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Novel Catalytic Process based on the hydrogen spillover phenomena

Planned Research

Project AreaSurface hydrogen engineering: Utilization of spillover hydrogen and verification of quantum tunneling effect
Project/Area Number 21H05099
Research Category

Grant-in-Aid for Transformative Research Areas (B)

Allocation TypeSingle-year Grants
Review Section Transformative Research Areas, Section (II)
Research InstitutionYokohama National University

Principal Investigator

Motokura Ken  横浜国立大学, 大学院工学研究院, 教授 (90444067)

Co-Investigator(Kenkyū-buntansha) 荻原 仁志  埼玉大学, 理工学研究科, 教授 (60452009)
Project Period (FY) 2021-08-23 – 2024-03-31
Project Status Completed (Fiscal Year 2023)
Budget Amount *help
¥34,060,000 (Direct Cost: ¥26,200,000、Indirect Cost: ¥7,860,000)
Fiscal Year 2023: ¥11,310,000 (Direct Cost: ¥8,700,000、Indirect Cost: ¥2,610,000)
Fiscal Year 2022: ¥10,400,000 (Direct Cost: ¥8,000,000、Indirect Cost: ¥2,400,000)
Fiscal Year 2021: ¥12,350,000 (Direct Cost: ¥9,500,000、Indirect Cost: ¥2,850,000)
Keywords固体酸触媒 / 担持金属触媒 / 水素スピルオーバー / 還元反応 / 酸化反応 / 固体触媒 / 固定化触媒 / 水素化 / C-H活性化 / 水素移動反応 / アルキル化反応
Outline of Research at the Start

触媒分野では水素スピルオーバー現象が古くから知られており、これを利用した触媒設計が行われている。本申請課題では、最新の触媒設計手法・原子分子レベル構造解析手法と水素スピルオーバー現象を組み合わせ、スピルオーバー水素を使いこなすための革新的触媒の開発を目的とし、i) 精密設計固体表面での水素スピルオーバーによる高選択的官能基変換、ii) 高速水素スピルオーバーを利用した高選択的連続反応、および iii) 水素の逆スピルオーバー現象によるC-H結合活性化・平衡制約回避、を実現するための新規触媒開発に取り組む。

Outline of Final Research Achievements

Several catalytic reaction systems for dehydrogenative/hydrogenative reaction accelerated by hydrogen spillover were developed. For example, palladium nanoparticles immobilized on outer surface of zeolite was prepared, and acted as a highly active catalysts for direct aromatic alkylation with alkanes through hydrogen transfer between acid site and Pd nanoparticles. In addition, CO2 hydrogenation reaction with active Si-H species on silicon surface and novel bimetallic nanoparticles formed via hydrogen spillover process were reported.

Academic Significance and Societal Importance of the Research Achievements

水素スピルオーバーとは、固体表面を活性な水素種が高速で移動する現象を指す。固体表面で進行する触媒反応は、水素スピルーバー現象を活用することで大幅に促進される。例えば、アルカンとベンゼンの脱水素カップリング反応では、酸点でアルカンから引き抜かれた水素種が触媒表面を高速で拡散し、金属粒子表面で再結合して水素分子となる。本研究ではこの反応経路に基づいて、酸点とパラジウムナノ粒子が共存する触媒を開発し、脱水素カップリング反応に活用した。これらの成果は、高効率な物質生産に寄与するだけでなく、これまでブラックボックスとされてきた触媒反応に寄与する水素種の挙動を明らかにした点で重要な成果である。

Report

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

    (46 results)

All 2024 2023 2022 2021 Other

All Int'l Joint Research (1 results) Journal Article (16 results) (of which Int'l Joint Research: 3 results,  Peer Reviewed: 16 results,  Open Access: 6 results) Presentation (25 results) (of which Int'l Joint Research: 8 results,  Invited: 6 results) Book (3 results) Remarks (1 results)

  • [Int'l Joint Research] European XFEL(ドイツ)

