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CO2 methanation using hydrogen storage alloys at ambient temperature

Research Project

Project/Area Number 19K15683
Research Category

Grant-in-Aid for Early-Career Scientists

Allocation TypeMulti-year Fund
Review Section Basic Section 36020:Energy-related chemistry
Research InstitutionTokai University

Principal Investigator

Gemma Ryota  東海大学, 工学部, 講師 (10803546)

Project Period (FY) 2019-04-01 – 2022-03-31
Project Status Completed (Fiscal Year 2021)
Budget Amount *help
¥2,730,000 (Direct Cost: ¥2,100,000、Indirect Cost: ¥630,000)
Fiscal Year 2021: ¥260,000 (Direct Cost: ¥200,000、Indirect Cost: ¥60,000)
Fiscal Year 2020: ¥1,300,000 (Direct Cost: ¥1,000,000、Indirect Cost: ¥300,000)
Fiscal Year 2019: ¥1,170,000 (Direct Cost: ¥900,000、Indirect Cost: ¥270,000)
KeywordsCO2メタン化 / ボールミリング / メカノケミカル反応 / 水素吸蔵合金 / アトムプローブ / メタン化 / LaNi5
Outline of Research at the Start

大気中二酸化炭素濃度の上昇を緩和する方法の一つとして、大気中CO2のメタン化が注目されている。しかし、これまでに開発されたメタン化プロセスでは、最低でも200℃以上の高温が必要とされているため、省エネルギーの観点から異なるプロセスによる低温化が望ましい。本研究では、水素(H2)とCO2からメタン(CH4)を低温下で合成する方法として、水素吸蔵合金を用いたメカノケミカル反応を利用した合成法について検証し、さらに、反応その場ガス分析と、アトムプローブを活用した合金ナノ組織の詳細な元素分析により、低温下にて有効なメタン生成触媒の探索を目的とする。

Outline of Final Research Achievements

We investigated the CO2 methanation behavior of hydrogen storage alloy powder by ball milling in a hydrogen + carbon dioxide mixed atmosphere. As a result, it was clarified that the behavior that the amount of hydrogen decreases faster than the consumption of carbon dioxide precedes the production of methane. That is, it was found that a part of hydrogen is absorbed in the alloy before methane is generated by the catalytic reaction on the alloy surface. This behavior was quicker when an alloy with a large amount of hydrogen solubility was used. That is, it was suggested that the onset of methanation was promoted by atomic hydrogen supply to the reaction site at the gas/solid interface.

Academic Significance and Societal Importance of the Research Achievements

水素吸蔵合金であるLa-Ni系合金粉末を用いてH2+CO2雰囲気にてボールミリングを行うことにより、メタン生成が可能であることが示された。合金粉末は相分離を生じるが、これに伴い合金中に吸蔵された水素が放出され、この水素の放出とメタン生成の開始に相関があることが示唆された。相分離によりLa酸化物等にNiが担持されたナノ構造をとるが、このままボールミリングを継続した場合でもメタン生成が継続することから、合金粉末は触媒前駆体と見なされることが明らかとなった。また、炭酸化物中の炭素がメタンの原料となりうることが示されたことから、関連する研究を展開する上で、示唆に富む成果が得られたものと考えられる。

Report

(4 results)
  • 2021 Annual Research Report   Final Research Report ( PDF )
  • 2020 Research-status Report
  • 2019 Research-status Report
  • Research Products

    (31 results)

All 2022 2021 2020 2019 Other

All Int'l Joint Research (2 results) Journal Article (4 results) (of which Int'l Joint Research: 2 results,  Peer Reviewed: 4 results) Presentation (24 results) (of which Int'l Joint Research: 8 results,  Invited: 2 results) Remarks (1 results)

  • [Int'l Joint Research] Karlsruhe Institute of Technology (KIT)(ドイツ)

    • Related Report
      2021 Annual Research Report
  • [Int'l Joint Research] Karlsruhe Institute of Technology (KIT)(ドイツ)

    • Related Report
      2019 Research-status Report
  • [Journal Article] Role of atomic hydrogen supply on the onset of CO2 methanation over La?Ni based hydrogen storage alloys studied by in-situ approach2022

    • Author(s)
      Sawahara Keito、Yatagai Kohei、Boll Torben、Pundt Astrid、Gemma Ryota
    • Journal Title

      International Journal of Hydrogen Energy

      Volume: - Issue: 44 Pages: 19051-19061

    • DOI

      10.1016/j.ijhydene.2022.04.089

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] In-situ monitoring of CO<sub>2</sub> methanation: pressure change upon ball-milling of LaNi<sub>5</sub> under CO<sub>2</sub> and H<sub>2</sub>2021

