Fluctuation at ice/freeze-concentrated-solution interface. Measurement by microspectroscopy and elucidation of its dynamics

• Project/Area Number: 19K15599
• Research Category: Grant-in-Aid for Early-Career Scientists
• Allocation Type: Multi-year Fund
• Review Section: Basic Section 34020:Analytical chemistry-related
• Research Institution: Utsunomiya University
• Principal Investigator: Inagawa Arinori 宇都宮大学, 工学部, 助教 (30828489)
• Project Period (FY): 2019-04-01 – 2023-03-31
• Project Status: Completed (Fiscal Year 2022)
• Budget Amount: ¥4,290,000 (Direct Cost: ¥3,300,000、Indirect Cost: ¥990,000); Fiscal Year 2022: ¥390,000 (Direct Cost: ¥300,000、Indirect Cost: ¥90,000); Fiscal Year 2021: ¥260,000 (Direct Cost: ¥200,000、Indirect Cost: ¥60,000); Fiscal Year 2020: ¥2,080,000 (Direct Cost: ¥1,600,000、Indirect Cost: ¥480,000); Fiscal Year 2019: ¥1,560,000 (Direct Cost: ¥1,200,000、Indirect Cost: ¥360,000)
• Keywords: 氷 / 凍結濃縮溶液 / 界面 / 界面揺らぎ / 固液相転移 / プロトン勾配 / レーザー分光 / 顕微分光法 / ルテニウム錯体

Outline of Research at the Start

水溶液が凍結してできた氷は、相分離により氷の単結晶と溶質が濃縮された凍結濃縮溶液(Freeze Concentrated Solution: FCS)からなる不均一な構造を持つ。この不均一構造における氷/FCS界面は同じ水分子で構成されており、界面の揺らぎの存在が示唆されている。しかし、そのダイナミクスの詳細は未解明である。本研究では、顕微分光法による界面計測手法を確立し、氷/FCS界面揺らぎのダイナミクスを輸送現象の観点から解明することを目的とする。その手法として顕微鏡下での発光スペクトルおよびレーザー分光測定を構築し、氷/FCS界面における物質拡散や熱フォノン共鳴測定を行う。

Outline of Final Research Achievements

Single beam type phonon resonance spectroscopy was developed. We have found that ice surface has an ability to induce ion exchange reaction with gallium(III) complex. As an unique phenomena of micrometer-sized freeze concentrated solutions, we examined the observation of the collosion process of iron contacting with freeze concentrated solutions. We found that the collosion behavior is regulated by the size of the freeze concentrated solutions .

Academic Significance and Societal Importance of the Research Achievements

氷は身近な物質であるにも関わらず、その物理化学的現象やそれが環境中での化学反応で果たす役割は未解明な点が多い。本研究内容は、マイクロサイズの凍結濃縮溶液がどのように反応に影響を及ぼすのか、またどのような反応場を提供するのかを明らかにするための一助になると考えている。

