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Hierarchical aggregation in a complex fluid; The Role of isomeric interconversion

Massey, D.*; Williams, C. D.*; Mu, J.*; Masters, A. J.*; 元川 竜平; 青柳 登; 上田 祐生; Antonio, M. R.*

Journal of Physical Chemistry B, 127(9), p.2052 - 2065, 2023/03

There is an ever-increasing body of evidence that metallic complexes, involving amphiphilic ligands, do not form normal solutions in organic solvents. Instead, they form complex fluids with intricate structures. For example, the metallic complexes may aggregate into clusters and these clusters themselves may aggregate into super-clusters. In order to gain a deeper insight into the mechanisms at play, we have used an improved force field to conduct extensive molecular dynamics simulations of a system composed of zirconium nitrate, water, nitric acid, tri-$$n$$-butyl phosphate and $$n$$-octane. The important new finding is that a dynamic equilibrium between the cis and trans isomers of the metal complex is likely to play a key role in the aggregation behavior. The isolated cis and trans isomers have similar energies but simulation indicates that the clusters consist predominantly of cis isomers. With increasing metal concentration, we hypothesize that more clustering occurs and the chemical equilibrium shifts towards the cis isomer. It is possible that such isomeric effects play a role in the liquid-liquid extraction of other species and the inclusion of such effects in flowsheet modelling may lead to a better description of the process.


Synthesis of hybrid magnesium hydroxide/magnesium oxide nanorods [Mg(OH)$$_{2}$$/MgO] for prompt and efficient adsorption of ciprofloxacin from aqueous solutions

Falyouna, O.*; Bensaida, K.*; Maamoun, I.; Ashik, U. P. M.*; 田原 淳士*; 田中 万也; 青柳 登; 杉原 裕司*; Eljamal, O.*

Journal of Cleaner Production, 342, p.130949_1 - 130949_15, 2022/03

 被引用回数:7 パーセンタイル:95.42(Green & Sustainable Science & Technology)

The antibiotic ciprofloxacin is recognized as a contaminant of emerging concern because its persistent occurrence in water accelerates the growth of deadly antimicrobial resistance genes. For the first time, the conventional precipitation technique was thermally modified to produce hybrid magnesium hydroxide/magnesium oxide nanorods for efficient and rapid adsorption of CIP from water. The successful synthesis was confirmed by the outcomes of TEM, EDS, XRD, and FTIR analysis. Mg(OH)$$_{2}$$/MgO exhibited an extraordinary capability to adsorb CIP from water regardless of CIP initial concentration under neutral pH and room temperature. FTIR analysis for the spent Mg(OH)$$_{2}$$/MgO revealed that bridging complexation with carboxylic group and electrostatic attraction with the positive amine group are the responsible mechanisms for CIP adsorption by Mg(OH)$$_{2}$$/MgO. Moreover, simulated CIP-contaminated river water was efficiently treated by Mg (OH)$$_{2}$$/MgO which proves the promising performance of Mg(OH)$$_{2}$$/MgO in field scale applications.


Uranium (VI) sorption on illite under varying carbonate concentrations; Batch experiments, modeling, and cryogenic time-resolved laser fluorescence spectroscopy study

Mei, H.; 青柳 登; 斉藤 拓巳*; 香西 直文; 杉浦 佑樹; 舘 幸男

Applied Geochemistry, 136, p.105178_1 - 105178_8, 2022/01

 被引用回数:2 パーセンタイル:0.01(Geochemistry & Geophysics)

Dissolved inorganic carbonate ions (DIC) present in groundwaters may affect both the aqueous and surface species of U(VI) due to its strong complexation ability with U(VI). However, it is still not clear how DIC affects U(VI) sorption on illite, which is one of the critical components in argillaceous rocks. In this study, the sorption of U(VI) on conditioned illite du Puy in presence of varying DIC concentrations (up to 250 mM DIC) as a function of pH was investigated by combining batch sorption experiments, surface complexation modeling, and the cryogenic time-resolved laser fluorescence spectroscopy (TRLFS). The distribution coefficients of U(VI) were sensitive to the DIC concentration, which decreased with an increase of DIC. There is no sorption of U(VI) under relatively high DIC concentrations (100 mM DIC). The U(VI) sorption behavior on illite was modeled by using the 2 Site Protolysis Non-Electrostatic Surface Complexation and Cation Exchange model. Two ternary surface complexation reactions with carbonate were needed to depict the experimental sorption data in addition to binary and ternary hydroxo surface complexation reactions employed for the description of U sorption to illite without carbonate. The cryogenic TRLFS revealed that U(VI) did sorb to illite in presence of high DIC concentration (up to 10 mM DIC). The spectra were unchanged with DIC at pH 8.5, suggesting the surface speciation of U(VI) remained the same. The decay curves were biexponential, which further indicated that at least two species were responsible for the sorption. Our finding will help to predict the transport and retention behaviors of U(VI) near radioactive waste repositories.


