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Japan-Thailand co-construction of innovative catalytic process decarbonizing CO2 emitted from industrial processes by capturing carbon and producing synthetic fuel

Research Project

Project/Area Number 23KK0089
Research Category

Fund for the Promotion of Joint International Research (International Collaborative Research)

Allocation TypeMulti-year Fund
Review Section Medium-sized Section 27:Chemical engineering and related fields
Research InstitutionShizuoka University

Principal Investigator

福原 長寿  静岡大学, 工学部, 教授 (30199260)

Co-Investigator(Kenkyū-buntansha) 冨田 靖正  静岡大学, 工学部, 教授 (50303532)
小林 正樹  八戸工業大学, 大学院工学研究科, 教授 (90312678)
河野 芳海  静岡大学, 工学部, 准教授 (50334959)
渡部 綾  静岡大学, 工学部, 准教授 (80548884)
片山 裕美  北九州市立大学, 国際環境工学部, 講師 (30823661)
Project Period (FY) 2023-09-08 – 2026-03-31
Project Status Granted (Fiscal Year 2024)
Budget Amount *help
¥21,060,000 (Direct Cost: ¥16,200,000、Indirect Cost: ¥4,860,000)
Fiscal Year 2025: ¥6,760,000 (Direct Cost: ¥5,200,000、Indirect Cost: ¥1,560,000)
Fiscal Year 2024: ¥8,190,000 (Direct Cost: ¥6,300,000、Indirect Cost: ¥1,890,000)
Fiscal Year 2023: ¥6,110,000 (Direct Cost: ¥4,700,000、Indirect Cost: ¥1,410,000)
KeywordsCO2処理 / メタン化反応 / オートメタネーション / 構造体触媒 / グリーンハウスガス / ドライ改質反応 / 固体炭素 / 合成ガス / CO2削減 / メタネーション / 構造体触媒システム / CO2資源化 / 社会実装 / ドライリフォーミング / 固体炭素捕集
Outline of Research at the Start

本研究では、申請者が発見した室温25℃域で高活性+高選択的にCO2からCH4に大量変換できるオートメタン化技術(通常約300℃での作動温度を室温域へ大幅低温化に成功、世界初の技術)を基軸に、日本とタイ国の参画者が保有する、CH4のドライ改質で合成ガス(H2+CO、C1化学産業の原料)を高効率に製造する技術、合成ガスから固体Cを捕集してプロセスの脱炭素化を図る技術、そして高圧条件下のFischer-Tropsch(FT)反応で合成ガスから合成燃料を製造する技術を融合した反応システムの開発である。各技術とも熱交換と原料処理の革新化を図ることができる構造体触媒システムを採用して構築する。

Outline of Annual Research Achievements

本研究では、CO2を含んだ工業排ガスを触媒変換プロセスで処理し、資源CH4や合成ガスを製造すること、そして合成ガスから固体炭素を連続的に捕集するCCU型触媒反応プロセスを構築するものである。推進においては海外機関(タイ国の大学)と共同し、COP会議で両国が宣言した、CO2削減目標に貢献する触媒反応プロセスの開拓を目指す。今年度の研究実施で以下の成果を得た。
1.構築した触媒変換プロセスは、メタン化反応(第一段階)で供給するH2量を通常の量論比4よりも少なくする(量論比2~3)ことができ、このH2量の減少がプロセス全体の効率性を高めた。
2.第一段階でのH2量の減少は、ドライ改質反応(第二段階)で使用する構造体触媒の改質機能性にプラス効果をもたらし、触媒物性の解析からドライ改質触媒の炭素析出耐性が向上していることがわかった。また、固体炭素捕集プロセス(第三段階)でも第一段階のH2量削減が捕集機能にプラス効果を与え、量論比2~3で最も効率的な捕集率を示した。
3.構築した炭素捕集プロセスに化学工学的な検討を加え、供給したCO2の56%分の炭素を捕集することに成功した。この達成は、本処理技術がCOP会議の約束草案に貢献できる有用な技術の一つになり得ることを示す。
4.上記の知見を踏まえ、タイ国側のCO2処理技術と資源化利用技術に関したワークセッションを日本とタイ国で開催した。その際、タイ国で構築した処理プロセス設備の課題点や改良点について協議し、より実践的な触媒変換プロセス構築への提言を行なった。
5.エクセルギーを指標とした連結型反応プロセス全体のエネルギー効率の評価から、本CO2変換システムが熱力学的に優位性をもつことが判明した。特に、メタン化反応場だけの単独CO2処理技術がエネルギー効率を大きく損なう結果に対し、本連結プロセスでは投入エネルギー以上の効率性を実施できることが判明した。

Current Status of Research Progress
Current Status of Research Progress

1: Research has progressed more than it was originally planned.

