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

Development of ELG-RP-TS method for efficient transition state controle in polymerization reactions

Research Project

Project/Area Number 16KT0059
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeMulti-year Fund
Section特設分野
Research Field Transition State Control
Research InstitutionKyushu University

Principal Investigator

青木 百合子  九州大学, 総合理工学研究院, 教授 (10211690)

Project Period (FY) 2016-07-19 – 2020-03-31
Project Status Completed (Fiscal Year 2019)
Budget Amount *help
¥18,590,000 (Direct Cost: ¥14,300,000、Indirect Cost: ¥4,290,000)
Fiscal Year 2018: ¥5,850,000 (Direct Cost: ¥4,500,000、Indirect Cost: ¥1,350,000)
Fiscal Year 2017: ¥5,850,000 (Direct Cost: ¥4,500,000、Indirect Cost: ¥1,350,000)
Fiscal Year 2016: ¥6,890,000 (Direct Cost: ¥5,300,000、Indirect Cost: ¥1,590,000)
Keywords量子化学計算 / メタロセン触媒 / Ziegler Natta触媒 / 高分子反応 / 効率的遷移状態探索 / Elongation法 / 遷移状態 / 量子化学 / ELG-RP-TS法 / 電子状態
Outline of Annual Research Achievements

本課題では高分子重合反応の効率的遷移状態制御のためのELG-RP-TS法、の開発と題して、均一系および不均一系触媒反応に対して適用している。これまで開発してきたElongation法にNudged Elastic Band(NEB)法による構造最適化ルーティンを呼び出すインターフェースの導入を行った。簡単なテストモデル高分子に適用して反応末端の構造が正しく計算できていることを確認し、内部座標によってさらに効率的に実行できるように開発している。一方、平面波基底による周期性固体用の密度汎関数プログラム(VASP)に対し、表面触媒反応の場合に、未知の反応前後の構造に対しても、効率的に遷移状態(TS)を見出す手法を展開した。NEB法、Climbing-Image-NEB法, Dimer 法を段階的に作用させることにより機械的にTSを見出す手法を構築し、不均一系Ziegler-Natta(ZN)触媒反応に適用を行った。また、反応前段階のTiCl4と助触媒AlEt3による活性点形成機構について、様々な反応機構が提唱されているものの未だ結論は出ていない。ZN触媒のオレフィン重合制御に重要と考える活性点形成機構および活性点形成の際に添加される内部ドナーの効果を解析した。一方、ポリオレフィン合成における高い構造制御能を持つため重合触媒として注目されている均一系メタロセン触媒について、構造選択性の機構解明や共重合生成ポリマーの特性予測を目的として、ポリプロピレン重合の構造制御メカニズム、反応ルート、助触媒の役割等を明らかにするべくTS計算とその詳細解析を行った。その一つとして、TSにおける軌道相互作用解析のために、活性中心重元素を含む系に適用可能なThrough Space/Bond(TS/TB)-TS解析法も組み合わせて、反応初期段階における立体規則性の決定要因について詳細な解析を行った。

Report

(3 results)
  • 2019 Annual Research Report
  • 2017 Research-status Report
  • 2016 Research-status Report

Research Products

(55 results)

All 2020 2019 2018 2017 2016 Other

All Int'l Joint Research Journal Article Presentation Book

  • [Int'l Joint Research] 華南師範大学(中国)

    • Related Report
      2019 Annual Research Report
  • [Int'l Joint Research] ジャギロニアン大学(ポーランド)

    • Related Report
      2019 Annual Research Report
  • [Int'l Joint Research] サンクトペテルブルク州立大学(ロシア連邦)

    • Related Report
      2019 Annual Research Report
  • [Journal Article] Synthesis of Monodispersedly Sized ZnO Nanowires from Randomly Sized Seeds2020

    • Author(s)
      Zhao Xixi、Nagashima Kazuki、Zhang Guozhu、Hosomi Takuro、Yoshida Hideto、Akihiro Yuya、Kanai Masaki、Mizukami Wataru、Zhu Zetao、Takahashi Tsunaki、Suzuki Masaru、Samransuksamer Benjarong、Meng Gang、Yasui Takao、Aoki Yuriko、Baba Yoshinobu、Yanagida Takeshi
    • Journal Title

      Nano Lett.

