Fabrication of Soft Photonic Crystals for Novel Functions

• Project Area: Soft Crystals: Science and Photofunctions of Easy-Responsive Systems with Felxibility and Higher-Ordering
• Project/Area Number: 17H06376
• Research Category: Grant-in-Aid for Scientific Research on Innovative Areas (Research in a proposed research area)
• Allocation Type: Single-year Grants
• Review Section: Science and Engineering
• Research Institution: Hokkaido University
• Principal Investigator: グン 剣萍 北海道大学, 先端生命科学研究院, 教授 (20250417)
• Co-Investigator(Kenkyū-buntansha): 黒川 孝幸 北海道大学, 先端生命科学研究院, 教授 (40451439) ; 野々山 貴行 北海道大学, 先端生命科学研究院, 特任准教授 (50709251)
• Project Period (FY): 2017-06-30 – 2022-03-31
• Project Status: Granted (Fiscal Year 2021)
• Budget Amount: ¥49,660,000 (Direct Cost: ¥38,200,000、Indirect Cost: ¥11,460,000); Fiscal Year 2021: ¥9,750,000 (Direct Cost: ¥7,500,000、Indirect Cost: ¥2,250,000); Fiscal Year 2020: ¥9,750,000 (Direct Cost: ¥7,500,000、Indirect Cost: ¥2,250,000); Fiscal Year 2019: ¥9,750,000 (Direct Cost: ¥7,500,000、Indirect Cost: ¥2,250,000); Fiscal Year 2018: ¥9,750,000 (Direct Cost: ¥7,500,000、Indirect Cost: ¥2,250,000); Fiscal Year 2017: ¥10,660,000 (Direct Cost: ¥8,200,000、Indirect Cost: ¥2,460,000)
• Keywords: 高分子構造・物性 / ソフトクリスタル / 構造色 / 生体模倣 / 刺激応答

Outline of Annual Research Achievements

脂質二分子膜と高分子網目が積層したフォトニックゲルは、層間隔に起因する構造色を示し弱い力学刺激に応答して、その構造色が変化する。ディスプレイなどの応用を考慮すると、電気で駆動できることが望ましい。電気化学的手法を用いて、電気で色を調整することが可能なフォトニックゲルを創製した。高分子網目のポリアクリル酸ナトリウムは、水の電気分解によって発生したプロトンによって、イオン交換が発生する。ポリアクリル酸の状態は電離度が下がり、イオン性浸透圧が下がるため膜厚が低下し、結果構造色がブルーシフトする。
脳の記憶は動的であり、重要でない情報をフィルタリングすることで自発的に忘れる。 ここでは温度に敏感な動的結合を持つハイドロゲルを用いて脳のような動的記憶素子を開発した。ゲルに熱をかけると動的結合は弱まり水分の移動が起こるが、急冷すると構造の復元が温度変化より遅いことから、一時的な相分離構造（情報）を形成する。この構造は時間とともに消失する。この忘却時間は、脳の行動と同様に、熱学習時間に比例する。
ダブルネットワーク（DN）ゲルは、軟骨や靭帯などの柔らかい支持組織の有望な人工置換材料の候補である。このような用途では、ゲルが骨と強固に接着することが必要不可欠である。DNゲルの表層にコーティングされた低結晶性ハイドロキシアパタイト（HAp）はゲル/骨複合層を形成する自発的な骨形成を誘起する。ここでは、44Ca同位体をドープしたHAp / DNゲルをウサギの大腿骨の欠損部に移植し、同位体顕微鏡を用いてカルシウム同位体比を追跡することにより、ゲル/骨界面での動的骨形成プロセスを分析した。 DNゲル表層では2週以降で傾斜構造の未熟な骨がゲル領域に形成され始め、その骨形成に合成HApから溶解したCaイオンを再利用していることが認められた。

Current Status of Research Progress

2: Research has progressed on the whole more than it was originally planned.