Reason

日本側ではメタン化反応場における使用H2量が量論比4以下(2.5が良好)で充分であるとの新しい知見を獲得したことと、固体炭素捕集場における捕集率56%を達成したこと、そしてタイ国側ではCO2の固体炭素化のための大型フロー装置が完成したことが理由である。

Strategy for Future Research Activity

R6年度の実施で得られた知見をもとに、産業排出CO2ガスの資源変換をさらに高効率化する触媒反応プロセスの構築を目指し、以下の項目について研究推進を図る。
1.炭素捕集プロセス(第三段階)に関して、炭素捕集率をさらにアップする(目標:捕集率60%以上)ための反応工学的な要素技術の関連性について検討する。そして、個々の操作パラメータが及ぼす影響を調査し、捕集率と反応操作との学術的な相関性を調査する。
2.メタン化反応プロセス(第一段階)+ドライ改質プロセス(第二段階)の知見から、逆水性ガスシフト反応によるCO2から炭素捕集を実施する連結型触媒プロセスについて検討する。その際、使用するH2量の削減効果に着目し、プロセス全体のエネルギー効率を検討する。
3.2の実施においては、逆水性ガスシフト反応のための構造体触媒(スパイラル形)を開発する。金属基材上へ析出させる触媒成分はCu系を基本とし、簡便で機能的な触媒調製を可能とするelectroless plating法を用いて検討する。
4.タイ国側で完成した大型フロー装置の稼働性の健全化を図りつつ、CO2からの固体炭素捕集に関する実測データの集積と、捕集炭素の機能性材料としての活用法について現地訪問やオンライン会議によって検討する。
5.構造体触媒の高機能性について、数値シミュレーションによる流体力学解析をさらに駆使して検討する。その際、メタン化反応場を対象としつつ、スワール流れの効果と触媒反応速度の促進効果との相関性に着目した検討を実施する。

Report

(2 results)
  • 2024 Research-status Report
  • 2023 Research-status Report
  • Research Products

    (43 results)

All 2025 2024 2023 Other

All Int'l Joint Research (2 results) Journal Article (19 results) (of which Int'l Joint Research: 8 results,  Peer Reviewed: 19 results,  Open Access: 18 results) Presentation (15 results) (of which Int'l Joint Research: 14 results,  Invited: 4 results) Book (1 results) Patent(Industrial Property Rights) (5 results) Funded Workshop (1 results)

  • [Int'l Joint Research] Mahidol University/Chulalongkorn University/King Mongkut's Institute of Technology(タイ)

    • Related Report
      2024 Research-status Report
  • [Int'l Joint Research] Indian Institute of Technology Delhi(インド)

    • Related Report
      2024 Research-status Report
  • [Journal Article] Multi-stage spiral-type structured catalyst system for direct large-scale methanation of industrial CO2 emissions: a feasibility study2025

    • Author(s)
      Akama Hiroshi、Watanabe Ryo、Verma Priyanka、Fukuhara Choji
    • Journal Title

      Reaction Chemistry & Engineering

      Volume: - Issue: 7 Pages: 1527-1538

    • DOI

      10.1039/d4re00606b

    • Related Report
      2024 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] A novel process of triple-passed CO2 methanation over gradient-coated spiral-structured Ni/CeO2 catalysts2025

    • Author(s)
      Suriya Porapak、Srifa Atthapon、Koo-Amornpattana Wanida、Kim-Lohsoontorn Pattaraporn、Assabumrungrat Suttichai、Fukuhara Choji、Ratchahat Sakhon
    • Journal Title

      Scientific Reports

      Volume: 15 Issue: 1

    • DOI

      10.1038/s41598-025-94262-0

    • Related Report
      2024 Research-status Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Fabrication of spiral-structured Ni-Ce catalyst supported on natural kaolin-derived metakaolin for CO2 methanation2025

    • Author(s)
      Suriya Porapak、Srifa Atthapon、Koo-Amornpattana Wanida、Watcharasing Sunisa、Charinpanitkul Tawatchai、Assabumrungrat Suttichai、Fukuhara Choji、Sano Noriaki、Ratchahat Sakhon
    • Journal Title

      International Journal of Hydrogen Energy

      Volume: 103 Pages: 513-527

    • DOI

      10.1016/j.ijhydene.2025.01.271

    • Related Report
      2024 Research-status Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Visible light-enhanced synergistic catalysis of AuCu nanostructures immobilized within porous support2025