    • Related Report
      2023 Annual Research Report
  • [Journal Article] Direct alkylation of benzene with branched alkanes using solid acids: Unexpected product selectivity based on the tertiary carbon position2024

    • Author(s)
      Motokura Ken、Nakamura Yukina、Takabatake Moe、Suzuki Kenta、Hasegawa Shingo
    • Journal Title

      Catalysis Today

      Volume: 425 Pages: 114363-114363

    • DOI

      10.1016/j.cattod.2023.114363

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Interparticle Hydrogen Spillover in Enhanced Catalytic Reactions2024

    • Author(s)
      Motokura Ken
    • Journal Title

      Chemistry An Asian Journal

      Volume: - Issue: 16

    • DOI

      10.1002/asia.202301083

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Pd Nanoparticles on the Outer Surface of Microporous Aluminosilicates for the Direct Alkylation of Benzenes using Alkanes2023

    • Author(s)
      Misaki Satoshi、Ariga-Miwa Hiroko、Ito Takashi U.、Yoshida Takefumi、Hasegawa Shingo、Nakamura Yukina、Tokutake Shunta、Takabatake Moe、Shimomura Koichiro、Chun Wang-Jae、Manaka Yuichi、Motokura Ken
    • Journal Title

      ACS Catalysis

      Volume: 13 Issue: 18 Pages: 12281-12287

    • DOI

      10.1021/acscatal.3c02309

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] In Situ Formation of RuSn Bimetallic Particles for Non-Oxidative Coupling of Methane2023

    • Author(s)
      Motokura Ken、Mizuno Ayaka、Hasegawa Shingo、Nambo Masayuki、Takabatake Moe、Suzuki Kenta、Manaka Yuichi、Uemura Yohei、Tsubaki Shuntaro、Chun Wang-Jae
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 127 Issue: 31 Pages: 15185-15194

    • DOI

      10.1021/acs.jpcc.3c03078

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Effect of Nafion Ionomer on Proton Exchange Membrane Electrolysis of Benzyl Alcohol2023

    • Author(s)
      Abdelnasser Shady、Matsushita Hibiki、Kurokawa Hideki、Ogihara Hitoshi
    • Journal Title

      Chemistry Letters

      Volume: 52 Issue: 7 Pages: 560-563

    • DOI

      10.1246/cl.230178

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Mg-Al hydrotalcite-based catalysts for one-pot synthesis of quinoline derivatives2023

    • Author(s)
      Motokura Ken
    • Journal Title

      Tetrahedron Green Chem

      Volume: 1 Pages: 100004-100004

    • DOI

      10.1016/j.tgchem.2023.100004

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Proton exchange membrane electrolysis of methanol for simultaneously synthesizing formaldehyde and hydrogen2023

    • Author(s)
      Kuramochi Nanako、Yoshida-Hirahara Miru、Ogihara Hitoshi、Kurokawa Hideki
    • Journal Title

      Sustainable Energy & Fuels

      Volume: 7 Issue: 3 Pages: 778-785

    • DOI

      10.1039/d2se01472f

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Electrochemical oxidation of 1-propanol through proton exchange membrane electrolysis2023

    • Author(s)
      Abdelnasser Shady、Hakamata Takumi、Ogihara Hitoshi、Kurokawa Hideki
    • Journal Title

      Journal of Electroanalytical Chemistry

      Volume: 928 Pages: 117009-117009

    • DOI

      10.1016/j.jelechem.2022.117009

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] CO2 conversion to formamide using a fluoride catalyst and metallic silicon as a reducing agent2022

    • Author(s)
      Wang Ruopeng、Nakao Kaiki、Manaka Yuichi、Motokura Ken
    • Journal Title

      Communications Chemistry

      Volume: 5 Issue: 1 Pages: 150-150

    • DOI

      10.1038/s42004-022-00767-4

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Transition-metal-free reaction sequence on solid base: One-pot synthesis of quinoline derivatives catalyzed by Mg-Al hydrotalcite2022