Reason

フォトニックゲルの電気駆動を達成し、応用を見据えたデバイスの開発が可能となった。

Strategy for Future Research Activity

2021年度は、ソフトフォトニックゲルと極限相分離ゲルについての評価を行う。
ソフトフォトニックゲルは、１）巨視的に一軸配向ラメラ構造を有するPhotonic PDGI/PAAmゲルがイオン性界面活性剤であるＳＤＳとの相互作用と構造変化を調べる。具体的には、様々なＳＤＳ溶液中におけるゲルの膨潤異方性の変化、力学物性の変化とラメラーミセル構造転移との相関を解明する。また、得られた結果を用いて、高速度・高力学感度・高空間分解能のイメージセンサーとして応用するための最適条件を見出す。また、巨視的に一軸配向ラメラ構造を有するPhotonic PDGI/PAAmゲルの力学物性について検討する。具体的には、固いPDGI層と柔らかいPAAmゲル層の弾性率の違いがこのゲルの力学物性、特に破壊靭性にどのような影響を与えるかについて、解明したい。具体的な手法としては、PAAmゲル層の含水率を幅広い範囲で調整し、PAAmゲル層の弾性率を系統的に変えることができる。その際のPDGI/PAAmゲルのPure shear テストにおける破壊エネルギーを測定し、弾性率変化による効果を解明する。ＳＡＸＳを使い、PDGI/PAAmゲルの変形時における構造変化（ラメラーミセル転移）を測定し、力学変形とエネルギー散逸の関係を解明する。
極限相分離ゲルについて、東工大の森川淳子教授及び名大の内橋貴之教授と共同で、相分離構造の形成・消失過程を観察する。森川教授の温度波測定を用いて、相分離形成時及びゴム－ガラス転移における熱拡散率を求め、相構造形成と高分子の運動性を評価する。内橋教授の高速AFMを用いて、相分離後の高分子濃厚相及び希薄相の局所弾性率を計測する。あらかじめ作製しておいた弾性率－高分子体積分率の校正曲線を用いて、局所の高分子体積分率を求め、正確な相図の作製を行う。