A Fluorous phosphate for the effective extraction of Ln$$^{III}$$ from nitrate media; Comparison with a conventional organic phosphate

上田 祐生; 菊池 圭*; 徳永 紘平; 杉田 剛; 青柳 登; 田中 万也; 岡村 浩之

Solvent Extraction and Ion Exchange, 39(5-6), p.491 - 511, 2021/00

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



Spectroscopic studies of M$"o$ssbauer, infrared, and laser-induced luminescence for classifying rare-earth minerals enriched in iron-rich deposits

青柳 登; Nguyen, T. T.*; 熊谷 友多; Nguyen, T. V.*; 中田 正美; 瀬川 優佳里; Nguyen, H. T.*; Le, B. T.*

ACS Omega (Internet), 5(13), p.7096 - 7105, 2020/04

 被引用回数:2 パーセンタイル:15.09(Chemistry, Multidisciplinary)

Rare-earth phosphates often appear as an accessory phase in igneous or metamorphic rocks; however, these rocks are composed of myriad chemical elements and nuclides that interfere with the qualitative or quantitative analyses of the rare-earth phosphates over a range of concentrations in the absence of a pretreatment. In addition, the limit of each analytical methodology constrains the approach as well as the usefulness of the results in geoscience applications. Here, we report the specific mineral characterization of rare-earth (RE)-containing ores from Yen Phu mine, Vietnam, using a range of state-of-the-art spectroscopic techniques in conjunction with microscopy: M$"o$ssbauer spectroscopy, infrared microspectroscopy, time-resolved laser-induced fluorescence spectroscopy (TRLFS), and scanning electron microscopy with energy-dispersive X-ray spectroscopy. Because the distribution of each element in the deposit differs, such combinatorial works are necessary and could lead to more plausible answers to questions surrounding the point of origin of rare-earth elements. The results of our M$"o$ssbauer spectroscopic analysis indicate that the three ores sampled at different locations all contain magnetite-like, hematite-like, and iron(III) salts other than hematite. In addition, we confirmed the presence of phosphate around the grain boundary in the magnetite-like mineral phase by infrared microspectroscopic analysis. The present analytical findings of trace amounts of europium(III) using TRLFS suggest that the europium ions generate identical luminescence spectra despite being embedded in three different matrices of iron minerals. This demonstration highlights the benefits of combinatorial spectroscopic analyses to gain insights into the effects of the environment of REs on their solid-state chemistry and shows the potential utility of TRLFS as a resource mining tool. Further applications of this approach in the analytical screening of rocks and minerals are feasible.


High-efficiency synthesis and properties of latent pigment red 272DPP-BOC by microwave irradiation

大石 知司*; 木村 ゆう*; 中島 清彦*; 渡邉 雅之; 青柳 登

Materials Sciences and Applications, 11(3), p.195 - 203, 2020/03

赤色ラテント顔料ジケトピロロピロール(Pig. Red 272: 272DPP)は、有機顔料として非常に重要な顔料である。本研究ではその高効率な合成法として272DPPをNMP(N-メチル-2-ピロリドン)溶媒中でマイクロウェーブ(MWs)を数秒照射することでDPPラテント顔料(272DPP-Boc)として86.2%の高収率で得ることに成功した。この顔料は、再結晶することで、赤色と黄色の二種類のラテント顔料結晶となり、その蛍光特性はこの二種類の結晶構造を反映した相違を示した。


Flow-electrode CDI removes the uncharged Ca-UO$$_{2}$$-CO$$_{3}$$ ternary complex from brackish potable groundwater; Complex dissociation, transport, and sorption

Ma, J.*; Zhang, Y.*; Collins, R. N.*; Tsarev, S.*; 青柳 登; Kinsela, A. S.*; Jones, A. M.*; Waite, T. D.*

Environmental Science & Technology, 53(5), p.2739 - 2747, 2019/03

 被引用回数:34 パーセンタイル:88.19(Engineering, Environmental)