    • Author(s)
      Motokura Ken、Sato Risako、Ozawa Nao、Manaka Yuichi
    • Journal Title

      Molecular Catalysis

      Volume: 528 Pages: 112419-112419

    • DOI

      10.1016/j.mcat.2022.112419

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Fluoride Catalysts and Organic Additives for Conversion of CO <sub>2</sub> to Formic Acid and Methanol using Powdered Silicon as Reducing Agent2022

    • Author(s)
      Motokura Ken、Nakao Kaiki、Manaka Yuichi
    • Journal Title

      Asian Journal of Organic Chemistry

      Volume: 11 Issue: 10

    • DOI

      10.1002/ajoc.202200230

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Catalytic reduction and reductive functionalisation of carbon dioxide with waste silicon from solar panel as the reducing agent2022

    • Author(s)
      Pramudita Ria Ayu、Nakao Kaiki、Nakagawa Chihiro、Wang Ruopeng、Mochizuki Toshimitsu、Takato Hidetaka、Manaka Yuichi、Motokura Ken
    • Journal Title

      Energy Advances

      Volume: 1 Issue: 6 Pages: 385-390

    • DOI

      10.1039/d1ya00077b

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Montmorillonite-based heterogeneous catalysts for efficient organic reactions2022

    • Author(s)
      Takabatake Moe、Motokura Ken
    • Journal Title

      Nano Express

      Volume: 3 Issue: 1 Pages: 014004-014004

    • DOI

      10.1088/2632-959x/ac5ac3

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Mesoporous silica-supported rhodium complexes alongside organic functional groups for catalysing the 1,4-addition reaction of arylboronic acid in water2022

    • Author(s)
      Kong Yuanyuan、Ding Siming、Endo Koichiro、Nakajima Kiyotaka、Manaka Yuichi、Chun Wang-Jae、Tomita Ikuyoshi、Motokura Ken
    • Journal Title

      Green Chemistry

      Volume: 24 Issue: 8 Pages: 3269-3276

    • DOI

      10.1039/d1gc04577f

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Rhodium-Iodide Complex on a Catalytically Active SiO2 Surface for One‐Pot Hydrosilylation CO2 Cycloaddition2021

    • Author(s)
      Usui Kei、Manaka Yuichi、Chun Wang‐Jae、Motokura Ken
    • Journal Title

      Chemistry - A European Journal

      Volume: in press Issue: 5

    • DOI

      10.1002/chem.202104001

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Enhanced Catalysis Based on the Surface Environment of the Silica-Supported Metal Complex2021

    • Author(s)
      Motokura Ken、Ding Siming、Usui Kei、Kong Yuanyuan
    • Journal Title

      ACS Catalysis

      Volume: 11 Issue: 19 Pages: 11985-12018

    • DOI

      10.1021/acscatal.1c03426

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Presentation] 種々の担持金属触媒と固体酸触媒によるプロパンとベンゼンからの直接クメン合成2024

    • Author(s)
      新島巧海・鈴木健太・長谷川慎吾・本倉健
    • Organizer
      第133回触媒討論会
    • Related Report
      2023 Annual Research Report
  • [Presentation] Supported Metal Complex Catalysis for Fine Chemical Synthesis Enhanced by Functionalized Surface Environment2023

    • Author(s)
      Ken Motokura, Siming Ding, Kei Usui, Yuanyuan Kong
    • Organizer
      International Symposium on Catalysis and Fine Chemicals 2023
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] 分岐アルカンによるベンゼンの直接アルキル化反応における固体酸の触媒作用2023

    • Author(s)
      本倉 健、中村 由紀菜、高畠 萌、鈴木 健太、長谷川 慎吾
    • Organizer
      第53回石油・石油化学討論会
    • Related Report
      2023 Annual Research Report
  • [Presentation] 固体酸と担持金属の混合触媒によるプロパンとベンゼンの脱水素カップリング反応2023

    • Author(s)
      鈴木健太・高畠萌・長谷川慎吾・本倉健
    • Organizer
      第132回触媒討論会
    • Related Report
      2023 Annual Research Report
  • [Presentation] メタン脱水素カップリング反応に活性を示すRu-Sn触媒のin-situ構造解析2023