      Volume: 20 Pages: 599-605

    • DOI

      10.1021/acs.nanolett.9b04367

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] An Attempt at Theoretical Calculation of Electronic Structure of model-DNA2019

    • Author(s)
      寺前裕之、青木百合子
    • Journal Title

      J. Comput. Chem. Jpn.

      Volume: 15 Issue: 6 Pages: 219-220

    • DOI

      10.2477/jccj.2016-0057

    • NAID

      130005310498

    • ISSN
      1347-1767, 1347-3824
    • Year and Date
      2019-02-15
    • Related Report
      2017 Research-status Report 2016 Research-status Report
    • Peer Reviewed / Open Access / Acknowledgement Compliant
  • [Journal Article] Elongation toward Linear Scaling: Two Electron Integrals in Regionally Localized Molecular Orbital Basis2019

    • Author(s)
      D. R. Price, L. Peng, S. Li, F. L. Gu, and Y. Aoki
    • Journal Title

      Acta Scientiarum Naturalium Universitatis Sunyatseni

      Volume: 58 Pages: 91-102

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Rational Method of Monitoring Molecular Transformations on Metal-Oxide Nanowire Surfaces2019

    • Author(s)
      C. Wang, T. Hosomi, K. Nagashima, T. Takahashi, G. Zhang, M. Kanai, H. Zeng, W. Mizukami, N. Shioya, T. Shimoaka, Y. Aoki, J. Terao, T. Hasegawa and T. Yanagida
    • Journal Title

      Nano Letters

      Volume: 19 Pages: 2443-2449

    • DOI

      10.1021/acs.nanolett.8b05180

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Extraction of One-Handed Helical Frontier Orbital in Even [n]Cumulenes by Breaking Mirror Images of Right- and Left-Handed Helical Orbitals: Theoretical Study2019

    • Author(s)
      Orimoto Yuuichi、Aoki Yuriko、Imamura Akira
    • Journal Title

      J. Phys. Chem. C

      Volume: 印刷中 Pages: 11134-11139

    • DOI

      10.1021/acs.jpcc.9b01829

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Extent of structural change during the reaction and its relationship to isoselectivity in polypropylene polymerization with ansa ‐zirconocene/borate catalyst: A computational study2019

    • Author(s)
      Y. Orimoto, S. Shirane, and Y. Aoki
    • Journal Title

      Journal of Computational Chemistry

      Volume: 40 Pages: 2622-2635

    • DOI

      10.1002/jcc.26040

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Role of Pyridinium Groups and Iodide Ions in Photoelectrochromism in Viologen-Based Ion-Pair Charge-Transfer Complexes: Molecular Orbital Analysis2018

    • Author(s)
      Yuuichi Orimoto, Kosuke Ishimoto, and Yuriko Aoki
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 122 Pages: 4546-4556

    • DOI

      10.1021/acs.jpcc.7b10281

    • Related Report
      2017 Research-status Report
    • Peer Reviewed
  • [Journal Article] Theoretical Study of Cu Intercalation through a Defect in Zero-Layer Graphene on SiC Surface2017

    • Author(s)
      Y. ORIMOTO, K. OTSUKA, K. YAGYU, H. TOCHIHARA, T. SUZUKI, Y. AOKI,
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 121 Pages: 7294-7302

    • DOI

      10.1021/acs.jpcc.7b00314

    • Related Report
      2017 Research-status Report 2016 Research-status Report
    • Peer Reviewed
  • [Journal Article] Importance of Through-Space Interaction of [2,2′]-Paracyclophane-oligo(p-phenylenevinylene) Molecular Wires for Photovoltaic Application and Effective Wire Design by Chemical Substitution2017