    • Author(s)
      Ajay、Jaipal Heeralal、Watanabe Ryo、Fukuhara Choji、Verma Priyanka
    • Journal Title

      Journal of Chemical Sciences

      Volume: 137 Issue: 1

    • DOI

      10.1007/s12039-025-02356-z

    • Related Report
      2024 Research-status Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Electric heating system for iso-C5 dehydrogenation in the presence of H2S2025

    • Author(s)
      Suganuma Hiroyasu、Watanabe Ryo、Verma Priyanka、Akama Hiroshi、Fukuhara Choji
    • Journal Title

      Chemistry Letters

      Volume: 54 Issue: 1

    • DOI

      10.1093/chemle/upae228

    • Related Report
      2024 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Utilization Technology of Hydrogen: Methanation2024

    • Author(s)
      福原 長寿
    • Journal Title

      Nihon Enerugii Gakkai Kikanshi Enermix

      Volume: 103 Issue: 3 Pages: 363-369

    • DOI

      10.20550/jieenermix.103.3_363

    • ISSN
      2432-3586, 2432-3594
    • Year and Date
      2024-05-20
    • Related Report
      2024 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Deactivation of an Fe-based catalyst in the dehydrogenation of light alkanes under H2S co-feeding: A case study2024

    • Author(s)
      Watanabe Ryo、Suganuma Hiroyasu、Yoda Yuta、Karasawa Fumiya、Verma Priyanka、Fukuhara Choji
    • Journal Title

      Applied Catalysis A: General

      Volume: 683 Pages: 119848-119848

    • DOI

      10.1016/j.apcata.2024.119848

    • Related Report
      2024 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Steam reforming of aromatics mixture as a model tar over Ni/Al2O3 structured catalyst2024

    • Author(s)
      Watanabe Ryo、Tanabe Takuya、Fushimi Yuya、Verma Priyanka、Fukuhara Choji
    • Journal Title

      New Journal of Chemistry

      Volume: 48 Issue: 18 Pages: 8213-8221

    • DOI

      10.1039/d4nj00856a

    • Related Report
      2024 Research-status Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Scalable one-step synthesis of reduced graphene oxide: Towards flexible transparent conductive films and active supercapacitor electrodes2024

    • Author(s)
      Yao Fangbo、Li Wenruo、SKS Saravana Karthikeyan、Fukuhara Choji、Badhulika Sushmee、Kong Chang Yi
    • Journal Title

      Chemical Engineering Journal

      Volume: 488 Pages: 150828-150828

    • DOI

      10.1016/j.cej.2024.150828

    • Related Report
      2023 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Effect of H2 S co-feeding on the performance of the Fe/SiO2 catalyst for isomerization and dehydrogenation of C5-monoolefin2024

    • Author(s)
      Karasawa Fumiya、Watanabe Ryo、Verma Priyanka、Miyagi Yuichi、Yamada Hikaru、Miyanari Setsuko、Fukuhara Choji
    • Journal Title

      New Journal of Chemistry

      Volume: 48 Issue: 8 Pages: 3357-3363

    • DOI

      10.1039/d3nj04923j

    • Related Report
      2023 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Influence of sulfur contamination on ethylene aromatization over a Ga-modified MFI-type zeolite2024

    • Author(s)
      Oshima Kazumasa、Konishi Eriko、Watanabe Ryo、Fukuhara Choji、Kishida Masahiro
    • Journal Title

      Chemical Engineering Journal

      Volume: 480 Pages: 148241-148241

    • DOI

      10.1016/j.cej.2023.148241

    • Related Report
      2023 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Plasmonic Heterojunction Photocatalysts for Hydrogen Generation: A Mini-Review2023

    • Author(s)
      Verma Priyanka、Kuwahara Yasutaka、Mori Kohsuke、Watanabe Ryo、Fukuhara Choji、Yamashita Hiromi
    • Journal Title

      Energy & Fuels

      Volume: 37 Issue: 23 Pages: 17652-17666

    • DOI

      10.1021/acs.energyfuels.3c02341

    • Related Report
      2023 Research-status Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] One-Step Synthesis of Fragment-Reduced Graphene Oxide as an Electrode Material for Supercapacitors2023

    • Author(s)
      Yao Fangbo、Li Wenruo、Khainunni Shabrina、Ma Jiaojiao、Fukuhara Choji、Kong Chang Yi
    • Journal Title

