Study of mechanism of non-destructive laser desorption ionization and development of efficient detection methods by controling excitation condisitons

• Project/Area Number: 15H03772
• Research Category: Grant-in-Aid for Scientific Research (B)
• Allocation Type: Single-year Grants
• Section: 一般
• Research Field: Physical chemistry
• Research Institution: Toyo University (2016-2019); Tokyo Metropolitan University (2015)
• Principal Investigator: Fujino Tatsuya 東洋大学, 理工学部, 教授 (20360638)
• Project Period (FY): 2015-04-01 – 2020-03-31
• Project Status: Completed (Fiscal Year 2019)
• Budget Amount: ¥16,640,000 (Direct Cost: ¥12,800,000、Indirect Cost: ¥3,840,000); Fiscal Year 2019: ¥3,250,000 (Direct Cost: ¥2,500,000、Indirect Cost: ¥750,000); Fiscal Year 2018: ¥3,250,000 (Direct Cost: ¥2,500,000、Indirect Cost: ¥750,000); Fiscal Year 2017: ¥3,250,000 (Direct Cost: ¥2,500,000、Indirect Cost: ¥750,000); Fiscal Year 2016: ¥3,250,000 (Direct Cost: ¥2,500,000、Indirect Cost: ¥750,000); Fiscal Year 2015: ¥3,640,000 (Direct Cost: ¥2,800,000、Indirect Cost: ¥840,000)
• Keywords: レーザー脱離イオン化 / 質量分析 / 時間分解分光 / ナノ粒子 / 質量分析法 / 分析科学 / ナノ微粒子 / 酸化物固体表面 / 微量分析 / マトリクス / MALDI法 / 分子脱離 / ダイナミクス

Outline of Final Research Achievements

Desorption dynamics in Matrix Assisted Laser Desorption Ionization (MALDI) has been studied. Based on the research results, we have developed useful matrices that improve reproducibility of analyte ion and enabled us quantification by MALDI mass spectrometry.

Academic Significance and Societal Importance of the Research Achievements

本研究は、反応機構の全体像の理解から出発することで、機能的に発展させたレーザー脱離イオン化法を提供する研究である。レーザー脱離イオン化法の問題点を包括的に解決し定量分析までを実現させる研究は他に類がない。生体物質の構造や薬物との反応が気相分光により可能になるという基礎研究への貢献だけでなく、医療現場における病源の特定、警察による取締現場における禁止薬物の同定、加工食品に含まれる農薬や不純物質、環境汚染物質の検出など、不純物を多く含み、本来なら分離作業を利用した精密かつ長時間の分析が必要な分野においても、簡便かつ有効な手法として本法を提供できるものと考えている。

