• Search Research Projects
  • Search Researchers
  • How to Use
  1. Back to previous page

Development of catalyst-free selective oxidation method using flow reactors that selectively arrange the desired active species

Research Project

Project/Area Number 21H01697
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Review Section Basic Section 27020:Chemical reaction and process system engineering-related
Research InstitutionTohoku University

Principal Investigator

Takahashi Atsushi  東北大学, 工学研究科, 准教授 (60357366)

Project Period (FY) 2021-04-01 – 2024-03-31
Project Status Completed (Fiscal Year 2023)
Budget Amount *help
¥17,810,000 (Direct Cost: ¥13,700,000、Indirect Cost: ¥4,110,000)
Fiscal Year 2023: ¥2,730,000 (Direct Cost: ¥2,100,000、Indirect Cost: ¥630,000)
Fiscal Year 2022: ¥4,160,000 (Direct Cost: ¥3,200,000、Indirect Cost: ¥960,000)
Fiscal Year 2021: ¥10,920,000 (Direct Cost: ¥8,400,000、Indirect Cost: ¥2,520,000)
Keywords選択酸化反応 / 低温大気圧プラズマ / 活性酸素種 / 速度論解析 / 選択酸化 / 速度論モデル / 触媒フリー / フローリアクターシステム / 貴金属触媒
Outline of Research at the Start

空気中の酸素のみを使って有機化合物を選択的に酸化することは、経済性、環境性、持続性から理想的な反応である。これまで不均一系触媒の使用が検討されてきたが、経済性や有限資源利用による持続性を考慮すると、触媒なしでの選択酸化技術の確立も今後重要となる。本研究では、水溶液への低温大気圧プラズマ照射により生成する活性酸素種を活用し、速度論解析による活性種の寿命予測と反応器のフローシステム化を組み合わせた活性種空間再配置型フローリアクターシステムを新たに構築し、触媒フリーで所望の選択酸化反応のみを進行させる手法を確立する。

Outline of Final Research Achievements

This research aimed to establish a method for conducting selective oxidation reactions using activated oxygen without catalysts. Utilizing low-temperature atmospheric pressure plasma under mild conditions, successful selective oxidation of glycerin was achieved. Kinetic model analysis confirmed that reactive oxygen species generated by plasma irradiation are effective for selective oxidation reactions. Notably, the study found that the oxidation mechanism switches with pH conditions, allowing the generation of selective oxidation products typically obtained using gold and platinum catalysts. Additionally, a flow reactor was designed and prototyped, demonstrating the capability for continuous production of glyceric acid. This study represents a significant step towards realizing sustainable oxidation processes without the need for catalysts.

Academic Significance and Societal Importance of the Research Achievements

学術的意義としては、触媒を使用しない選択酸化反応の新たなアプローチを示した点にある。低温大気圧プラズマを利用することで、従来の貴金属触媒に依存しない新たな反応システムの可能性が開かれた。特に、水へのプラズマ照射で生成する活性酸素種に選択酸化が可能な種が存在することを明示したことは意義深い。社会的意義としては、希少かつ有限資源である貴金属を使用せず、かつ温和な条件での選択酸化プロセスの確立により、資源の節約に加え、環境負荷の低減ならびに省エネルギーも期待される。また、再生可能資源であるバイオマスの有効利用法としても本選択酸化システムの活用によって持続可能な社会の実現に貢献することが期待される。

Report

(4 results)
  • 2023 Annual Research Report   Final Research Report ( PDF )
  • 2022 Annual Research Report
  • 2021 Annual Research Report
  • Research Products

    (15 results)

All 2024 2023 2022 2021

All Journal Article (2 results) (of which Peer Reviewed: 2 results,  Open Access: 1 results) Presentation (13 results) (of which Int'l Joint Research: 5 results,  Invited: 6 results)

  • [Journal Article] Application of nonthermal atmospheric-pressure plasma irradiation as a new method for noncatalytic liquid-phase selective oxidation of polyhydric alcohols2024

    • Author(s)
      T. Chida,K. Hiromori,N. Shibasaki-Kitakawa,S. Sasaki,T. Kaneko,and A. Takahashi
    • Journal Title

      Plasma Processes and Polymers

      Volume: 21 Issue: 4 Pages: 2300163-2300163

    • DOI

      10.1002/ppap.202300163

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Comprehensive Study on Kinetic Modeling of Liquid-Phase Selective Oxidation Using Au-Supported Catalysts for Efficient Production of Value-Added Chemicals from Glycerol2023

    • Author(s)
      Tsutomu Chida、Kousuke Hiromori、Naomi Shibasaki-Kitakawa、Naoki Mimura、Aritomo Yamaguchi、Atsushi Takahashi
    • Journal Title

      Industrial & Engineering Chemistry Research

      Volume: 62 Issue: 18 Pages: 6932-6942

    • DOI

      10.1021/acs.iecr.3c00336

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed
  • [Presentation] 触媒フリーの選択酸化反応に向けた低温大気圧プラズマの応用2024