      ACS Applied Materials & Interfaces

      Volume: 15 Issue: 36 Pages: 42424-42438

    • DOI

      10.1021/acsami.3c05764

    • Related Report
      2023 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Effect of Ga substitution with Al in ZSM-5 zeolite in methanethiol-to-hydrocarbon conversion2023

    • Author(s)
      Watanabe Ryo、Oba Natsu、Smith Suchada、Oshima Kazumasa、Kishida Masahiro、Miyake Koji、Nishiyama Norikazu、Verma Priyanka、Fukuhara Choji
    • Journal Title

      RSC Advances

      Volume: 13 Issue: 31 Pages: 21441-21447

    • DOI

      10.1039/d3ra01852k

    • Related Report
      2023 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Electric-Field-Assisted Catalytic Methanethiol Decomposition Using Pt/CeO2 Catalyst2023

    • Author(s)
      Oshima Kazumasa、Watanabe Ryo、Fukuhara Choji、Kishida Masahiro
    • Journal Title

      Catalysis Letters

      Volume: 154 Issue: 4 Pages: 1398-1403

    • DOI

      10.1007/s10562-023-04416-w

    • Related Report
      2023 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Ethylene Production via Thermal Coupling of Methanethiol2023

    • Author(s)
      Watanabe Ryo、Oba Natsu、Kakuno Itsuki、Smith Suchada、Oshima Kazumasa、Kishida Masahiro、Verma Priyanka、Fukuhara Choji
    • Journal Title

      Chemistry Letters

      Volume: 52 Issue: 8 Pages: 661-664

    • DOI

      10.1246/cl.230228

    • Related Report
      2023 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Performance Intensification of CO2 Methanation by Co-Feeding Oxygen Over Various Ru-Based Catalysts2023

    • Author(s)
      Fukuhara Choji、Hirata Nozomu、Ozaki Ren、Watanabe Ryo
    • Journal Title

      Journal of Chemical Engineering of Japan

      Volume: 56 Issue: 1 Pages: 1-12

    • DOI

      10.1080/00219592.2023.2194327

    • Related Report
      2023 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Synthesis of 2,5-dimethylhexene by isobutene dimerization with H2S co-feeding2023

    • Author(s)
      Ryo Watanabe, Riku Tanikawa, Arisa Kurosaki, Kazumasa Oshima, Masahiro Kishida, Priyanka Verma, Choji Fukuhara
    • Journal Title

      RSC Advances

      Volume: 13 Issue: 21 Pages: 14097-14101

    • DOI

      10.1039/d3ra01324c

    • Related Report
      2023 Research-status Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] AuxPdy‐based Heterogeneous Nanocatalysts for Plasmon‐mediated Enhanced Catalysis under Visible Light Irradiation2023

    • Author(s)
      Verma Priyanka, Mhembere Panashe M., Tallone Paolo, Manzoli Maela, Cerrato Giuseppina, Watanabe Ryo, Fukuhara Choji, Raja Robert, Yamashita Hiromi
    • Journal Title

      ChemNanoMat

      Volume: 00 Issue: 6 Pages: 1-9

    • DOI

      10.1002/cnma.202300053

    • Related Report
      2023 Research-status Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Presentation] Multi-stage structured catalyst system for converting GHG (CO2) to useful materials2024

    • Author(s)
      Choji Fukuhara, Hiroshi Akama, Yuki Yamada, Ryo Watanabe
    • Organizer
      Canadian Chemical Engineering Conference (CSChE 2024)
    • Related Report
      2024 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Novel alkane dehydrogenation system with high selectivity of C5 olefins controlling by electrical heating2024

    • Author(s)
      Ryo Watanabe, Choji Fukuhara
    • Organizer
      Canadian Chemical Engineering Conference (CSChE 2024)
    • Related Report
      2024 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Innovative catalytic reaction system converting greenhouse gas: Multi-stage structured catalyst system for CCUS2024

    • Author(s)
      Choji Fukuhara, Hiroto Naiki, Hiroshi Akama, Ryo Watanabe
    • Organizer
      27th Canadian Symposium on Catalysis
    • Related Report
      2024 Research-status Report
    • Int'l Joint Research
  • [Presentation] Acceleration of low alkane (C4, C5) dehydrogenation by lattice S2- species of iron sulfide catalyst2024

    • Author(s)
      Ryo Watanabe, Hiroshi Akama, Priyanka Verma, Choji Fukuhara
    • Organizer
      27th Canadian Symposium on Catalysis
    • Related Report
      2024 Research-status Report
    • Int'l Joint Research
  • [Presentation] Multi-stage structured-catalyst system for post-treatment of Greenhouse Gas emitted from industrial process2024