Research Products

• [Int'l Joint Research] Chinese Academy of Agricultural Sciences/Xi’an Polytechnic University(中国)
• [Journal Article] MALDI Mass Spectrometry of Small Molecules Using Nanometer-sized Clay (2020)
  • Author(s): J. Xu J. N. Kondo, and T. Fujino
  • Journal Title: Analytical Sciences Volume: 36 Issue: 2 Pages: 177-181
  • DOI: 10.2116/analsci.19P213
  • NAID: 130007796073
  • ISSN: 0910-6340, 1348-2246
  • Year and Date: 2020-02-10
  • Peer Reviewed
• [Journal Article] Metal Nanoparticles Loaded on Zeolite for Laser Desorption/Ionization Mass Spectrometry of Low-molecular-weight Compounds (2019)
  • Author(s): J. Xu and T. Fujino
  • Journal Title: BUNSEKI KAGAKU Volume: 68 Issue: 11 Pages: 817-824
  • DOI: 10.2116/bunsekikagaku.68.817
  • NAID: 130007759822
  • ISSN: 0525-1931
  • Year and Date: 2019-11-05
  • Peer Reviewed
• [Journal Article] Time dependent changes of nicotine and cotinine in mouth cavity after smoking studied by MALDI MS using functional organic analog of zeolite (2019)
  • Author(s): J. Xu, M. Saklurai, K. Akiyama, S. Kurosu, S. Sato and T. Fujino
  • Journal Title: Biomed. J. Sci. Tech. Res. Volume: 19 Issue: 1 Pages: 1-1
  • DOI: 10.26717/bjstr.2019.19.003235
  • Peer Reviewed / Open Access
• [Journal Article] Matrix-assisted laser desorption ionization mass spectrometry of compounds containing carboxyl groups using CdTe and CuO nanoparticles (2018)
  • Author(s): M. Sakurai, T. Sato, J. Xu, S. Sato and T. Fujino
  • Journal Title: Appl. Sci. Volume: 8 Issue: 4 Pages: 492-492
  • DOI: 10.3390/app8040492
  • Peer Reviewed / Open Access
• [Journal Article] Silver nanoparticles loaded on ammonium exchanged zeolite as matrix for MALDI-TOF-MS analysis of short-chain n-alkanes (2018)
  • Author(s): M. Yang, K. Hashimoto and T. Fujino
  • Journal Title: Chem. Phys. Lett. Volume: 706 Pages: 525-532
  • DOI: 10.1016/j.cplett.2018.07.002
  • Peer Reviewed / Int'l Joint Research
• [Journal Article] Copper ion production using zeolite and application to MALDI MS of small molecules (2018)
  • Author(s): M. Sakurai, M. Yang, J. Xu, M. T. Nguyene, T. Yonezawa, K. Hashimoto and T. Fujino
  • Journal Title: Int. J. Mass Spectrom. Volume: 434 Pages: 179-184
  • DOI: 10.1016/j.ijms.2018.09.028
  • Peer Reviewed / Int'l Joint Research
• [Journal Article] Chirality and structure-selective MALDI using mold matrix (2018)
  • Author(s): Y. Fujii, J. Xu and T. Fujino
  • Journal Title: Sci. Rep. Volume: 8 Issue: 1 Pages: 13138-13138
  • DOI: 10.1038/s41598-018-31629-6
  • Peer Reviewed / Open Access
• [Journal Article] Vibrational cooling effect of zeolite on molecular desorption studied by time-resolved laser desorption ionization mass spectrometry (2018)
  • Author(s): J. Xu and T. Fujino
  • Journal Title: Biomed. J. Sci. Tech. Res. Volume: 12 Issue: 1 Pages: 2-2
  • DOI: 10.26717/bjstr.2018.12.002191
  • Peer Reviewed / Open Access
• [Journal Article] Detection and Quantification of 4-Methylimidazole in Cola by Matrix-assisted Laser Desorption Ionization Mass Spectrometry with Fe₂O₃ Nanoparticles on Zeolite (2018)