Research Products

• [Int'l Joint Research] ESPCI Paris/Paris-Saclay University/Sorbonne University(フランス)
• [Int'l Joint Research] Cornell University(米国)
• [Int'l Joint Research] University of Dhaka(バングラデシュ)
• [Int'l Joint Research] Southern Univ of Science and Technology/South China University of Technology(中国)
• [Int'l Joint Research] University of Wollongong(オーストラリア)
• [Int'l Joint Research] Cornell University(米国)
• [Int'l Joint Research] ESPCI Paris(フランス)
• [Int'l Joint Research] South China University of Technology/Zhejiang University/Southern Univ of Sci and Tech(中国)
• [Int'l Joint Research] University of Bordeux(フランス)
• [Int'l Joint Research] Iowa State University(米国)
• [Int'l Joint Research] University of Dhaka(バングラデシュ)
• [Int'l Joint Research] University of Dhaka(Bangladesh)
• [Journal Article] Ultrapurified Alginate Gel Containing Bone Marrow Aspirate Concentrate Enhances Cartilage and Bone Regeneration on Osteochondral Defects in a Rabbit Model (2021)
  • Author(s): Liang Xu, Atsushi Urita, Tomohiro Onodera, Ryosuke Hishimura, Takayuki Nonoyama, Masanari Hamasaki, Dawei Liang, Kentarou Houman, Jian Ping Gong, Norimasa Iwasaki
  • Journal Title: The American Journal of Sports Medicine Volume: accepted
  • Peer Reviewed
• [Journal Article] Ultrahigh‐Water‐Content Photonic Hydrogels with Large Electro‐Optic Responses in Visible to Near‐Infrared Region (2021)
  • Author(s): Yue Youfeng、Norikane Yasuo、Gong Jian Ping
  • Journal Title: Advanced Optical Materials Volume: published online Pages: 2002198-2002198
  • DOI: 10.1002/adom.202002198
  • Peer Reviewed / Open Access
• [Journal Article] Molecular mechanism of abnormally large nonsoftening deformation in a tough hydrogel (2021)
  • Author(s): Ye Ya Nan、Cui Kunpeng、Hong Wei、Li Xueyu、Yu Chengtao、Hourdet Dominique、Nakajima Tasuku、Kurokawa Takayuki、Gong Jian Ping
  • Journal Title: Proceedings of the National Academy of Sciences Volume: 118
  • DOI: 10.1073/pnas.2014694118
  • NAID: 120007160280
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Bone Marrow Aspirate Concentrate Combined with in Situ Forming Bioresorbable Gel Enhances Intervertebral Disc Regeneration in Rabbits (2021)
  • Author(s): Ukeba Daisuke、Yamada Katsuhisa、Tsujimoto Takeru、Ura Katsuro、Nonoyama Takayuki、Iwasaki Norimasa、Sudo Hideki
  • Journal Title: Journal of Bone and Joint Surgery Volume: Publish Ahead of Print
  • DOI: 10.2106/jbjs.20.00606
  • Peer Reviewed
• [Journal Article] Tough Double Network Hydrogel and Its Biomedical Applications (2021)
  • Author(s): Nonoyama Takayuki、Gong Jian Ping
  • Journal Title: Annual Review of Chemical and Biomolecular Engineering Volume: 12
  • DOI: 10.1146/annurev-chembioeng-101220-080338
  • Peer Reviewed / Open Access
• [Journal Article] 忘却能力を持つ動的記憶素子の構築～人間の脳の動的な記憶・忘却挙動に触発されて～ (2021)
  • Author(s): 崔 昆朋、グン 剣萍
  • Journal Title: 超分子研究会アニュアルレビュー Volume: 41 Pages: 12-13
• [Journal Article] Hydrogels toughened by biominerals providing energy-dissipative sacrificial bonds (2020)
  • Author(s): Fukao Kazuki、Tanaka Kazuki、Kiyama Ryuji、Nonoyama Takayuki、Gong Jian Ping
  • Journal Title: Journal of Materials Chemistry B Volume: 8 Pages: 5184-5188
  • DOI: 10.1039/d0tb00833h
  • NAID: 120007099139
  • Peer Reviewed / Open Access
• [Journal Article] Lamellar Bilayer to Fibril Structure Transformation of Tough Photonic Hydrogel under Elongation (2020)
  • Author(s): Haque M. Anamul、Cui Kunpeng、Ilyas Muhammad、Kurokawa Takayuki、Marcellan Alba、Brulet Annie、Takahashi Riku、Nakajima Tasuku、Gong J. Ping
  • Journal Title: Macromolecules Volume: 53 Pages: 4711-4721
  • DOI: 10.1021/acs.macromol.0c00878
  • NAID: 120007089525