    • Author(s)
      Choji Fukuhara, Hiroto Naiki, Hiroshi Akama, Ryo Watanabe
    • Organizer
      18th International Congress on Catalysis
    • Related Report
      2024 Research-status Report
    • Int'l Joint Research
  • [Presentation] Acceleration of low-alkane (C4, C5) dehydrogenation by lattice S2- species of iron sulfide catalyst2024

    • Author(s)
      Ryo Watanabe, Fumiya Karasawa, Priyanka Verma, Choji Fukuhara
    • Organizer
      18th International Congress on Catalysis
    • Related Report
      2024 Research-status Report
    • Int'l Joint Research
  • [Presentation] Performance intensification of CO2 methanation by co-feeding oxygen over various Ru-based catalysts2024

    • Author(s)
      福原長寿、平田 望、尾崎 練、渡部 綾
    • Organizer
      化学工学会第55回秋季大会
    • Related Report
      2024 Research-status Report
    • Invited
  • [Presentation] A powerful CO2 methanation system by electrically heating spiral-type structured catalyst2024

    • Author(s)
      Ryo Watanabe, Kohki Nishide, Hiroshi Akama, Choji Fukuhara
    • Organizer
      SCEJ 90th Annual Meeting
    • Related Report
      2024 Research-status Report
    • Int'l Joint Research
  • [Presentation] Advantage of Ni-Cu structured catalyst prepared by electroless plating for CH4 decomposition to produce H22024

    • Author(s)
      Rasaili Prithvi, Hiroshi Akama, Ryo Watanabe, Choji Fukuhara
    • Organizer
      SCEJ 90th Annual Meeting
    • Related Report
      2024 Research-status Report
    • Int'l Joint Research
  • [Presentation] Innovative Catalytic Reaction System Converting Greenhouse Gas (GHG) Emitted from Industrial Process2023

    • Author(s)
      Choji Fukuhara, Hiroshi Akama et al.
    • Organizer
      ASCON-IEEChE2023
    • Related Report
      2023 Research-status Report
    • Int'l Joint Research
  • [Presentation] Innovative Catalytic Reaction System Contributing to Reduce and Utilize Greenhouse Gas (GHG)2023

    • Author(s)
      Choji Fukuhara, Ryo Watanabe et al.
    • Organizer
      20th Asian Pacific Confederation of Chemical Engineering
    • Related Report
      2023 Research-status Report
    • Int'l Joint Research
  • [Presentation] Innovative Chemical Reaction System Contributing to Reduce and Utilize Greenhouse Gas (GHG)2023

    • Author(s)
      Choji Fukuhara, Hiroto Niki et al.
    • Organizer
      27th International Symposium of Chemical Reaction Engineering, Canada 2023
    • Related Report
      2023 Research-status Report
    • Int'l Joint Research
  • [Presentation] C4,C5-Alkane Dehydrogenation Utilizing Lattice 2-Species of Metal Sulfide Catalyst2023

    • Author(s)
      Ryo Watanabe, Choji Fukuhara et al.
    • Organizer
      27th International Symposium of Chemical Reaction Engineering, Canada 2023
    • Related Report
      2023 Research-status Report
    • Int'l Joint Research
  • [Presentation] Performance intensification of converting greenhouse gas (GHG) by auto-methanation with structured catalyst system: A novel transforming route of methanation2023

    • Author(s)
      Choji Fukuhara, Ryo Watanabe et al.
    • Organizer
      11th World Congress of Chemical Engineering
    • Related Report
      2023 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Redox dehydrogenation of propane utilizing lattice S2- in metal sulfide catalyst2023

    • Author(s)
      Ryo Watanabe, Choji Fukuhara et al.
    • Organizer
      11th World Congress of Chemical Engineering
    • Related Report
      2023 Research-status Report
    • Int'l Joint Research
  • [Book] メタンと二酸化炭素 ~その触媒的化学変換技術の現状と展望~2023

    • Author(s)
      福原長寿
    • Total Pages
      442
    • Publisher
      シーエムシー・リサーチ
    • ISBN
      9784910581361
    • Related Report
      2023 Research-status Report
  • [Patent(Industrial Property Rights)] メタンを含むガスを製造する方法、及び反応装置2025

    • Inventor(s)
      福原長寿,赤間 弘,渡部 綾
    • Industrial Property Rights Holder
      福原長寿,赤間 弘,渡部 綾
    • Industrial Property Rights Type
      特許
    • Industrial Property Number
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Published: 2023-09-12   Modified: 2025-12-26  

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