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Molecular Science of Methanol Synthesis by CO2 Hydrogenation using Zirconia-Based Catalysts

Research Project

Project/Area Number 21K04988
Research Category

Grant-in-Aid for Scientific Research (C)

Allocation TypeMulti-year Fund
Section一般
Review Section Basic Section 32010:Fundamental physical chemistry-related
Research InstitutionIbaraki University

Principal Investigator

Joutsuka Tatsuya  茨城大学, 理工学研究科(工学野), 講師 (70823003)

Co-Investigator(Kenkyū-buntansha) 多田 昌平  北海道大学, 工学研究院, 助教 (60769941)
Project Period (FY) 2021-04-01 – 2024-03-31
Project Status Completed (Fiscal Year 2023)
Budget Amount *help
¥4,160,000 (Direct Cost: ¥3,200,000、Indirect Cost: ¥960,000)
Fiscal Year 2023: ¥260,000 (Direct Cost: ¥200,000、Indirect Cost: ¥60,000)
Fiscal Year 2022: ¥1,430,000 (Direct Cost: ¥1,100,000、Indirect Cost: ¥330,000)
Fiscal Year 2021: ¥2,470,000 (Direct Cost: ¥1,900,000、Indirect Cost: ¥570,000)
Keywords第一原理計算 / 触媒 / CO2 / 分子動力学シミュレーション / 表面 / 固溶体触媒 / 界面 / 水素化 / ジルコニア
Outline of Research at the Start

CO2の再資源化を目的として、ジルコニア系触媒を用いたCO2水素化によるメタノール合成が注目を集めている。本研究では、ジルコニア系触媒による触媒反応における分子科学を電子状態計算により明らかにし触媒活性との相関を解明する。そして、ジルコニア系触媒を用いたCO2水素化反応を題材とし、constrained density functional theory (CDFT)法などの触媒反応の理論的解析手法の更なる開発と応用の開拓を目指す。

Outline of Final Research Achievements

CO2 is a greenhouse gas that adversely affects climate change and ocean acidification; as a CO2 recycling technology, methanol synthesis by CO2 hydrogenation is attracting attention, and zirconia-based catalysts in particular show high activity and selectivity. In this study, we investigated the CO2 hydrogenation reaction using zirconia-based catalysts from both molecular science and experimental approaches using first-principles DFT calculations, with the aim of developing high-performance catalysts. Specifically, the adsorption energy and reaction mechanism were analyzed considering the effects of hydroxy groups, amorphous nature, and metal clusters on the catalyst surface; in the ZnZrOx solid solution catalyst, Zn species were found to decompose H2 and Zr species to activate CO2, while Cu nanoparticle formation and InZrOx catalyzed methane byproduct reactions were also elucidated.

Academic Significance and Societal Importance of the Research Achievements

パリ協定が掲げる2℃シナリオに沿ってカーボンサイクルの実現に向けた研究開発が世界的に進んでいる。要となる技術がCO2の再資源化であり、本研究はジルコニア系触媒をターゲットとしている。この触媒系は高いメタノール選択性により世界中で研究競争が続いており、理論計算による検討も活発になってきている。本研究では、今までの理論計算にて軽視されてきたヒドロキシ基などの反応への寄与を計算により明らかにした。また、計算量の多さから敬遠されてきたアモルファス表面上での反応にも解明した。特に、ZnZrOxやInZrOxなどの固溶体触媒表面での反応機構が明らかになったため、今後これらの触媒の更なる応用が期待される。

Report

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

    (32 results)

All 2024 2023 2022 2021 Other

All Journal Article (10 results) (of which Int'l Joint Research: 1 results,  Open Access: 2 results,  Peer Reviewed: 3 results) Presentation (19 results) (of which Int'l Joint Research: 5 results,  Invited: 6 results) Remarks (3 results)

  • [Journal Article] Difference in reaction mechanism between ZnZrO<sub><i>x</i></sub> and InZrO<sub><i>x</i></sub> for CO<sub>2</sub> hydrogenation2024

