hasn't been reported yet. The present study demonstrated that the addition of oxalate to Fe$$^{0}$$ nanoparticles improved the removal of CIP under the following optimum conditions: dose = 0.3 g L$$^{-1}$$, oxalate = 0.3 mM, initial pH = 7, and temperature = 25 $$^{circ}$$C. Furthermore, the experimental results illustrated that high concentrations of dissolved oxygen in the aqueous solution greatly decreased the removal efficiency of CIP by Fe$$^{0}$$ oxalate system. In addition, the desorption experiments and the results of SEM-EDS, XRD, and FTIR revealed that physisorption and chemisorption were responsible for CIP removal by Fe$$^{0}$$ oxalate system as the addition of 0.3 mM of oxalate boosted the surface complexation between Fe$$^{0}$$ nanoparticles and the carboxylic, ketone, and piperazinyl groups in CIP. These results were supported by the outcomes of kinetics, isotherm, and thermodynamic analysis. Finally, this study proved that Fe$$^{0}$$ oxalate system is inexpensive, practical, and more efficient than most of the reported Fe$$^{0}$$-based systems with a maximum adsorption capacity of 294.66 mg g$$^{-1}$$.

論文

Rapid and efficient chromium (VI) removal from aqueous solutions using nickel hydroxide nanoplates (nNiHs)

Maamoun, I.; Bensaida, K.*; Eljamal, R.*; Falyouna, O.*; 田中 万也; Tosco, T.*; 杉原 裕司*; Eljamal, O.*

Journal of Molecular Liquids, 358, p.119216_1 - 119216_13, 2022/07

https://doi.org/10.1016/j.molliq.2022.119216
 被引用回数：26 パーセンタイル：98.36(Chemistry, Physical)

In this study, nickel hydroxide nanoplates (nNiHs) were developed to achieve rapid and significant Cr(VI) removal from aqueous solutions. nNiHs showed an average particle size and crystallite size of 36.8 nm and 8.68 nm, respectively. Different reaction parameters were investigated, including nNiHs dosage, pH, reaction temperature, initial Cr(VI) concentration, and co-existing anions. nNiHs could efficiently remove 20 mg/L Cr(VI) concentration over a wide pH and temperature range(s). Pseudo 2nd order kinetic model and Freundlich isotherm model were the best to fit experimental data. A maximum Cr(VI) sorption capacity of 71.25 mg/g was achieved at the optimal reaction conditions, comparable to the previously reported values. The governing Cr(VI) removal mechanism by nNiHs involved the high dominance of electrostatic adsorption and the low dominance of co-precipitation. The high sorption potential of the nNiHs and the high affinity of the aqueous Cr(VI) species, enabled the proposed adsorbent to yield an efficient performance in binary environmental systems.

論文

Structure of an aqueous RbCl solution in the gigapascal pressure range by neutron diffraction combined with empirical potential structure refinement modeling

Zhang, W. Q.*; 山口 敏男*; Fang, C. H.*; 吉田 亨次*; Zhou, Y. Q.*; Zhu, F. Y.*; 町田 真一*; 服部 高典; Li, W.*

Journal of Molecular Liquids, 348, p.118080_1 - 118080_11, 2022/02

https://doi.org/10.1016/j.molliq.2021.118080
 被引用回数：2 パーセンタイル：34.79(Chemistry, Physical)

3mol/kgのRbCl水溶液におけるイオンの水和・会合と水素結合した水の構造を、298K/0.1MPa, 298K/1GPa, 523K/1GPa, 523K/4GPaにおける中性子回折と経験的ポテンシャル構造精密化モデリングにより調べた。その結果、構造パラメータは温度と圧力に依存していることがわかった。高圧・高温条件では、Rb$$^+$$とCl$$^-$$の第二水和層がより明確になる。第一水和層におけるRb$$^+$$の平均酸素配位数は、配位距離を0.290nmから0.288nmに縮めながら、常圧では6.3だったのが、4GPaでは8.9に増加した。第一水和シェルのCl$$^-$$の平均酸素配位数は、常圧で5.9、4GPaで9.1と圧力により増加し、対応する配位距離は0.322nmから0.314nmへと減少した。Rb$$^+$$と中心の水分子の第一溶媒和シェルにおける水双極子の配向は圧力に敏感であるが、Cl$$^-$$の第一溶媒和シェルにおける水双極子の配向は温度圧力によらずあまり変化しなかった。Rb$$^+$$-Cl$$^-$$の隣接イオンペアの数は、温度が高くなると減少し、圧力が高くなると増加する。水分子は密に詰まっており、極限状態では水分子の四面体水素結合ネットワークはもはや存在しない。