  • Author(s): Yosuke FUJII, Yuqi DING, Taichi UMEZAWA, Takafumi AKIMOTO, Jiawei XU, Takashi UCHIDA, and Tatsuya FUJINO
  • Journal Title: Analytical Sciences Volume: 34 Issue: 2 Pages: 221-225
  • DOI: 10.2116/analsci.34.221
  • NAID: 130006342067
  • ISSN: 0910-6340, 1348-2246
  • Peer Reviewed / Int'l Joint Research
• [Journal Article] Direct Measurement and Quantification of Drugs and Their Metabolites in Urine by MALDI-MS Using Zeolite (2017)
  • Author(s): C. Kitaoka, T. Asano, T. Fujino
  • Journal Title: Bulletin of the Chemical Society of Japan Volume: 90 Issue: 2 Pages: 154-160
  • DOI: 10.1246/bcsj.20160311
  • NAID: 130005332371
  • ISSN: 0009-2673, 1348-0634
  • Peer Reviewed / Acknowledgement Compliant
• [Journal Article] Laser Desorption Ionization Mass Spectrometry of Pentacene Using 2-step Excitation Energy Transfer from Anthracene (2017)
  • Author(s): Yosuke Fujii, and Tatsuya Fujino
  • Journal Title: BUNSEKI KAGAKU Volume: 66 Issue: 2 Pages: 115-119
  • DOI: 10.2116/bunsekikagaku.66.115
  • NAID: 130005465015
  • ISSN: 0525-1931
  • Peer Reviewed
• [Journal Article] Synthesis of hydrogen- and methyl-capped long-chain polyynes by intense ultrashort laser pulse irradiation of toluene (2017)
  • Author(s): Ali Ramadhan, Michal Wesolowski, Tomonari Wakabayashi, Haruo Shiromaru, Tatsuya Fujino, Takeshi Kodama, Walter Duley, Joseph Sanderson
  • Journal Title: Carbon Volume: 118 Pages: 680-685
  • DOI: 10.1016/j.carbon.2017.03.096
  • Peer Reviewed / Int'l Joint Research
• [Journal Article] 2-Step励起エネルギー移動を利用したペンタセンのレーザー脱離イオン化質量分析法 (2017)
  • Author(s): 藤井洋佑, 藤野竜也
  • Journal Title: 分析化学 Volume: 66 Pages: 115-119
  • NAID: 130005465015
  • Peer Reviewed / Acknowledgement Compliant
• [Journal Article] Ammonium ion exchanged zeolite for laser desorption/ionization mass spectrometry of phosphorylated peptides (2015)
  • Author(s): M. Yang, *Tatsuya Fujino
  • Journal Title: International Journal of Analytical Chemistry Volume: 2015(513761) Pages: 1-5
  • Peer Reviewed / Open Access / Int'l Joint Research / Acknowledgement Compliant
• [Journal Article] Analyte-size-dependent ionization and quantification of monosaccharides in human plasma using cation-exchanged smectite layers (2015)
  • Author(s): Y. Ding, K. Kawakita, J. Xu, K. Akiyama, *Tatsuya Fujino
  • Journal Title: Analytical Chemistry Volume: 87(15) Pages: 7944-7950
  • Peer Reviewed / Int'l Joint Research / Acknowledgement Compliant
• [Presentation] Chiral and Structural selective MALDI using Mold Matrix (2019)
  • Author(s): J. Xu and T. Fujino
  • Organizer: Beijing Conference and Exhibition on Instrumental Analysis 2019
  • Int'l Joint Research
• [Presentation] 見たい分子を選択的に高強度に検出するレーザーイオン化法 (2019)
  • Author(s): 藤野竜也
  • Organizer: 日本Archaea研究会第３２回講演会
  • Invited
• [Presentation] 試料分子の構造を認識して検出するレーザー脱離イオン化質量分析法 (2019)
  • Author(s): 藤野竜也
  • Organizer: 日本分光学会生細胞分光部会シンポジウム
  • Invited