    • Author(s)
      Tada Shohei、Ogura Yurika、Sato Motohiro、Yoshida Akihiro、Honma Tetsuo、Nishijima Masahiko、Joutsuka Tatsuya、Kikuchi Ryuji
    • Journal Title

      Physical Chemistry Chemical Physics

      Volume: 26 Issue: 18 Pages: 14037-14045

    • DOI

      10.1039/d4cp00635f

    • Related Report
      2023 Annual Research Report
    • Open Access
  • [Journal Article] Oxide Solid?Solution Catalysts with Good Redox Properties for Liquid?Phase Aerobic Additive?Free Oxidation: A Review2024

    • Author(s)
      Tada Shohei、Kondo Masaru、Joutsuka Tatsuya
    • Journal Title

      ChemCatChem

      Volume: - Issue: 12

    • DOI

      10.1002/cctc.202301367

    • Related Report
      2023 Annual Research Report
  • [Journal Article] Neutron crystallography and quantum chemical analysis of bilin reductase PcyA mutants reveal substrate and catalytic residue protonation states2023

    • Author(s)
      Joutsuka Tatsuya、Nanasawa Ryota、Igarashi Keisuke、Horie Kazuki、Sugishima Masakazu、Hagiwara Yoshinori、Wada Kei、Fukuyama Keiichi、Yano Naomine、Mori Seiji、Ostermann Andreas、Kusaka Katsuhiro、Unno Masaki
    • Journal Title

      Journal of Biological Chemistry

      Volume: 299 Issue: 1 Pages: 102763-102763

    • DOI

      10.1016/j.jbc.2022.102763

    • Related Report
      2022 Research-status Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Catalysis of surface dispersed Cu2+ species on t-ZrO2: square-planar Cu catalyzed cross-coupling of arylboronic acid and imidazole2023

    • Author(s)
      Kondo Masaru、Joutsuka Tatsuya、Fujiwara Kakeru、Honma Tetsuo、Nishijima Masahiko、Tada Shohei
    • Journal Title

      Catalysis Science &amp; Technology

      Volume: 13 Issue: 7 Pages: 2247-2254

    • DOI

      10.1039/d3cy00024a

    • Related Report
      2022 Research-status Report
  • [Journal Article] Study of Cu-growth feature by selective low-pressure chemical vapor deposition using a CuI precursor2023

    • Author(s)
      Toyoda Gento、Kikuchi Hikari、Yamauchi Satoshi、Joutsuka Tatsuya、Fuse Takashi、Kubota Yusuke
    • Journal Title

      Japanese Journal of Applied Physics

      Volume: 62 Issue: SH Pages: SH1002-SH1002

    • DOI

      10.35848/1347-4065/acc257

    • Related Report
      2022 Research-status Report
    • Peer Reviewed
  • [Journal Article] Adsorption of CO2 on Amorphous and Crystalline Zirconia: A DFT and Experimental Study2023

    • Author(s)
      Joutsuka Tatsuya、Tada Shohei
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 127 Issue: 14 Pages: 6998-7008

    • DOI

      10.1021/acs.jpcc.3c01185

    • Related Report
      2022 Research-status Report
  • [Journal Article] Active Sites on ZnxZr1-xO2-x Solid Solution Catalysts for CO2-to-Methanol Hydrogenation2022

    • Author(s)
      Tada Shohei、Ochiai Nagomu、Kinoshita Hiroka、Yoshida Mitsuhiro、Shimada Natsumi、Joutsuka Tatsuya、Nishijima Masahiko、Honma Tetsuo、Yamauchi Noriko、Kobayashi Yoshio、Iyoki Kenta
    • Journal Title

      ACS Catalysis

      Volume: 12 Issue: 13 Pages: 7748-7759

    • DOI

      10.1021/acscatal.2c01996

    • Related Report
      2022 Research-status Report
  • [Journal Article] Molecular Mechanism of Autodissociation in Liquid Water: Ab Initio Molecular Dynamics Simulations2022