論文

Spontaneous formations of nanoconfined water in ionic liquids by small-angle neutron scattering

阿部 洋*; 根本 文也*; 廣井 孝介; 大石 一城*; 高田 慎一

Journal of Molecular Liquids, 346, p.117035_1 - 117035_6, 2022/01

https://doi.org/10.1016/j.molliq.2021.117035
 被引用回数：4 パーセンタイル：61.27(Chemistry, Physical)

In this study, monodispersive nanoconfined water ("water pocket") is organized spontaneously in hydrophilic ionic liquid (IL). The IL is 1-alkyl-3-methylimidazolium nitrate ([C$$_{n}$$mim][NO$$_{3}$$] $$n$$ = 2, 6, and 8). By small-angle neutron scattering (SANS), D$$_{2}$$O aggregations in the IL are detected. There are no SANS peaks for [C$$_{2}$$mim][NO$$_{3}$$]-D$$_{2}$$O, but, in [C$$_{6}$$mim][NO$$_{3}$$]-$$x$$ mol% D$$_{2}$$O, a SANS peak can be observed at $$70 < x < 90$$ mol%. The peak intensity, position, and profile change according to water concentration and temperature. Pure [C$$_{8}$$mim][NO$$_{3}$$] has a distinct SANS peak, reflecting on the nanodomains at room temperature. Above 70 mol%, the SANS peak of [C$$_{8}$$mim][NO$$_{3}$$]-D$$_{2}$$O sharply increases and shifts to the low-Q position. The water pocket develops proportionate to water concentration, and its morphologies are visualized using an ${it ab initio}$ bead model. The alkyl chain length dependence of the water pocket is clarified by a three-dimensional reconstruction method.

論文

Experimental analysis on dynamics of liquid molecules adjacent to particles in nanofluids

橋本 俊輔*; 中島 健次; 菊地 龍弥*; 蒲沢 和也*; 柴田 薫; 山田 武*

Journal of Molecular Liquids, 342, p.117580_1 - 117580_8, 2021/11

https://doi.org/10.1016/j.molliq.2021.117580
 被引用回数：3 パーセンタイル：27(Chemistry, Physical)

エチレングリコール水溶液中に二酸化ケイ素(SiO$$_{2}$$)ナノ粒子を分散したナノ流体の準弾性中性子散乱測定(QENS)およびパルス磁場勾配核磁気共鳴分析(PFGNMR)を行った。研究目的は、このナノ流体の熱伝導率が理論値を超えて増加するメカニズムを解明することだった。得られた実験結果は、SiO$$_{2}$$ナノ粒子の周りの液体分子の運動が非常に制限されているため、SiO$$_{2}$$ナノ粒子の添加により、エチレングリコール水溶液中の液体分子の自己拡散係数が低下していることを示す。そして温度一定の条件で、SiO$$_{2}$$ナノ流体中で、液体分子の自己拡散係数が減少するにつれて、熱伝導率が増加した。

論文

The Effect of alkyl ammonium ionic liquids on thermal denaturation aggregation of $$beta$$-lactoglobulin

吉田 亨次*; 禪院 知寛*; Fujiyoshi, Ayako*; 真田 雄介*; 山口 敏男*; Murata, Kunihiko*; 高田 慎一; 廣井 孝介; 竹清 貴浩*; 吉村 幸浩*