Unacceptably high uranium concentrations in decentralized and remote potable groundwater resources, especially those of high hardness, are a common worldwide problem. The complexation of alkali earth metals, carbonate and uranium(VI) results in the formation of thermodynamically stable ternary aqueous species that are predominantly neutrally-charged. The removal of the uncharged (non-adsorbing) complexes is a problematic issue for many water treatment technologies. As such, we have evaluated the efficacy of a recently-developed electrochemical technology, termed flow-electrode capacitive deionization (FCDI), to treat a synthetic groundwater, the composition of which is comparable to groundwater resources in the Northern Territory, Australia. Theoretical calculations and time-resolved laser fluorescence spectroscopy analyses confirmed that the complex was the primary aqueous species followed. Results under different operating conditions demonstrated that FCDI is versatile in reducing uranium concentrations to $$<$$ 10 $$mu$$g L$$^{-1}$$ with low electrical consumption (e.g. $$sim$$ 0.1 kWh m$$^{-3}$$). It is concluded that the capability of FCDI to remove uranium under these common conditions depends on the dissociation kinetics of the complex in the electrical field.


Optical properties of trinuclear citrate complexes containing 4f and 5f block metals

青柳 登; Palladino, G.*; 長崎 晋也*; 木村 貴海

Bulletin of the Chemical Society of Japan, 91(6), p.882 - 890, 2018/06

 被引用回数:1 パーセンタイル:4.93(Chemistry, Multidisciplinary)



Europium binding to humic substances extracted from deep underground sedimentary groundwater studied by time-resolved laser fluorescence spectroscopy

斉藤 拓巳*; 青柳 登; 寺島 元基

Journal of Nuclear Science and Technology, 54(4), p.444 - 451, 2017/04

 被引用回数:4 パーセンタイル:41.83(Nuclear Science & Technology)




瀬川 優佳里; 堀田 拓摩; 北辻 章浩; 熊谷 友多; 青柳 登; 中田 正美; 音部 治幹; 田村 行人*; 岡本 久人; 大友 隆; et al.

JAEA-Technology 2016-039, 64 Pages, 2017/03




Role of Tf$$_{2}$$N$$^{-}$$ anions in the ionic liquid-water distribution of europium(III) chelates

岡村 浩之; 青柳 登; 下条 晃司郎; 長縄 弘親; 井村 久則*

RSC Advances (Internet), 7(13), p.7610 - 7618, 2017/01

 被引用回数:16 パーセンタイル:54.43(Chemistry, Multidisciplinary)

液-液分配および時間分解レーザー励起蛍光分光法(TRLFS)によって、2-テノイルトリフルオロアセトン(Htta)によるEu(III)キレートのイオン液体-水分配系におけるビス(トリフルオロメタンスルホニル)イミド(Tf$$_{2}$$N$$^{-}$$)アニオンの役割を研究した。Eu(tta)$$_{3}$$の分配定数に対するイオン液体の効果を正則溶液論に基づいて評価したところ、1-アルキル-3-メチルイミダゾリウムビス(トリフルオロメタンスルホニル)イミド([C$$_{n}$$mim][Tf$$_{2}$$N])におけるEu(tta)$$_{3}$$の分配定数は、[C$$_{n}$$mim][Tf$$_{2}$$N]中のEu(tta)$$_{3}$$の溶媒和効果により著しく増加することがわかった。また、合成した[Eu(tta)$$_{3}$$(H$$_{2}$$O)$$_{3}$$]のTRLFSから、一連の[C$$_{n}$$mim][Tf$$_{2}$$N]中ではEu(tta)$$_{3}$$キレートはほぼ完全に脱水和することが明らかになった。さらに、20Mの水を含む過塩素酸1-エチル-3-メチルイミダゾリウム([C$$_{2}$$mim][ClO$$_{4}$$])中では、2あるいは3分子の水が配位していたのに対して、0.50 MのTf$$_{2}$$N$$^{-}$$と20 Mの水を含む[C$$_{2}$$mim][Tf$$_{2}$$N, ClO$$_{4}$$]中では水和数は約1となった。これらの結果から、[Eu(tta)$$_{3}$$(H$$_{2}$$O)$$_{3}$$]の配位水がTf$$_{2}$$N$$^{-}$$アニオンに置換されることが示された。実際、[C$$_{4}$$mim][Tf$$_{2}$$N]存在下におけるエレクトロスプレーイオン化質量分析法により、アニオン性の付加物[Eu(tta)$$_{3}$$(Tf$$_{2}$$N)]$$^{-}$$が観測された。