    • Author(s)
      Joutsuka Tatsuya
    • Journal Title

      The Journal of Physical Chemistry B

      Volume: 126 Issue: 24 Pages: 4565-4571

    • DOI

      10.1021/acs.jpcb.2c01971

    • Related Report
      2022 Research-status Report
  • [Journal Article] Understanding the structure of Cu-doped MgAl2O4 for CO2 hydrogenation catalyst precursor using experimental and computational approaches2022

    • Author(s)
      Joutsuka Tatsuya、Hamamura Ryu、Fujiwara Kakeru、Honma Tetsuo、Nishijima Masahiko、Tada Shohei
    • Journal Title

      International Journal of Hydrogen Energy

      Volume: 47 Issue: 50 Pages: 21369-21374

    • DOI

      10.1016/j.ijhydene.2022.04.295

    • Related Report
      2022 Research-status Report
  • [Journal Article] Efficient Free-Energy Calculation of Proton Transfer by Constrained Density Functional Theory and Geometrically Restrained Molecular Dynamics Simulation2021

    • Author(s)
      Joutsuka Tatsuya、Ando Koji
    • Journal Title

      Chemistry Letters

      Volume: - Issue: 7 Pages: 1325-1328

    • DOI

      10.1246/cl.210132

    • NAID

      130008065512

    • Related Report
      2021 Research-status Report
    • Peer Reviewed
  • [Presentation] t-ZrO2中の固溶Cu種を活性種としたイミダゾールとフェニルボロン酸のカップリング反応2024

    • Author(s)
      多田昌平、近藤健、城塚達也、藤原翔、本間徹生、西嶋雅彦
    • Organizer
      第133回触媒討論会
    • Related Report
      2023 Annual Research Report
  • [Presentation] Cu-Zr酸化物固溶体触媒を用いたカップリング反応の開拓2024

    • Author(s)
      多田昌平、近藤健、城塚達也
    • Organizer
      化学系学協会北海道支部2024年冬季研究発表会
    • Related Report
      2023 Annual Research Report
  • [Presentation] ゼオライトを用いたメタノールからオレフィンへの変換性能のDFT計算と機械学習による研究2023

    • Author(s)
      猪爪尚輝、城塚達也
    • Organizer
      第34回 日本化学会関東支部 茨城地区研究交流会
    • Related Report
      2023 Annual Research Report
  • [Presentation] CO2水素化によるメタノール合成用ジルコニア系触媒のDFT計算と触媒探索2023

    • Author(s)
      城塚達也、近藤健、多田昌平
    • Organizer
      第132回触媒討論会
    • Related Report
      2023 Annual Research Report
  • [Presentation] t-ZrO2中の固溶Cu2+種を活性種としたイミダゾールとフェニルボロン酸のカップリング反応2023

    • Author(s)
      多田昌平、近藤健、城塚達也、藤原翔、本間徹生、西嶋雅彦
    • Organizer
      化学工学会 第54回秋季大会
    • Related Report
      2023 Annual Research Report
  • [Presentation] DFT Calculations and Catalyst Exploration of Zirconia-Based Catalysts for Methanol Synthesis by CO2 Hydrogenation2023

    • Author(s)
      Tatsuya Joutsuka
    • Organizer
      The Fifth Asian Workshop of Experiment and Theory in Quantum Beam Molecular Sciences
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] ビリン還元酵素PcyA-ビリベルジンⅨα複合体の計算科学的研究2023

    • Author(s)
      萬代充裕、飯島愛璃、圷優佳、海野昌喜、城塚達也、森聖治
    • Organizer
      スーパーコンピュータワークショップ2022
    • Related Report
      2022 Research-status Report
  • [Presentation] CO2 Hydrogenation to Methanol by Zirconia Solid Solution: Theoretical Analysis by Ab Initio Calculations2022