Research Products

• [Journal Article] Rapid acquisition of absorption spectra to monitor proton migration in nanoliter space using the RGB-spectrum-conversion method with a 10?ms interval (2023)
  • Author(s): Kimura Yusuke、Inagawa Arinori、Uehara Nobuo
  • Journal Title: Analytical Sciences Volume: - Issue: 8 Pages: 1425-1432
  • DOI: 10.1007/s44211-023-00348-y
• [Journal Article] Contact Area Dependence of the Dissolution of Ferrous Ions from Pure Iron Wires into Freeze-Concentrated Solutions Revealed by a Combination of Microscopy and Image Processing (2023)
  • Author(s): Maeda Minami、Inagawa Arinori、Uehara Nobuo
  • Journal Title: Bulletin of the Chemical Society of Japan Volume: 96 Issue: 4 Pages: 367-372
  • DOI: 10.1246/bcsj.20230021
• [Journal Article] Charge-Selective Aggregation Behavior of Thermoresponsive Polyelectrolytes Having Low Charge Density in Aqueous Solutions of Organic Counterions (2023)
  • Author(s): Yasuda Asahi、Inagawa Arinori、Uehara Nobuo
  • Journal Title: Langmuir Volume: 39 Issue: 5 Pages: 1730-1739
  • DOI: 10.1021/acs.langmuir.2c02286
• [Journal Article] Dissolution Behavior of Iron in Contact with Frozen Electrolyte Solutions (2022)
  • Author(s): Minami Maeda, Nobuo Uehara, Arinori Inagawa
  • Journal Title: Journal of Ion Exchange Volume: 33 Issue: 4 Pages: 142-146
  • DOI: 10.5182/jaie.33.142
  • ISSN: 0915-860X, 1884-3360
  • Year and Date: 2022-11-04
  • Peer Reviewed / Open Access
• [Journal Article] In situ Visualization of Ferrous Ions Dissolved from Pure Iron Wire into Thin Frozen Aqueous Solution Films by Combination of Microscopy and Image Processing (2022)
  • Author(s): Inagawa Arinori、Maeda Minami、Uehara Nobuo
  • Journal Title: Sensors and Materials Volume: 34 Issue: 3 Pages: 915
  • DOI: 10.18494/SAM.2021.3448
  • ISSN: 0914-4935, 2435-0869
  • Year and Date: 2022-03-03
  • Peer Reviewed / Open Access
• [Journal Article] Fabrication of paper-based analytical devices by a laminating method with thermal ink ribbons, sticky notes, and office appliances (2022)
  • Author(s): Arinori Inagawa, Ken-ichi Iimura , Nobuo Uehara
  • Journal Title: Analytical Methods Volume: 15 Issue: 4 Pages: 537-542
  • DOI: 10.1039/d2ay01981g
  • Peer Reviewed / Open Access
• [Journal Article] 色彩情報が拓く比色分析の多様化 (2022)
  • Author(s): 稲川有徳
  • Journal Title: ぶんせき Volume: 1 Pages: 22-23
  • Peer Reviewed
• [Journal Article] デジタルカラー画像の色彩情報を用いた比色分析の開発とその展開 (2022)
  • Author(s): 稲川有徳、上原伸夫
  • Journal Title: 日本海水学会誌 Volume: 76 Pages: 2-10
  • Peer Reviewed
• [Journal Article] Total protein assay by PCA-based RGB-spectrum conversion methods with smartphone-acquired digital images (2022)
  • Author(s): Inagawa Arinori、Kimura Miwa、Uehara Nobuo
  • Journal Title: Analytical Sciences Volume: -
  • Peer Reviewed
• [Journal Article] Sulfated Steelmaking Slags as Se(IV) Adsorbents: Effects of Preparation Conditions on Adsorption Performance (2021)
  • Author(s): Hanada Kazutoshi、Watanabe Shun、Inagawa Arinori、Uehara Nobuo
  • Journal Title: ISIJ International Volume: 61 Issue: 1 Pages: 506-512