Journal of Molecular Liquids, 293, p.111477_1 - 111477_9, 2019/11

https://doi.org/10.1016/j.molliq.2019.111477
 被引用回数：8 パーセンタイル：39.14(Chemistry, Physical)

Differential scanning calorimetry (DSC), small-angle X-ray scattering (SAXS), small-angle neutron scattering (SANS) measurements, and scanning and transmission electron microscope (SEM and TEM) of $$beta$$-lactoglobulin ($$beta$$-LG) are performed in alkyl (methyl, ethyl, and propyl) ammonium nitrate ionic liquids (RAN-ILs)-water mixtures at 25-100$$^{circ}$$C. The addition of these RANs decreased the thermal denaturation temperature of $$beta$$-LG, and the effect is larger with an increase of the hydrophobic part of the cation of the ILs. In ethyl ammonium nitrate (EAN) and propyl ammonium nitrate (PAN) mixtures, the fractal aggregate structure of $$beta$$-LG was found after the thermal denaturation occurred. These results are similar to those of alcohol-water mixtures. The nanoheterogeneous structure of the RAN-water mixture which consists of the hydrophobic and hydrophilic parts might affect the aggregation structure of $$beta$$-LG.

論文

Dynamic properties of nano-confined water in an ionic liquid

阿部 洋*; 山田 武*; 柴田 薫

Journal of Molecular Liquids, 264, p.54 - 57, 2018/08

https://doi.org/10.1016/j.molliq.2018.05.006
 被引用回数：14 パーセンタイル：60.51(Chemistry, Physical)

Nano-confined water (a water pocket) was spontaneously formed using an ionic liquid (IL), 1-butyl-3-methylimidazolium nitrate ([C$$_{4}$$mim][NO$$_{3}$$]), in [C$$_{4}$$mim][NO$$_{3}$$]-H$$_{2}$$O and [C$$_{4}$$mim][NO$$_{3}$$]-D$$_{2}$$O mixtures. The static average size of the water pocket in [C$$_{4}$$mim][NO$$_{3}$$]-80 mol% D$$_{2}$$O has been estimated to be around 20${AA}$, determined via small-angle neutron scattering measurements. In this study, the dynamics of the water pocket in the IL were directly examined using incoherent quasielastic neutron scattering. Using the H-D difference of a neutron incoherent scattering cross section, the extent of the diffusion of the water molecules in the water pocket was determined. The water pocket could be characterized due to the slow dynamics of the water compared with those of bulk water.

論文

Chemical state analysis of high-temperature molten slag components by using high-energy XAFS

岡本 芳浩; 大杉 武史; 赤堀 光雄; 小林 徹; 塩飽 秀啓

Journal of Molecular Liquids, 232, p.285 - 289, 2017/04

https://doi.org/10.1016/j.molliq.2017.02.072
 被引用回数：3 パーセンタイル：12.21(Chemistry, Physical)

高温溶融スラグ(SiO$$_{2}$$-CaO-Fe$$_{2}$$O$$_{3}$$-CeO$$_{2}$$)中のセリウムの化学状態について調べるために、セリウムK吸収端を使用した高エネルギーXAFS測定を実施した。EXAFS解析から得られたCe-O距離の変化から、セリウムの化学状態は、溶融状態では4価、固体状態では3価をとっていることが分かった。室温におけるデバイワーラー因子は非常に大きく、その値は高温溶融状態でもその変化量は大変小さかった。この結果は、セリウム元素が固体スラグ中で極めて構造秩序が低く、かつ安定な状態にあることを示唆している。

論文

Terahertz dynamics of water before and after water shedding from reverse micelles

村上 洋

Journal of Molecular Liquids, 210, Part A, p.37 - 43, 2015/10

https://doi.org/10.1016/j.molliq.2015.03.015
 被引用回数：10 パーセンタイル：38.6(Chemistry, Physical)