    • Author(s)
      高橋厚
    • Organizer
      東北プラズマフォーラム(仙台)
    • Related Report
      2023 Annual Research Report
    • Invited
  • [Presentation] Design of catalyst-free selective oxidation system for glycerol valorization using nonthermal atmospheric pressure plasma2024

    • Author(s)
      Tsutomu Chida, Yuya Nakagaki, Shota Sasaki, Kousuke Hiromori, Naomi Shibasaki-Kitakawa, Atsushi Takahashi
    • Organizer
      2024 AOCS Annual Meeting & Expo(Montreal, Quebec, Canada)
    • Related Report
      2023 Annual Research Report
    • Invited
  • [Presentation] Non-catalytic selective oxidation of glycerol under mildcondition by low-temperature atmospheric pressure plasmairradiation2023

    • Author(s)
      Tsutomu Chida, Yuya Nakagaki, Kousuke Hiromori, Naomi Shibasaki-Kitakawa, Shota Sasaki, Atsushi Takahashi
    • Organizer
      2023 AOCS Annual Meeting & Expo(Denver, Colorado, USA)
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] 低温大気圧プラズマを用いた触媒フリーの選択酸化反応場の設計2023

    • Author(s)
      千田 勤,廣森 浩祐,北川 尚美,高橋 厚
    • Organizer
      化学工学会第54回秋季大会(福岡)
    • Related Report
      2023 Annual Research Report
    • Invited
  • [Presentation] 低温大気圧プラズマを用いた無触媒選択酸化によるポリオールの高付加価値化2023

    • Author(s)
      中垣友哉,千田勤,廣森浩祐,北川尚美,佐々木渉太,高橋厚
    • Organizer
      第12回 JACI/GSCシンポジウム (東京)
    • Related Report
      2023 Annual Research Report
  • [Presentation] 低温大気圧プラズマ照射からの活性酸素種を利用した選択酸化に関する基礎的研究2023

    • Author(s)
      中垣 友哉,千田 勤,廣森 浩祐,北川 尚美,佐々木 渉太,高橋 厚
    • Organizer
      化学工学会第54回秋季大会(福岡)
    • Related Report
      2023 Annual Research Report
  • [Presentation] 低温大気圧プラズマ照射を利用した常温下でのグリセリン選択酸化2023

    • Author(s)
      千田 勤・中垣 友哉・ 廣森 浩祐・北川 尚美・ 佐々木 渉太・高橋 厚
    • Organizer
      化学工学会第88年会(東京), 口頭発表
    • Related Report
      2022 Annual Research Report
  • [Presentation] 大気圧非平衡プラズマ照射によるグリセリンの無触媒液相選択酸化2023

    • Author(s)
      中垣 友哉・千田 勤・廣森 浩祐・北川 尚美・佐々木 渉太・高橋 厚
    • Organizer
      第25回化学工学会学生発表会(オンライン), 口頭発表
    • Related Report
      2022 Annual Research Report
  • [Presentation] Process design for efficient production from glycerol into high-value chemicals2022

    • Author(s)
      Tsutomu Chida, Kousuke Hiromori, Naomi Shibasaki-Kitakawa, Naoki Mimura, Aritomo Yamaguchi, Atsushi Takahashi
    • Organizer
      2022 AOCS Annual Meeting & Expo (Atlanta, Georgia, USA), Oral
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Control of selective oxidation of biomass by kinetic model incorporating multiple active sites and key reactive oxygen species2022

    • Author(s)
      Tsutomu Chida, Kousuke Hiromori, Naomi Shibasaki-Kitakawa, Naoki Mimura, Aritomo Yamaguchi, Atsushi Takahashi
    • Organizer
      TOCAT9 (Fukuoka, Japan), Oral
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 廃グリセリンの高付加価値化を目指した選択的酸化プロセスの設計2021

    • Author(s)
      千田勤、廣森浩祐、北川尚美、三村直樹、山口有朋、高橋厚
    • Organizer
      第10回 JACI/GSCシンポジウム
    • Related Report
      2021 Annual Research Report
  • [Presentation] Kinetic model for process design of efficient production of high value-chemicals from glycerol2021

    • Author(s)
      Tsutomu Chida, Kousuke Hiromori, Naomi Shibasaki-Kitakawa, Naoki Mimura, Aritomo Yamaguchi, Atsushi Takahashi
    • Organizer
      2021 AOCS Annual Meeting & Expo
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Efficient conversion of waste glycerol into high value-added chemicals by selective oxidation2021

    • Author(s)
      Tsutomu Chida, Kousuke Hiromori, Naomi Shibasaki-Kitakawa, Naoki Mimura, Aritomo Yamaguchi, Atsushi Takahashi
    • Organizer
      The International Chemical Congress of Pacific Basin Societies 2021
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research

URL: 

Published: 2021-04-28   Modified: 2025-01-30  

Information User Guide FAQ News Terms of Use Attribution of KAKENHI

Powered by NII kakenhi