  • DOI: 10.2355/isijinternational.ISIJINT-2020-420
  • NAID: 130007969880
  • ISSN: 0915-1559, 1347-5460
  • Year and Date: 2021-01-15
  • Peer Reviewed / Open Access
• [Journal Article] Geometrical pH mapping of Microfluids by principal-component-analysis-based xyz-spectrum conversion method (2021)
  • Author(s): Inagawa Arinori、Saito Kana、Fukuyama Mao、Numata Munenori、Uehara Nobuo
  • Journal Title: Analytica Chimica Acta Volume: 1182 Pages: 338952-338952
  • DOI: 10.1016/j.aca.2021.338952
  • Peer Reviewed / Open Access
• [Journal Article] Quantitative Reduction of Iron under Nitrogen Atmosphere for Potassium Dichromate Titration (2021)
  • Author(s): Kadowaki Yuto、Yanagihara Yuko、Inagawa Arinori、Uehara Nobuo
  • Journal Title: Tetsu-to-Hagane Volume: 107 Issue: 7 Pages: 566-576
  • DOI: 10.2355/tetsutohagane.TETSU-2021-019
  • NAID: 130008058728
  • ISSN: 0021-1575, 1883-2954
  • Peer Reviewed / Open Access
• [Journal Article] Manipulation of aggregation-induced emission of thermoresponsive fluorescent polymers having Au(I)-S groups for a fluorescent chemosensor (2021)
  • Author(s): Uehara Nobuo、Masubuchi Yoshiki、Inagawa Arinori
  • Journal Title: Colloids and Surfaces A: Physicochemical and Engineering Aspects Volume: 618 Pages: 126459-126459
  • DOI: 10.1016/j.colsurfa.2021.126459
  • Peer Reviewed / Open Access
• [Journal Article] Linear Momentum of a Microfluid Realizes an Anisotropic Reaction at the Ends of a Supramolecular Nanofiber (2021)
  • Author(s): Kanzaki Chisako、Matoba Shota、Inagawa Arinori、Fukuhara Gaku、Okada Tetsuo、Narushima Tetsuya、Okamoto Hiromi、Numata Munenori
  • Journal Title: Bulletin of the Chemical Society of Japan Volume: 94 Issue: 2 Pages: 579-589
  • DOI: 10.1246/bcsj.20200279
  • NAID: 130007995343
  • Peer Reviewed
• [Journal Article] Dataset for reproducing absorption spectra of methyl orange from the RGB values of microscopic images (2020)
  • Author(s): Inagawa Arinori、Saito Kana、Sasaki Asuka、Uehara Nobuo
  • Journal Title: Data in Brief Volume: 31 Pages: 105998-105998
  • DOI: 10.1016/j.dib.2020.105998
• [Journal Article] Sample enrichment for microchip electrophoresis by target-selective extraction induced by phase separation of aqueous ionic liquids (2020)
  • Author(s): Arinori Inagawa, Nozomi Masuda, Toshiyuki Nikata, Nobuo Uehara
  • Journal Title: Chem Lett. Volume: 49 Issue: 8 Pages: 974-977
  • DOI: 10.1246/cl.200330
  • NAID: 130007884728
  • Peer Reviewed / Open Access
• [Journal Article] Spontaneous growth of gold nanoclusters to form gold nanoparticles in the presence of high molecular weight poly(ethylene glycol) (2020)
  • Author(s): Uehara Nobuo、Sonoda Natsumi、Iwamatsu Tsubasa、Haneishi Chikara、Inagawa Arinori
  • Journal Title: Colloids and Surfaces A: Physicochemical and Engineering Aspects Volume: 585 Pages: 124113-124113
  • DOI: 10.1016/j.colsurfa.2019.124113
  • Peer Reviewed / Open Access
• [Journal Article] Interaction between antifreeze protein and ice crystal facet evaluated by ice-channel electrophoretic measurements of threshold electric field strength (2020)