    • Author(s)
      SAWAHARA Keito、GEMMA Ryota
    • Journal Title

      Journal of Advanced Science

      Volume: 33 Issue: 0 Pages: n/a

    • DOI

      10.2978/jsas.33107

    • NAID

      130008077164

    • ISSN
      0915-5651, 1881-3917
    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Mechanochemical CO2 methanation over LaNi-based alloys2020

    • Author(s)
      Kohei Yatagai, Yuto Shishido, Ryota Gemma, Torben Boll, Haruhisa Uchida, Kazuya Oguri
    • Journal Title

      International Journal of Hydrogen Energy

      Volume: 45 Issue: 8 Pages: 5264-5275

    • DOI

      10.1016/j.ijhydene.2019.07.055

    • Related Report
      2019 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Methanation of CO<sub>2</sub> by using LaNi<sub>5</sub> alloy with ball-milling method2019

    • Author(s)
      Kohei YATAGAI, Ryota GEMMA, Haru-Hisa UCHIDA, Kazuya OGURI
    • Journal Title

      Journal of Advanced Science

      Volume: 31 Issue: 0 Pages: n/a

    • DOI

      10.2978/jsas.31101

    • NAID

      130007695542

    • ISSN
      0915-5651, 1881-3917
    • Related Report
      2019 Research-status Report
    • Peer Reviewed
  • [Presentation] Mechanochemical CO2 methanation over LaNi-based alloys2021

    • Author(s)
      Keito Sawahara, Torben Boll, Haru-Hisa Uchida, Kazuya Oguri, Ryota Gemma
    • Organizer
      Thermec'2021 Virtual Conference
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research
  • [Presentation] In-situ monitoring of CO2 methanation: pressure change upon ball-milling of LaNi5 under CO2 and H22021

    • Author(s)
      Keito Sawahara, Kohei Yatagai, Tomochika Hayashi, Shuntaro Nakahiro, Shohei Moriki, Haru-Hisa Uchida, Kazuya Oguri, Ryota Gemma
    • Organizer
      Thermec'2021 Virtual Conference
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Early stages of mechanochemical methanation over La-Ni based alloys2021

    • Author(s)
      Keito Sawahara, Ryota Gemma
    • Organizer
      3rd International Hydrogen Energy Congress and Exhibition (IHEC2021)
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research
  • [Presentation] La-Ni系合金によるメカノケミカルCO2メタネーション2021

    • Author(s)
      澤原 馨登、源馬 龍太
    • Organizer
      2021年第82回応用物理学会秋季学術講演会
    • Related Report
      2021 Annual Research Report
  • [Presentation] LaNi系薄膜上におけるCO2メタン化反応2021

    • Author(s)
      澤本 裕一、中廣 駿太郎、源馬 龍太
    • Organizer
      2021年第82回応用物理学会秋季学術講演会
    • Related Report
      2021 Annual Research Report
  • [Presentation] 水素吸蔵合金を用いたメカノケミカルCO2メタネーションにおける原子状水素供給の影響2021

    • Author(s)
      澤原 馨登、源馬 龍太
    • Organizer
      日本金属学会2021年秋季(第169回)講演大会
    • Related Report
      2021 Annual Research Report
  • [Presentation] La化合物を用いたメカノケミカルCO2メタネーションのin-situ測定2021

    • Author(s)
      澤原 馨登、源馬 龍太
    • Organizer
      33rd '21 SAS Symposium
    • Related Report
      2021 Annual Research Report
  • [Presentation] The Impact of Atomic-H supply for Mechanochemical CO2 Methanation2021

    • Author(s)
      Keito Sawahara, Yuichi Sawamoto, Torben Boll, Ryota Gemma
    • Organizer
      Material Research Meeting (MRM) 2021
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 振動型ボールミルを用いたLaNi5によるCO2メタン化反応のモニタリング2021

    • Author(s)
      澤原 馨登、源馬 龍太
    • Organizer
      東海大学マイクロ・ナノ啓発会【Tμne】第13回学術講演会
    • Related Report
      2020 Research-status Report
  • [Presentation] 振動型ボールミルを用いたLaNi5によるCO2メタン化反応のモニタリング2020

    • Author(s)
      澤原 馨登、源馬 龍太
    • Organizer
      2020年第81回応用物理学会秋季学術講演会
    • Related Report
      2020 Research-status Report
  • [Presentation] スパッタリング法により作製したLa-Ni系合金薄膜上におけるCO2メタン化反応2020