    • Author(s)
      Yuuichi Orimoto, Kohei Kato, and Yuriko Aoki
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 121 Pages: 17703-17711

    • DOI

      10.1021/acs.jpcc.7b05730

    • Related Report
      2017 Research-status Report
    • Peer Reviewed
  • [Journal Article] An Attempt at Ab Initio Crystal Orbital Calculation of Electronic Structure of B-type Model-DNA2017

    • Author(s)
      Hiroyuki Teramae and Yuriko Aoki
    • Journal Title

      AIP Conference Proceedings

      Volume: 1906 Pages: 030023-030023

    • DOI

      10.1063/1.5012302

    • Related Report
      2017 Research-status Report
    • Peer Reviewed
  • [Journal Article] An efficient unrestricted PCM-elongation method for large high-spin polymer/dendrimer systems2016

    • Author(s)
      Xun Zhu, Yuuichi Orimoto, and Yuriko Aoki
    • Journal Title

      Zeitschrift fur Physikalische Chemie

      Volume: 印刷中 Pages: 667-680

    • DOI

      10.1515/zpch-2015-0722

    • Related Report
      2016 Research-status Report
    • Peer Reviewed / Acknowledgement Compliant
  • [Journal Article] Development of molecular fragment interaction method for designing organic ferromagnets2016

    • Author(s)
      Xun Zhu and Yuriko Aoki
    • Journal Title

      Journal of Mathematical Chemistry

      Volume: 54 Pages: 1585-1595

    • DOI

      10.1007/s10910-016-0638-3

    • Related Report
      2016 Research-status Report
    • Peer Reviewed / Acknowledgement Compliant
  • [Journal Article] Automated property optimization via ab initio O(N) elongation method: application to (hyper-)polarizability in DNA2016

    • Author(s)
      Yuuichi Orimoto and Yuriko Aoki
    • Journal Title

      The Journal of Chemical Physics

      Volume: 145

    • DOI

      10.1063/1.4956456

    • Related Report
      2016 Research-status Report
    • Peer Reviewed / Acknowledgement Compliant
  • [Journal Article] Computational study of Cu-containing artificial DNA: twist angle dependence of magnetism2016

    • Author(s)
      Yuuichi Orimoto and Yuriko Aoki
    • Journal Title

      ChemistrySelect

      Volume: 1 Pages: 5521-5529

    • DOI

      10.1002/slct.201600940

    • Related Report
      2016 Research-status Report
    • Peer Reviewed / Acknowledgement Compliant
  • [Journal Article] Computational scheme to determine local vibrations of large systems using elongation method2016

    • Author(s)
      Lin Jin, Yun-an Yan, and Yuriko Aoki
    • Journal Title

      Theoretical Chemistry Accounts

      Volume: 136

    • DOI

      10.1007/s00214-016-2030-6

    • Related Report
      2016 Research-status Report
    • Peer Reviewed / Acknowledgement Compliant
  • [Presentation] 高分子における量子化学計算2019

    • Author(s)
      青木 百合子
    • Organizer
      高分子東海シンポジウム
    • Related Report
      2019 Annual Research Report
    • Invited
  • [Presentation] Ge(001)表面におけるPTCDA分子のホッピング過程の第一原理計算:協奏的機構と遷移状態構造2019

    • Author(s)
      塩田知弥、水上渉、栃原浩、柳生数馬、鈴木孝将、青木百合子
    • Organizer
      日本表面真空学会九州支部学術講演会
    • Related Report
      2019 Annual Research Report
  • [Presentation] 第一原理計算によるGe(001)表面上でのPTCDA分子拡散機構の解明2019

    • Author(s)
      塩田知弥, 水上渉, 栃原浩, 柳生数馬, 鈴木孝将, 青木百合子
    • Organizer
      第56回化学関連支部合同九州大会
    • Related Report
      2019 Annual Research Report
  • [Presentation] Linear-scaling two-ways elongation method for local perturbation on nanotubes/DNA2019