  • Author(s): Inagawa Arinori、Uehara Nobuo、Okada Tetsuo
  • Journal Title: Analytica Chimica Acta Volume: 1110 Pages: 122-130
  • DOI: 10.1016/j.aca.2020.03.025
  • Peer Reviewed / Open Access
• [Journal Article] Reproducing absorption spectra of pH indicators from RGB values of microscopic images (2020)
  • Author(s): Inagawa Arinori、Sasaki Asuka、Uehara Nobuo
  • Journal Title: Talanta Volume: - Pages: 120952-120952
  • DOI: 10.1016/j.talanta.2020.120952
  • Peer Reviewed / Open Access
• [Journal Article] Proton-gradient-driven self-assembly of porphyrin and in situ dynamic analysis in a microflow platform (2020)
  • Author(s): Chisako Kanzaki, Arinori Inagawa, Gaku Fukuhara, Tetsuo Okada, Munenori Numata
  • Journal Title: ChemSystemsChem Volume: -
  • Peer Reviewed
• [Journal Article] 氷マイクロフルイディクス：氷内部に形成したナノ・マイクロ構造を利用した分離・分析場の構築 (2020)
  • Author(s): 稲川有徳、岡田哲男
  • Journal Title: ぶんせき Volume: 3 Pages: 85-93
  • NAID: 40022201076
  • Peer Reviewed
• [Journal Article] Size-Tunable Micro-/Nanofluidic Channels Fabricated by Freezing Aqueous Sucrose (2019)
  • Author(s): Fujino Saori、Inagawa Arinori、Harada Makoto、Okada Tetsuo
  • Journal Title: ACS Omega Volume: 4 Issue: 8 Pages: 13570-13576
  • DOI: 10.1021/acsomega.9b01966
  • Peer Reviewed / Open Access
• [Presentation] Development of colorimetric analysis procedure with smartphone-captured images based on RGB-spectrumconversion methods (2020)
  • Author(s): A. Inagawa, N. Uehara
  • Organizer: RSC Tokyo International Conference 2020
  • Int'l Joint Research
• [Presentation] Selective detection of acidic amino acids using aggregation of cationic stimuli-responsive polymer (2020)
  • Author(s): A. Yasuda, N.Uehara, A. Inagawa
  • Organizer: RSC Tokyo International Conference 2020
  • Int'l Joint Research
• [Presentation] Development of Near-Infrared Fluorescent Organic-Inorganic Hybrids for Polysaccharide Sensors (2020)
  • Author(s): Y. Awaya, A. Inagawa, N. Uehara
  • Organizer: RSC Tokyo International Conference 2020
  • Int'l Joint Research
• [Presentation] Effect of molecular structure on fluorescence fluctuation of water-soluble polymer incorporating fluorophore (2020)
  • Author(s): H. Shimazu, A. Inagawa, N. Uehara
  • Organizer: RSC Tokyo International Conference 2020
  • Int'l Joint Research
• [Presentation] RGB- スペクトル変換法によるスマートフォン画像を利用した比色分析法の開発”、令和2年度分析イノベーション交流会 (2020)
  • Author(s): 稲川有徳、上原伸夫
  • Organizer: 令和2年度分析イノベーション交流会
• [Presentation] 氷表面のダングリングボンドとガリウム(III)錯体との配位子交換反応 (2020)
  • Author(s): 稲川有徳、高山俊也、上原伸夫
  • Organizer: 第80回分析化学討論会
• [Presentation] 透過顕微画像のRGB値を用いた微小空間における吸収スペクトルの再現 (2020)
  • Author(s): 佐々木明日香、上原伸夫、稲川有徳
  • Organizer: 第80回分析化学討論会
• [Presentation] イオン液体/水系の相分離を利用したマイクロチップ電気泳動の高感度化 (2020)
  • Author(s): 増田望実、上原伸夫、稲川有徳
  • Organizer: 第80回分析化学討論会
• [Presentation] カチオン性刺激応答性高分子の静電相互作用を利用した呈味性アミノ酸の検出 (2020)
  • Author(s): 保田あさ陽、上原伸夫、稲川有徳
  • Organizer: 第80回分析化学討論会
• [Presentation] ポリエチレングリコールを用いて調製した金ナノ粒子の崩壊に基づくチオール化合物の定量 (2020)
  • Author(s): 岩松翼、稲川有徳、上原伸夫
  • Organizer: 第80回分析化学討論会
• [Presentation] Charging of ice surfaces studied by zeta potential determination (2019)