Sorption of Eu$$^{3+}$$ on Na-montmorillonite studied by time-resolved laser fluorescence spectroscopy and surface complexation modeling

佐々木 隆之*; 上田 健揚*; 斉藤 拓巳; 青柳 登; 小林 大志*; 高木 郁二*; 木村 貴海; 舘 幸男

Journal of Nuclear Science and Technology, 53(4), p.592 - 601, 2016/04

 被引用回数:12 パーセンタイル:78.53(Nuclear Science & Technology)

ナトリウム型モンモリロナイトへのEu(III)の収着に対するpH, Eu濃度,硝酸塩濃度の影響について、バッチ収着試験と時間分解型レーザー誘起蛍光分光(TRLFS)によって調査された。0.01M硝酸ナトリウム中では分配係数(Kd)はpHにほとんど依存せず、一方で、1M硝酸ナトリウム中ではKdはpHに大きく依存した。陽イオン交換モデルと1サイトの静電補正を考慮しない表面錯体モデルを組み合せたモデルによってKdデータが解釈された。Eu表面化学種に対するTRLFSスペクトルはパラレル因子分析法(PARAFAC)により解析され、1つの外圏錯体(ファクターA)と2つの内圏錯体(ファクターB及びC)への対応が示唆された。ファクターAとBは、イオン交換サイトへ収着したEu、エッジの水酸基との内圏錯体に、それぞれ対応するものである。ファクターCは比較的高いpH、イオン強度条件で支配的であり、表面におけるEu(OH)$$_{3}$$の析出物と評価された。


Physicochemical and ion-binding properties of highly aliphatic humic substances extracted from deep sedimentary groundwater

斉藤 拓巳; 寺島 元基; 青柳 登; 長尾 誠也*; 藤嶽 暢英*; 大貫 敏彦

Environmental Science; Processes & Impacts, 17(8), p.1386 - 1395, 2015/08

 被引用回数:7 パーセンタイル:27.83(Chemistry, Analytical)



Uranium binding mechanisms of the acid-tolerant fungus ${{it Coniochaeta fodinicola}}$

V$'a$zquez-Campos, X.*; Kinsela, A. S.*; Collins, R. N.*; Neilan, B. A.*; 青柳 登; Waite, T. D.*

Environmental Science & Technology, 49(14), p.8487 - 8496, 2015/07

 被引用回数:28 パーセンタイル:68.5(Engineering, Environmental)

本論文は、ウラン鉱山の処理水試料から単離された、好酸性/耐酸性菌の菌株によるウランの吸着や結合挙動を研究したものである。菌株の生存率は、溶液からウランを除去する容量に決定的に依存することがわかった。実際に、2時間の反応で、生きた菌は乾燥重量で16mg U/gのウランを除去し、死滅した菌は45mg U/gを除去した。さらに10分間の酸による洗浄でウランの20$$sim$$50%は溶出・除去された。X線吸収分光の結果はウランの結合は細胞の生存率に大きく依存しており、生きた細胞では、炭素やリン原子との距離は同様であったが、秩序だったウランの結合環境が見られた。レーザー分光と組み合わせることで、菌細胞死によって放出されたと考えられる有機酸およびリン酸塩, 多糖類は、この系において最初のウランの結合を決定づけることがわかった。この結果は、フロントエンドにおける湿式精錬法においてウランの金属イオン封鎖作用を理解する重要な進展である。


Photophysical property of $$catena$$-bis(thiocyanato)aurate(I) complexes in ionic liquids

青柳 登; 榛葉 祐介*; 池田 篤史*; 芳賀 芳範; 下条 晃司郎; Brooks, N. R.*; 泉岡 明*; 長縄 弘親; 木村 貴海; Binnemans, K.*

Crystal Growth & Design, 15(3), p.1422 - 1429, 2015/03

 被引用回数:11 パーセンタイル:66.61(Chemistry, Multidisciplinary)



Optical properties of tetravalent uranium complexes in non-aqueous media

青柳 登; 渡邉 雅之; 桐島 陽*; 佐藤 修彰*; 木村 貴海

Journal of Radioanalytical and Nuclear Chemistry, 303(2), p.1095 - 1098, 2015/02

 被引用回数:5 パーセンタイル:43.03(Chemistry, Analytical)