    • Author(s)
      Tatsuya Joutsuka
    • Organizer
      7th International Symposium of Quantum Beam Science at Ibaraki University
    • Related Report
      2022 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] DFT Study of Surface Structure of Solid Solution Catalyst ZnxZr1-xO2-x for CO2-to-methanol hydrogenation2022

    • Author(s)
      Mitsuhiro Yoshida, Tatsuya Joutsuka, Shohei Tada
    • Organizer
      TOCAT9
    • Related Report
      2022 Research-status Report
    • Int'l Joint Research
  • [Presentation] メタノール合成触媒ZnxZr1-xO2-xの活性点構造の解明2022

    • Author(s)
      多田 昌平、落合 和、吉田 光宏、城塚 達也
    • Organizer
      第130回触媒討論会
    • Related Report
      2022 Research-status Report
  • [Presentation] CO2水素化反応からのメタノール合成用亜鉛ジルコニア触媒のDFT計算による表面構造の解析2022

    • Author(s)
      吉田光宏、城塚達也、多田昌平
    • Organizer
      石油学会第64回年会
    • Related Report
      2022 Research-status Report
  • [Presentation] Constrained DFT計算による凝縮相中における電荷移動反応の解析2022

    • Author(s)
      城塚達也
    • Organizer
      凝縮系の理論化学2022
    • Related Report
      2021 Research-status Report
    • Invited
  • [Presentation] Understanding Charge-Transfer Reactions by Constrained Density Functional Theory2022

    • Author(s)
      Tatsuya Joutsuka
    • Organizer
      日本化学会 第101春季年会 アジア国際シンポジウム
    • Related Report
      2021 Research-status Report
    • Invited
  • [Presentation] DFT Study of Solid Solution Catalyst ZnxZr1-xO2-x for Methanol Synthesis via CO2 Hydrogenation2021

    • Author(s)
      Mitsuhiro Yoshida, Tatsuya Joutsuka, Shohei Tada
    • Organizer
      17th International Student Conference at Ibaraki
    • Related Report
      2021 Research-status Report
    • Int'l Joint Research
  • [Presentation] 電子状態計算によるアナターゼ型TiO2における光触媒活性の解析2021

    • Author(s)
      吉成啓人、城塚達也
    • Organizer
      第21回 大つくば物理化学セミナー
    • Related Report
      2021 Research-status Report
  • [Presentation] Theoretical Study of Charge-Transfer Reactions by Constrained Density Functional Theory2021

    • Author(s)
      Tatsuya Joutsuka
    • Organizer
      Sakura Science Workshop at Ibaraki University 2021 (SSWIU2021)
    • Related Report
      2021 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Theoretical Study of Charge-Transfer Reactions in TiO2 Photocatalysis2021

    • Author(s)
      城塚達也
    • Organizer
      化学系学協会東北大会
    • Related Report
      2021 Research-status Report
    • Invited
  • [Presentation] 酸化チタンにおける光触媒活性:Constrained DFT法による解析2021

    • Author(s)
      吉成啓人、城塚達也
    • Organizer
      第15回分子科学討論会
    • Related Report
      2021 Research-status Report
  • [Presentation] 電子状態計算によるアナターゼ型酸化チタンにおける光触媒活性の解析2021

    • Author(s)
      吉成啓人、城塚達也
    • Organizer
      第23回理論化学討論会
    • Related Report
      2021 Research-status Report
  • [Remarks] 所属機関が作成したwebページ

    • URL

      https://info.ibaraki.ac.jp/Profiles/104/0010400/profile.html

    • Related Report
      2022 Research-status Report 2021 Research-status Report
  • [Remarks] 個人ページ

    • URL

      https://sites.google.com/view/theorchem/

    • Related Report
      2022 Research-status Report
  • [Remarks] 個人ページ

    • URL

      https://sites.google.com/view/theorchem/publications

    • Related Report
      2021 Research-status Report

URL: 

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

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