• [Presentation] レーザー支援脱離イオン化質量分析を用いたトマト缶に含まれる環境ホルモンの新規定量分析法の開発 (2018)
  • Author(s): Jiawei Xu ・ 藤野竜也
  • Organizer: 日本分析化学会 第６７年会
• [Presentation] 酸化鉄ナノ粒子を用いたMALDI法における清涼飲料水中発がん性物質の検出 (2017)
  • Author(s): 藤井洋佑、藤野竜也
  • Organizer: 日本分析化学会 第66年会
• [Presentation] 有機構造体をマトリクスに使用した MALDI -MS測定 (2017)
  • Author(s): 櫻井萌、藤野竜也
  • Organizer: 日本分析化学会 第66年会
• [Presentation] Improvement of the Ionization Efficiency of MALDI Using Zeolite Matrix for Simultaneous Imaging of Multiple Drugs Administered in Cancer Cells (2017)
  • Author(s): Shusei Nomura, Hisanao Hazama, Yasufumi Kaneda, Tatsuya Fujino, Kunio Awazu
  • Organizer: 65th American Society for Mass Spectrometry (ASMS) Annual Conference on Mass Spectrometry and Allied Topics
  • Int'l Joint Research
• [Presentation] 分子間励起エネルギー移動を用いたレーザー脱離イオン化質量分析の研究 (2016)
  • Author(s): 藤井洋佑、藤野竜也
  • Organizer: 日本分析化学会第６５年会（札幌）
  • Place of Presentation: 北海道大学工学部
  • Year and Date: 2016-09-14
• [Presentation] ハイドロキシアパタイトとニ酸化チタンを用いた マトリクスの有用性に関する研究 (2016)
  • Author(s): 川喜田健人、藤野竜也
  • Organizer: 日本分析化学会第６５年会（札幌）
  • Place of Presentation: 北海道大学工学部
  • Year and Date: 2016-09-14
• [Presentation] 一価の銅イオン付加によるタンパク質の高効率MALDI-MS検出に向けて (2016)
  • Author(s): 櫻井萌、藤野竜也
  • Organizer: 日本分析化学会第６５年会（札幌）
  • Place of Presentation: 北海道大学工学部
  • Year and Date: 2016-09-14
• [Presentation] マイクロ・ナノ構造体を利用した分子レーザーイオン化法の研究 (2016)
  • Author(s): 藤野竜也
  • Organizer: 第７６回分析化学討論会
  • Place of Presentation: 岐阜薬科大学・岐阜大学
  • Year and Date: 2016-05-28
• [Presentation] カチオン置換型スメクタイト層による測定物サイズに依存したレーザーイオン化及びヒト血漿中単糖類の定量分析に関する研究 (2015)
  • Author(s): 川喜田健人（発表）, Y. Ding, J. Xu, 秋山和彦, 藤野竜也
  • Organizer: 日本分析化学会 第64年会
  • Place of Presentation: 九州大学
  • Year and Date: 2015-09-09
• [Presentation] レーザーイオン化法によるスポーツドーピング薬の高感度検出に関する研究 (2015)
  • Author(s): 中圓尾綾（発表）, 藤野竜也
  • Organizer: 日本分析化学会 第64年会
  • Place of Presentation: 九州大学
  • Year and Date: 2015-09-09
• [Presentation] MALDI法による薬物代謝物の同時検出及び定量に関する研究 (2015)
  • Author(s): 北岡千裕（発表）, 浅野貴史, 藤野竜也
  • Organizer: 日本分析化学会 第64年会
  • Place of Presentation: 九州大学
  • Year and Date: 2015-09-09
• [Presentation] Application of CdTe Nanoparticles for Laser Ionization of Small Molecules (2015)
  • Author(s): Tatsuya Fujino
  • Organizer: Collaborative Conference on 3D and Materials Research (CC3DMR)
  • Place of Presentation: Busan, South Kore
  • Year and Date: 2015-06-15
  • Int'l Joint Research / Invited
• [Presentation] Quantitative Analysis of Free Fatty Acids in Human Serum Using CdTe Nanoparticles (2015)
  • Author(s): Tatsuya Fujino
  • Organizer: Annual Conference and EXPO of AnalytiX-2015
  • Place of Presentation: Nanjin, China
  • Year and Date: 2015-04-25
  • Int'l Joint Research / Invited
• [Book] 現代を生きるための化学 (2018)
  • Author(s): 橋本健朗、藤野竜也、三島正規
  • Total Pages: 252
  • Publisher: 放送大学教育振興会
  • ISBN: 9784595319020
• [Book] 理工系学生のための基礎化学 (2018)
  • Author(s): 吉田泰彦、田代基慶、谷村景貴、田島正弘、浜名浩、佐々木直樹、松浦宏昭、徳村雅弘、相沢宏明、菅又功、萩原時男、相川俊一、越後輝敦、熊澤隆、藤野竜也
  • Total Pages: 180
  • Publisher: 培風館
  • ISBN: 9784563046262