Tetravalent uranium halides were studied to understand photo-physical behaviors under the unexplored condition such as in non-aqueous media at ambient condition or at a cryogenic temperature. The anhydrous uranium tetrahalides (synthesized) were added into a series of dry organic solvents or a hydrophilic ionic liquid to observe their UV-Vis-NIR absorption spectra and time-resolved luminescence spectra in detail. The lower energy bands of UX$$_{4}$$ (X = F, Br, and I) appearing in UV-Vis-NIR absorption spectra in dry 1,4-dioxane were assigned as the transition from the ground state manifold to higher multiples ranging from 6,000 to 12,000 cm$$^{-1}$$. In contrast, there is the spectral emerging for these absorption spectra in the IL at higher energy band around 12,000 to 18,000 cm$$^{-1}$$ with each peak broadened. These complexes exhibit white photoluminescence by UV-pulse excitation at $$lambda$$$$_{ex}$$ = 394 nm, with broad multiple peaks assigned. The fluorescence lifetimes for these are 12.8 ns (1,4-dioxane) and 18.6 ns (IL) in spite of the longer U-I separation than that of U-NCS. Chemical species and the coordination number of U$$^{rm IV}$$ in water, in organic solutions, and in an IL could be thoroughly different, resulting in a variety of spectra.


Time-resolved laser-induced fluorescence spectroscopy combined with parallel factor analysis; A Robust speciation technique for UO$$_{2}$$$$^{2+}$$

斉藤 拓巳; 青柳 登; 木村 貴海

Journal of Radioanalytical and Nuclear Chemistry, 303(2), p.1129 - 1132, 2015/02

 被引用回数:14 パーセンタイル:78.53(Chemistry, Analytical)

時間分解型レーザ蛍光法(TRLFS)は蛍光性イオンの化学種分布評価に有用な分析手法であり、その化学種弁別能はマルチモード因子分析の一種であるPARAFACと組み合わせることで、さらに向上する。本研究では、ケイ酸存在下でのウラニルの化学種分布の評価をTRLFSとPARAFACを組合せて行うことで、ウラニルへの同手法の適用性を示した。異なるケイ酸濃度で測定した一連のTRLFSデータにPARAFACを適用することで、フリーのUO$$_{2}$$$$^{2+}$$, UO$$_{2}$$SiO(OH)$$_{3}$$$$^{+}$$, UO$$_{2}$$OH$$^{+}$$に対応する3つの蛍光成分が存在することが分かった。そして、それらの成分の濃度変化より、ウラニルとケイ酸の錯生成の安定度定数を決定した。


Radioactive fallout cesium in sewage sludge ash produced after the Fukushima Daiichi nuclear accident

香西 直文; 鈴木 伸一; 青柳 登; 坂本 文徳; 大貫 敏彦

Water Research, 68, p.616 - 626, 2015/01

 被引用回数:19 パーセンタイル:64.66(Engineering, Environmental)




伊奈川 潤; 宝徳 忍; 小田 哲三; 青柳 登; 間柄 正明

JAEA-Technology 2014-007, 48 Pages, 2014/03




Highly efficient extraction separation of lanthanides using a diglycolamic acid extractant

下条 晃司郎; 青柳 登; 斎藤 拓巳*; 岡村 浩之; 久保田 富生子*; 後藤 雅宏*; 長縄 弘親

Analytical Sciences, 30(2), p.263 - 269, 2014/02

 被引用回数:43 パーセンタイル:85.59(Chemistry, Analytical)

$$N$$,$$N$$-dioctyldiglycolamic acid (DODGAA) enables the quantitative partitioning of all Ln$$^{3+}$$ ions from moderately acidic solutions, while showing selectivity for heavier lanthanides, and provides remarkably high extraction separation performance for Ln$$^{3+}$$ compared with typical carboxylic acid extractants. Furthermore, the mutual separation abilities of DODGAA for light lanthanides are higher than those of organophosphorus extractants. Slope analysis, loading tests, and electrospray ionization mass spectrometry measurements demonstrated that the transfer of Ln$$^{3+}$$ with DODGAA proceeded through a proton-exchange reaction, forming a 1:3 complex, Ln(DODGAA)$$_{3}$$. The stripping of Ln$$^{3+}$$ from the extracting phase was successfully achieved under acidic conditions. Time-resolved laser-induced fluorescence spectroscopy revealed that the extracted Eu$$^{3+}$$ ions were completely dehydrated by complexation with DODGAA.

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