  • Author(s): Arinori Inagawa Tetsuo Okada
  • Organizer: 9th International Colloids Conference
  • Int'l Joint Research
• [Presentation] Controlled Self-assembly of Porphyrins in Microflow Space (2019)
  • Author(s): Chisako Kanzaki, Arinori Inagawa, Gaku Fukuhara, Tetsuo Okada, Munenori Numata
  • Organizer: International Society of Heterocyclic Chemistry Congress
  • Int'l Joint Research
• [Presentation] Fluorescence Fluctuation of Stimuli-Responsive Polymers Conjugated with Fluorescent Moiety (2019)
  • Author(s): Ryo Saito, Arinori Inagawa, Nobuo Uehara
  • Organizer: RSC Tokyo International Conference 2019
  • Int'l Joint Research
• [Presentation] Extraction of Free MgO in Steel Slugs with 2,2,2-Trichloroethanol (2019)
  • Author(s): Yuto Kadowaki, Arinori Inagawa, Nobuo Uehara
  • Organizer: RSC Tokyo International Conference 2019
  • Int'l Joint Research
• [Presentation] Near-Infrared Fluorescent Silica Gel Containing Gold(I)-Thiol Moiety Prepared by Sol-Gel Method (2019)
  • Author(s): Yuuki Awaya, Arinori Inagawa, Nobuo Uehara
  • Organizer: RSC Tokyo International Conference 2019
  • Int'l Joint Research
• [Presentation] 氷グレインバウンダリー電気泳動法による氷-不凍たんぱく質間に働く相互作用力の単一分子レベルでの定量的評価 (2019)
  • Author(s): 稲川有徳、上原伸夫、岡田哲男
  • Organizer: 日本分析化学会第68年会
• [Presentation] 金ナノクラスターとポリエチレングリコールとの反応に及ぼすチオール化合物の影響 (2019)
  • Author(s): 岩松翼・稲川有徳・上原伸夫
  • Organizer: 日本分析化学会第68年会
• [Presentation] 凝集誘起増感に基づく刺激応答型蛍光性金ポリマーを用いるたんぱく質の定量 (2019)
  • Author(s): 上原伸夫・増渕由樹・稲川有徳
  • Organizer: 日本分析化学会第68年会
• [Presentation] 氷グレインバウンダリー電気泳動法による氷-不凍たんぱく質間に働く相互作用力の評価 (2019)
  • Author(s): 稲川有徳・上原伸夫・岡田哲男
  • Organizer: 第39回キャピラリー電気泳動シンポジウム
• [Presentation] 氷グレインバウンダリーを用いる不凍たんぱく質と氷の相互作用の定量的評価 (2019)
  • Author(s): 稲川有徳・上原伸夫・岡田 哲男
  • Organizer: 第79回分析化学討論会
• [Presentation] 郵送型検査キットによる体臭測定と、その応用によるバイオマーカー探索 (2019)
  • Author(s): 石田翔太・稲川有徳・関本奏子
  • Organizer: 第79回分析化学討論会
• [Presentation] 定常的なエネルギー供給により実現する高活性超分子の創製とその速度論的安定化 (2019)
  • Author(s): 神崎千沙子・稲川有徳・福原学・岡田哲男・沼田宗典
  • Organizer: 第17回ホスト―ゲスト・超分子化学シンポジウム
• [Presentation] 蛍光スペクトルに揺らぎを示す刺激応答型蛍光性高分子の創製と評価 (2019)
  • Author(s): 齋藤凌・稲川有徳・上原伸夫
  • Organizer: 令和元年度日本分析化学会関東支部若手交流会
• [Presentation] 金(I)-チオール部位を有する蛍光性シリカゲルのゾルゲル法による創製とその物性評価 (2019)
  • Author(s): 粟屋友貴・稲川有徳・上原伸夫
  • Organizer: 令和元年度日本分析化学会関東支部若手交流会
• [Presentation] 金(Ⅰ)-チオール部位を有する蛍光性シリカゲルのゾルゲル法による創製とその物性評価 (2019)
  • Author(s): 粟屋友貴・稲川有徳・上原伸夫
  • Organizer: 日本分析化学会第68年会
• [Presentation] 蛍光スペクトルにゆらぎを示す刺激応答型蛍光性高分子の創製と評価 (2019)
  • Author(s): 齋藤凌・稲川有徳・上原伸夫
  • Organizer: 日本分析化学会第68年会
• [Presentation] トリクロロエタノールを用いる製鋼スラグからの遊離状態のMgOの抽出と定量 (2019)
  • Author(s): 門脇優人・稲川有徳・上原伸夫
  • Organizer: 日本分析化学会第68年会
• [Book] Ice Microfluidics Ice as Size-Tunable Separation Field and Physicochemical Nature of Freeze Concentrated Solutions (2019)
  • Author(s): Arinori Inagawa
  • Total Pages: 125
  • Publisher: Springer Singapore
• [Remarks] プレスリリース：計測化学研究室が画像解析による新しい顕微分光法を開発
  • URL: http://www.chem.utsunomiya-u.ac.jp/home/info.html#d200324
• [Remarks] プレスリリース：稲川有徳助教がSpringer Thesis Award を受賞
  • URL: http://www.chem.utsunomiya-u.ac.jp/home/info.html#d190527