    • Author(s)
      Y. Aoki, Y. Orimoto, and A. Pomogaeva
    • Organizer
      Current Trends in Theoretical Chemistry VIII(CTTC 8)
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] 直線炭素鎖分子Cumuleneの特異な螺旋状分子軌道―化学修飾による左右螺旋の分離と機能設計―2019

    • Author(s)
      折本 裕一,大川 育子,青木 百合子
    • Organizer
      第13回分子科学討論会
    • Related Report
      2019 Annual Research Report
  • [Presentation] 特異的な構造特性と電子状態を示す有限ナノリボンと有機太陽電池ワイヤへの応用2019

    • Author(s)
      青木 百合子,折本 裕一
    • Organizer
      第13回分子科学討論会
    • Related Report
      2019 Annual Research Report
  • [Presentation] 第一原理計算によるGe(001)表面上でのPTCDA分子ホッピングの解析2019

    • Author(s)
      塩田 知弥,水上 渉,栃原 浩,柳生 数馬,鈴木 孝将,青木 百合子
    • Organizer
      第13回分子科学討論会
    • Related Report
      2019 Annual Research Report
  • [Presentation] Geometry optimization of polymers via ONIOM based elongation method2019

    • Author(s)
      Denis Mashkovtsev, 水上 渉, Jacek Korchowiec, Anna Stachowicz-kusnierz, 青木 百合子
    • Organizer
      第13回分子科学討論会
    • Related Report
      2019 Annual Research Report
  • [Presentation] A linear scaling approach for efficient geometry optimization in perturbed DNAs2019

    • Author(s)
      Y. Aoki, Y. Orimoto, and A. Pomogaeva
    • Organizer
      The Ninth Conference of the Asia-Pacific Association of Theoretical and Computational Chemists (APATCC2019)
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Computer-aided molecular design for DNA bulge recognition ligands by order-N elongation method2019

    • Author(s)
      Y. Orimoto, A. Pomogaeva, K. Hisama, A. Yano, K. Miyagawa, K. Nakatani, and Y. Aoki
    • Organizer
      The 46th International Symposium on Nucleic Acids Chemistry(ISNAC2019)
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Elongation法によるDNA損傷修復解明のための見える化システムの構築2019

    • Author(s)
      青木 百合子、 折本 裕一
    • Organizer
      2019年度 九州大学オープンイノベーションワークショップ
    • Related Report
      2019 Annual Research Report
  • [Presentation] Elucidation of the diffusion mechanism of PTCDA on Ge(001) using first principles calculations2019

    • Author(s)
      T. Shiota, W. Mizukami, H. Tochihara, K. Yagyu, T. Suzuki, and Y. Aoki
    • Organizer
      81st Okazaki Conference : Forefront of Measurement Technologies for Surface Chemistry and Physics in Real-Space, k-Space, and Real-Time
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Mechanism of Highly Selective Olefin Polymerization by Metallocene Catalyst: Computational Approach2018

    • Author(s)
      Yuuichi Orimoto, Satoru Shirane, and Yuriko Aoki
    • Organizer
      IRCCS-JST CREST Joint Symposium
    • Related Report
      2017 Research-status Report
    • Int'l Joint Research
  • [Presentation] Ab Initio Electronic Structure Calculation of Polymononucleotide, a Model of B‐type DNA2018

    • Author(s)
      Hiroyuki Teramae and Yuriko Aoki
    • Organizer
      14th International Conference of Computational Methods in Sciences and Engineering(ICCMSE 2018)
    • Related Report
      2017 Research-status Report
    • Int'l Joint Research
  • [Presentation] Elongation method for efficient quantum chemistry calculations toward functional designs of bio/nano materials2018