    • Author(s)
      本倉健・水野彩香・長谷川慎吾・南保雅之・高畠萌・鈴木健太・眞中雄一・上村洋平・椿俊太郎・田旺帝
    • Organizer
      第132回触媒討論会
    • Related Report
      2023 Annual Research Report
  • [Presentation] 固体酸-担持金属触媒混合系による分岐アルカンを用いたベンゼンのアルキル化反応2023

    • Author(s)
      中村由紀菜・高畠萌・長谷川慎吾・本倉健
    • Organizer
      第131回触媒討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 固体酸と担持白金の混合触媒系によるプロパンとベンゼンの脱水素カップリング反応2023

    • Author(s)
      鈴木健太・高畠萌・長谷川慎吾・本倉健
    • Organizer
      第131回触媒討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 固体酸触媒と固体塩基触媒を活用した高難度・高効率合成反応2022

    • Author(s)
      本倉健
    • Organizer
      第130回触媒討論会
    • Related Report
      2022 Annual Research Report
    • Invited
  • [Presentation] 機能集積型触媒を用いる高効率・高難度分子変換反応2022

    • Author(s)
      本倉健
    • Organizer
      2022年電気化学秋季大会 有機電子移動研究会
    • Related Report
      2022 Annual Research Report
    • Invited
  • [Presentation] Direst alkylation of various nucleophiles using catalyst mixture of supported Pd and solid acid2022

    • Author(s)
      Moe Takabatake, Satoshi Misaki, Wang-Jae Chun, Yuichi Manaka, Ken Motokura
    • Organizer
      Post Symposium of TOCAT9, 60th Aurora seminar, The 9th International Symposium of Institute for Catalysis
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Direct alkylation of aromatics with alkanes using a catalyst mixture of solid acid zeolites and hydrotalcite supported Pd2022

    • Author(s)
      Moe Takabatake, Satoshi Misaki, Wang-Jae Chun, Yuichi Manaka, Ken Motokura
    • Organizer
      The 9th Tokyo Conference on Advanced Catalytic Science and Technology
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 水素のみを副生するプロパンによるベンゼンの直接アルキル化反応2022

    • Author(s)
      鈴木健太、高畠萌、本倉健
    • Organizer
      第11回 JACI/GSCシンポジウム
    • Related Report
      2022 Annual Research Report
  • [Presentation] 固体酸によるプロパンとベンゼンの脱水素カップリング反応における担持白金の添加効果2022

    • Author(s)
      鈴木 健太、高畠 萌、本倉 健
    • Organizer
      日本化学会 第102春季年会
    • Related Report
      2021 Annual Research Report
  • [Presentation] 担持金属-固体酸混合触媒系によるアルカンとベンゼンの脱水素カップリング反応2022

    • Author(s)
      高畠 萌、美崎 慧、南保 雅之、田 旺帝、眞中 雄一、本倉 健
    • Organizer
      日本化学会 第102春季年会
    • Related Report
      2021 Annual Research Report
  • [Presentation] Development of supported catalyst systems for highly efficient/challenging organic reactions2022

    • Author(s)
      Ken Motokura
    • Organizer
      International Conference on State-of-the Art Catalysis and Surface/Interface Science for Sustainable Society - 11th Iwasawa conference
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] 固体酸触媒と金属錯体・金属ナノ粒子の協奏効果による反応加速2022

    • Author(s)
      本倉 健
    • Organizer
      令和3年度 触媒学会東日本支部講演会
    • Related Report
      2021 Annual Research Report
    • Invited
  • [Presentation] Dehydrogenative coupling of alkane and benzene accelerated by interparticle hydrogen transfer2021

    • Author(s)
      Moe Takabatake, Ayako Hashimoto, Wang-Jae Chun, Masayuki Nambo, Yuichi Manaka, Ken Motokura
    • Organizer
      18th Japan-Korea Symposium on Catalysis
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research
  • [Presentation] One-pot Synthesis of Quinoline Derivatives via Hydrogen Transfer and Cyclization Reactions with Solid Base Hydrotalcites2021