    • Author(s)
      林 諄眞、源馬 龍太、中廣 駿太郎
    • Organizer
      2020年第81回応用物理学会秋季学術講演会
    • Related Report
      2020 Research-status Report
  • [Presentation] TiFe系合金粉末を用いたCO2のメタン化2020

    • Author(s)
      鈴木 琢也、源馬 龍太
    • Organizer
      2020年第81回応用物理学会秋季学術講演会
    • Related Report
      2020 Research-status Report
  • [Presentation] Recent hydrogen storage-related topics and application of hydrogen storage alloys for CO2 methanation reaction2020

    • Author(s)
      Ryota Gemma
    • Organizer
      Tokai University x DTU Joint Energy Seminar -Energy Transitions: Decarbonization of Energy Systems for Sustainable Society: Improving QoL-
    • Related Report
      2020 Research-status Report
  • [Presentation] スパッタリング法により作製したLa-Ni系合金薄膜上におけるCO2メタン化反応2020

    • Author(s)
      林 諄眞、中廣 駿太郎、源馬 龍太
    • Organizer
      32nd '20 SAS Symposium
    • Related Report
      2020 Research-status Report
  • [Presentation] 振動型ボールミルを用いたLaNi5によるCO2メタン化反応のモニタリング2020

    • Author(s)
      澤原 馨登、源馬 龍太
    • Organizer
      32nd '20 SAS Symposium
    • Related Report
      2020 Research-status Report
  • [Presentation] 水素吸蔵合金によるCO2のメタン化と微細組織変化2020

    • Author(s)
      源馬 龍太
    • Organizer
      Tμne第12回学術講演会
    • Related Report
      2019 Research-status Report
  • [Presentation] 振動型ボールミルを用いたLaNi5によるCO2 メタン化反応のモニタリング2019

    • Author(s)
      澤原 馨登、源馬 龍太
    • Organizer
      31st '19 SAS Symposium
    • Related Report
      2019 Research-status Report
  • [Presentation] LaNi5とCO2の反応性2019

    • Author(s)
      森木 翔平、源馬 龍太
    • Organizer
      31st '19 SAS Symposium
    • Related Report
      2019 Research-status Report
  • [Presentation] アトムプローブによる金属中重水素の検出と水素吸蔵材料を用いたCO2のメタン化2019

    • Author(s)
      源馬 龍太
    • Organizer
      カメカテクニカルセミナー2019
    • Related Report
      2019 Research-status Report
    • Invited
  • [Presentation] Impact of CO2 pretreatment on methanation over La-Ni based alloys2019

    • Author(s)
      Kohei Yatagai, Ryota Gemma, Torben Boll, Haruhisa Uchida, Kazuya Oguri
    • Organizer
      Hydrogen-Metal Systems, Gordon Research Conference
    • Related Report
      2019 Research-status Report
    • Int'l Joint Research
  • [Presentation] Mechanochemical CO2 methanation over LaNi-based alloys2019

    • Author(s)
      Ryota Gemma, Kohei Yatagai, Torben Boll, Haruhisa Uchida, Kazuya Oguri
    • Organizer
      Hydrogen-Metal Systems, Gordon Research Conference
    • Related Report
      2019 Research-status Report
    • Int'l Joint Research
  • [Presentation] CO2 methanation over hydrogen storage alloys via mechanical milling -Study by atom probe tomography (APT)-2019

    • Author(s)
      Ryota Gemma
    • Organizer
      Asia Pacific Society for Materials Research (APSMR) 2019 Annual Meeting
    • Related Report
      2019 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Methanation of CO2 by LaNi5 alloy by using ball-milling method2019

    • Author(s)
      Kohei Yatagai, Torben Boll, Haruhisa Uchida, Kazuya Oguri, Ryota Gemma
    • Organizer
      The 8th World Hydrogen Technologies Convention (WHTC 2019)
    • Related Report
      2019 Research-status Report
    • Int'l Joint Research
  • [Presentation] LaNi5を用いたCO2からのメタン生成2019

    • Author(s)
      谷田貝 昂平, 鈴木 琢也, Boll Torben, 内田 晴久, 小栗 和也, 源馬 龍太
    • Organizer
      2019年 希土類討論会
    • Related Report
      2019 Research-status Report
  • [Remarks] Referenced publications

    • URL

      https://www.knmf.kit.edu/publications.php

    • Related Report
      2019 Research-status Report

URL: 

Published: 2019-04-18   Modified: 2023-01-30  

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