    • Author(s)
      青木 百合子, 水上 渉, 大川 育子, 折本 裕一
    • Organizer
      第1回 九州大学女性研究者ダイバーシティシンポジウム ―理工系分野―
    • Related Report
      2017 Research-status Report
  • [Presentation] Efficient quantum chemical method for functional material design2017

    • Author(s)
      Yuriko Aoki
    • Organizer
      The 10th International Conference on Computational Physics (ICCP10)
    • Place of Presentation
      Holiday Inn Macao (China)
    • Year and Date
      2017-01-16
    • Related Report
      2016 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Efficient quantum chemical method for functional material design2017

    • Author(s)
      Yuriko Aoki
    • Organizer
      The 10th International Conference on Computational Physics(ICCP10)
    • Related Report
      2017 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Ab Initio Crystal Orbital Calculation of Electronic Structure of B-type model-DNA2017

    • Author(s)
      Hiroyuki Teramae and Yuriko Aoki
    • Organizer
      11th Triennial Congress of the World Association of Theoretical and Computational Chemists(WATOC 2017)
    • Related Report
      2017 Research-status Report
    • Int'l Joint Research
  • [Presentation] Ab Initio Calculations on Polymononucleotide and Polydinucleotides as Model of B-type DNA Polymers2017

    • Author(s)
      Hiroyuki Teramae and Yuriko Aoki
    • Organizer
      11th European Conference on Theoretical and Computational Chemistry(EUCO-TCC 2017)
    • Related Report
      2017 Research-status Report
    • Int'l Joint Research
  • [Presentation] 第一原理計算によるPt-Rhバイメタリックナノ粒子触媒の物性評価2017

    • Author(s)
      山本 瞳, 水上 渉, 木村 加奈, 北條 元, 青木 百合子, 永長 久寛
    • Organizer
      第120回触媒討論会
    • Related Report
      2017 Research-status Report
  • [Presentation] Zr,Hfを導入した不均一系 Ziegler-Natta 触媒の理論化学的研究2017

    • Author(s)
      坂上 弘樹, 水上 渉, 青木 百合子
    • Organizer
      第120回触媒討論会
    • Related Report
      2017 Research-status Report
  • [Presentation] 表面化学反応に対する第一原理遷移状態計算のガウス過程を用いた高速化2017

    • Author(s)
      水上 渉, 青木 百合子
    • Organizer
      第120回触媒討論会
    • Related Report
      2017 Research-status Report
  • [Presentation] Elongation法による生体高分子の効率的構造最適化および反応解析法2017

    • Author(s)
      青木 百合子, 水上 渉, 伊藤 雅浩, 折本 裕一
    • Organizer
      第11回分子科学討論会
    • Related Report
      2017 Research-status Report
  • [Presentation] 生体分子の反応機構解明と機能設計を目指した量子化学的手法開発とその応用2017

    • Author(s)
      折本 裕一, 汐見 彩花, 青木 百合子
    • Organizer
      第11回分子科学討論会
    • Related Report
      2017 Research-status Report
  • [Presentation] メタロセン触媒重合の構造制御機構の解明と超効率的計算手法によるポリマー特性の解析2017

    • Author(s)
      白根 聡, 折本 裕一, 青木 百合子
    • Organizer
      第11回分子科学討論会
    • Related Report
      2017 Research-status Report
  • [Presentation] モデルDNAのHartree-Fock計算2017

    • Author(s)
      寺前 裕之, 青木 百合子
    • Organizer
      第11回分子科学討論会
    • Related Report
      2017 Research-status Report
  • [Presentation] Elongation法を用いた化学反応計算とポテンシャル面のon the fly構築によるその高速化2017

    • Author(s)
      水上 渉, 青木 百合子
    • Organizer
      第11回分子科学討論会
    • Related Report
      2017 Research-status Report
  • [Presentation] Computational design of DNAs: property control via elongation method2017