    • Author(s)
      Risako Sato, Nao Ozawa, Yuichi Manaka, Ken Motokura
    • Organizer
      18th Japan-Korea Symposium on Catalysis
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Direct addition of aromatics to alkanes in the presence of various zeolites and supported Pd catalysts2021

    • Author(s)
      Satoshi Misaki, Moe Takabatake, Masayuki Nambo, Yuichi Manaka, Ken Motokura
    • Organizer
      18th Japan-Korea Symposium on Catalysis
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Synergistic catalysis of supported metal catalysts for fine chemicals synthesis2021

    • Author(s)
      Ken Motokura
    • Organizer
      Synergistic catalysis of supported metal catalysts for fine chemicals synthesis
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] 各種ゼオライトと担持Pd種共存下でのアルカンへの芳香族直接付加反応2021

    • Author(s)
      美崎 慧・高畠 萌・南保 雅之・眞中 雄一・本倉 健
    • Organizer
      第11回CSJ化学フェスタ2021
    • Related Report
      2021 Annual Research Report
  • [Presentation] 担持白金触媒と固体酸触媒の混合系によるアルカンを用いるベンゼンのアルキル化反応2021

    • Author(s)
      高畠 萌・美崎 慧・田 旺帝・眞中 雄一・本倉 健
    • Organizer
      第11回CSJ化学フェスタ2021
    • Related Report
      2021 Annual Research Report
  • [Presentation] Mg-Alハイドロタルサイトによる水素移動・環化反応を経由するキノリン誘導体のワンポット合成2021

    • Author(s)
      佐藤 吏沙子・小澤 奈央・眞中 雄一・本倉 健
    • Organizer
      第11回CSJ化学フェスタ2021
    • Related Report
      2021 Annual Research Report
  • [Presentation] 固体塩基のみによる水素移動・環化反応を経由するキノリン誘導体の合成2021

    • Author(s)
      佐藤 吏沙子、小澤 奈央、眞中 雄一、本倉 健
    • Organizer
      第128回触媒討論会
    • Related Report
      2021 Annual Research Report
  • [Presentation] 担持Pt-固体酸混合触媒を用いるアルカンによるベンゼンのアルキル化反応2021

    • Author(s)
      高畠 萌、美崎 慧、田 旺帝、眞中 雄一、本倉 健
    • Organizer
      第128回触媒討論会
    • Related Report
      2021 Annual Research Report
  • [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~( 担当: 分担執筆 , 範囲: 第3章 第2節 メタンを用いる液相での炭素―炭素結合形成反応)2023

    • Author(s)
      本倉 健
    • Total Pages
      442
    • Publisher
      シーエムシー・リサーチ
    • Related Report
      2022 Annual Research Report
  • [Book] 触媒総合事典(担当: 分担執筆 , 範囲: アルキル化、ワンポット合成)2023

    • Author(s)
      本倉健
    • Total Pages
      544
    • Publisher
      朝倉書店
    • ISBN
      9784254252743
    • Related Report
      2022 Annual Research Report
  • [Book] 二酸化炭素有効利用技術 (担当: 分担執筆 , 範囲: 第2章 第2節 “有機分子触媒を利用した二酸化炭素からのギ酸誘導体の合成” )2022

    • Author(s)
      本倉健
    • Total Pages
      342
    • Publisher
      エヌ・ティー・エス
    • ISBN
      9784860437862
    • Related Report
      2022 Annual Research Report
  • [Remarks] 【プレスリリース】アルカンとベンゼンの直接結合反応のための金属ナノ粒子-ゼオライト複合触媒を開発

    • URL

      https://www.ynu.ac.jp/hus/koho/30639/detail.html

    • Related Report
      2023 Annual Research Report

URL: 

Published: 2021-10-22   Modified: 2025-01-30  

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