ナノメートルスケールの微小液滴を保持する逆ミセルは、水の構造・ダイナミクスに及ぼす空間拘束効果を調べるだけでなく、その微少液滴中に蛋白質などを可溶化することができるため、細胞類似環境下での生体高分子や水の状態を調べるために有用な系である。一方、THz分光によりピコ秒領域の水の集団的運動を調べることができる。本研究では、THz時間領域分光を用いた温度変化測定のために、溶媒と溶液試料を同時に温度制御できる装置を開発し測定を行った。液体水では、その拡散的運動に起因する10ps程度の時定数が水の融点付近まで温度減少と共に徐々に増加するのに対して、半径5nm程度の逆ミセル中の水では、285Kまで急激な増加を示す。これは、水の協同的運動が逆ミセルの空間拘束により阻害されることに起因する運動のスローダウンと考えられる。さらに、その温度以下で逆ミセルからの水流出が起こり、時定数の温度依存性が液体水と同様の振る舞いを示し、流出水は水の特性を回復することが明らかになった。

論文

High-energy EXAFS study of molten GdCl$$_3$$ systems

岡本 芳浩; 塩飽 秀啓; 矢板 毅; 鈴木 伸一; Gaune-Escard, M.*

Journal of Molecular Liquids, 187, p.94 - 98, 2013/11

https://doi.org/10.1016/j.molliq.2013.05.018
 被引用回数：14 パーセンタイル：47.65(Chemistry, Physical)

溶融塩化ガドリニウムとそのLiCl-KCl共晶塩との混合融体の局所構造を、GdのK吸収端を利用した高エネルギーEXAFS測定技術を使用して調べた。カーブフィッティング解析の結果、塩化ガドリニウム単独塩融体中では、最近接Gd$$^{3+}$$-Cl$$^-$$間距離は2.74$$pm$$0.02${AA}$で、その配位数は6.5$$pm$$0.3だった。一方、10%混合融体中では、2.70$$pm$$0.01${AA}$ and 6.1$$pm$$0.3へ減少することがわかった。これらの結果は、混合によって、八面体配位構造(GdCl$$_6$$)$$^{3-}$$が形成され安定化することを示唆した。解析の結果を、YCl$$_3$$及びLaCl$$_3$$混合系と比較検討した。

論文

Structure of water from ambient to 4 GPa revealed by energy-dispersive X-ray diffraction combined with empirical potential structure refinement modeling

山口 敏男*; 藤村 恒児*; 内 和哉*; 吉田 亨次*; 片山 芳則

Journal of Molecular Liquids, 176, p.44 - 51, 2012/12

https://doi.org/10.1016/j.molliq.2012.08.021
 被引用回数：18 パーセンタイル：55.59(Chemistry, Physical)

実験室のX線回折計を用いた水のエネルギー分散型X線回折測定を、298K/30MPa, 473K/30MPa and 573K/30MPaの熱力学条件下で行った。対分布関数,配位数,3次元空間密度関数の温度圧力変化から水素結合の特徴を明らかにするために、これらのX線構造因子と、過去にシンクロトロンX線を用いて298K/1GPa, 473K/0.35GPa and 486K/4GPaで測定されたものに対して、経験ポテンシャル構造精密化(EPSR)によるモデル化を適用した。圧力や温度によって、どの程度、水素結合ネットワークが影響を受けるか明らかになった。

論文

Femtosecond time-resolved fluorescence spectra of a coumarin dye in glycerol

村上 洋

Journal of Molecular Liquids, 89(1-3), p.33 - 45, 2000/12

https://doi.org/10.1016/S0167-7322(00)90003-5
 被引用回数：9 パーセンタイル：27.49(Chemistry, Physical)

ガラス形成物質の構造緩和についての情報を得るために、室温でグリセリン中クマリン色素のフェムト秒時間分解蛍光分光を1ナノ秒にわたって行った。モード同期チタンサファイアレーザーを光源とした和周波発生法を用いた。時間分解蛍光スペクトルは1ナノ秒まで長波長シフトを示した。スペクトルのピーク波長の時間発展の解析から色素分子の電子励起状態のエネルギー緩和は三つの成分を持つことがわかった。一つは振動緩和に、ほかの二つの成分はグリセリンのいわゆる速い$$beta$$過程及び$$alpha$$緩和に起因すると考えられる。

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