    • Author(s)
      Yuuichi Orimoto and Yuriko Aoki
    • Organizer
      The 44th International Symposium on Nucleic Acids Chemistry(ISNAC 2017)
    • Related Report
      2017 Research-status Report
    • Int'l Joint Research
  • [Presentation] Selectivity of olefin polymerization with metallocene catalyst and the effects of producted polymers on its mechanism2017

    • Author(s)
      Satoru Shirane, Yuuichi Orimoto, and Yuriko Aoki
    • Organizer
      The 19th Cross Straits Symposium on Energy and Environmental Science and Technology(CSS-EEST19)
    • Related Report
      2017 Research-status Report
    • Int'l Joint Research
  • [Presentation] An efficient NLO functional optimization by elongation method for nanotubes and DNA2016

    • Author(s)
      Yuriko Aoki and Yuuichi Orimoto
    • Organizer
      Stereodynamics 2016
    • Place of Presentation
      Institute of Atomic and Molecular Sciences (Taiwan)
    • Year and Date
      2016-11-06
    • Related Report
      2016 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Modeling Molecular Interactions in Halogen-bonding Cocrystal2016

    • Author(s)
      Wataru Mizukami and Yuriko Aoki
    • Organizer
      International Symposium on Multi-scale Simulation of Condensed-phase Reacting Systems ( MSCRS2016 )
    • Place of Presentation
      名古屋大学 (愛知県名古屋市)
    • Year and Date
      2016-10-10
    • Related Report
      2016 Research-status Report
    • Int'l Joint Research
  • [Presentation] Theoretical approach to the property and reaction design of DNA/proteins by through- space/bond interaction analysis and elongation method2016

    • Author(s)
      Yuuichi Orimoto and Yuriko Aoki
    • Organizer
      第43回国際核酸化学シンポジウム
    • Place of Presentation
      熊本大学 (熊本県熊本市)
    • Year and Date
      2016-09-27
    • Related Report
      2016 Research-status Report
    • Int'l Joint Research
  • [Presentation] 閉殻系および開殻系 Elongation 法の展開と機能性ナノワイヤへの応用2016

    • Author(s)
      Yuriko Aoki, Wataru Mizukami, Yuuichi Orimoto, and Kai Liu
    • Organizer
      第10回分子科学討論会
    • Place of Presentation
      神戸ファッションマート (兵庫県神戸市)
    • Year and Date
      2016-09-13
    • Related Report
      2016 Research-status Report
  • [Presentation] 酵素反応機構解明のための軌道相互作用解析法の開発と応用2016

    • Author(s)
      Yuuichi Orimoto and Yuriko Aoki
    • Organizer
      第10回分子科学討論会
    • Place of Presentation
      神戸ファッションマート (兵庫県神戸市)
    • Year and Date
      2016-09-13
    • Related Report
      2016 Research-status Report
  • [Presentation] Linear-scaling elongation method for efficient search of the best functional polymers-applications to DNA2016

    • Author(s)
      Yuriko Aoki and Yuuichi Orimoto
    • Organizer
      Current Trends in Theoretical Chemistry VII
    • Place of Presentation
      Jagiellonian University (Poland)
    • Year and Date
      2016-09-04
    • Related Report
      2016 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] スピン制約を導入したElongation法の開発2016

    • Author(s)
      Wataru Mizukami and Yuriko Aoki
    • Organizer
      第10回分子科学討論会
    • Place of Presentation
      神戸ファッションマート (兵庫県神戸市)
    • Related Report
      2016 Research-status Report
  • [Book] Quantum chemical approach for organic ferromagnetic material design2017

    • Author(s)
      Yuriko Aoki, Yuuichi Orimoto, and Akira Imamura
    • Total Pages
      138
    • Publisher
      Springer International Publishing
    • ISBN
      9783319498294
    • Related Report
      2017 Research-status Report 2016 Research-status Report

URL: 

Published: 2016-07-20   Modified: 2021-01-27  

Information User Guide FAQ News Terms of Use Attribution of KAKENHI

Powered by NII kakenhi