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Fiber‐Reinforced Viscoelastomers Show Extraordinary Crack Resistance That Exceeds Metals (2020)
  • Author(s): Cui Wei、King Daniel R.、Huang Yiwan、Chen Liang、Sun Tao Lin、Guo Yunzhou、Saruwatari Yoshiyuki、Hui Chung‐Yuen、Kurokawa Takayuki、Gong Jian Ping
  • Journal Title: Advanced Materials Volume: 32 Pages: 1907180-1907180
  • DOI: 10.1002/adma.201907180
  • NAID: 120007126055
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Hydrogels as dynamic memory with forgetting ability (2020)
  • Author(s): Yu Chengtao、Guo Honglei、Cui Kunpeng、Li Xueyu、Ye Ya Nan、Kurokawa Takayuki、Gong Jian Ping
  • Journal Title: Proceedings of the National Academy of Sciences Volume: 117 Pages: 18962-18968
  • DOI: 10.1073/pnas.2006842117
  • NAID: 120006957256
  • Peer Reviewed / Open Access
• [Journal Article] Preparation of Tough Double- and Triple-Network Supermacroporous Hydrogels through Repeated Cryogelation (2020)
  • Author(s): Sedlacik Tomas、Nonoyama Takayuki、Guo Honglei、Kiyama Ryuji、Nakajima Tasuku、Takeda Yoshihiro、Kurokawa Takayuki、Gong Jian Ping
  • Journal Title: Chemistry of Materials Volume: 32 Pages: 8576-8586
  • DOI: 10.1021/acs.chemmater.0c02911
  • NAID: 120007165399
  • Peer Reviewed / Open Access
• [Journal Article] Isotope Microscopic Observation of Osteogenesis Process Forming Robust Bonding of Double Network Hydrogel to Bone (2020)
  • Author(s): Nonoyama Takayuki、Wang Lei、Tsuda Masumi、Suzuki Yuki、Kiyama Ryuji、Yasuda Kazunori、Tanaka Shinya、Nagata Kousuke、Fujita Ryosuke、Sakamoto Naoya、Kawasaki Noriyuki、Yurimoto Hisayoshi、Gong Jian Ping
  • Journal Title: Advanced Healthcare Materials Volume: 10 Pages: 2001731-2001731
  • DOI: 10.1002/adhm.202001731
  • NAID: 120007187747
  • Peer Reviewed / Open Access
• [Journal Article] Fabrication of Bioinspired Hydrogels: Challenges and Opportunities (2020)
  • Author(s): Fan Hailong、Gong Jian Ping
  • Journal Title: Macromolecules Volume: 53 Pages: 2769-2782
  • DOI: 10.1021/acs.macromol.0c00238
  • Peer Reviewed / Open Access
• [Journal Article] Non-linear rheological study of hydrogel sliding friction in water and concentrated hyaluronan solution (2020)
  • Author(s): Hirayama Satoshi、Kurokawa Takayuki、Gong Jian Ping
  • Journal Title: Tribology International Volume: 147 Pages: 106270-106270
  • DOI: 10.1016/j.triboint.2020.106270
  • Peer Reviewed / Open Access
• [Journal Article] Meet the phase-separation polymeric gel (2020)
  • Author(s): Nonoyama Takayuki、Gong Jian Ping
  • Journal Title: The Innovation Platform Volume: 1 Pages: 73-74
• [Journal Article] Superior fracture resistance of fiber reinforced polyampholyte hydrogels achieved by extraordinarily large energy-dissipative process zones (2019)
  • Author(s): Huang Yiwan、King Daniel R.、Cui Wei、Sun Tao Lin、Guo Honglei、Kurokawa Takayuki、Brown Hugh R.、Hui Chung-Yuen、Gong Jian Ping
  • Journal Title: Journal of Materials Chemistry A Volume: 7 Pages: 13431-13440
  • DOI: 10.1039/c9ta02326g
  • NAID: 120006863161
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Hydrophobic Hydrogels with Fruit‐Like Structure and Functions (2019)
  • Author(s): Guo Hui、Nakajima Tasuku、Hourdet Dominique、Marcellan Alba、Creton Costantino、Hong Wei、Kurokawa Takayuki、Gong Jian Ping
  • Journal Title: Advanced Materials Volume: 31 Pages: 1900702-1900702
  • DOI: 10.1002/adma.201900702
  • NAID: 120006863168
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Facile synthesis of novel elastomers with tunable dynamics for toughness, self-healing and adhesion (2019)
  • Author(s): Chen Liang、Sun Tao Lin、Cui Kunpeng、King Daniel R.、Kurokawa Takayuki、Saruwatari Yoshiyuki、Gong Jian Ping
  • Journal Title: Journal of Materials Chemistry A Volume: 7 Pages: 17334-17344
  • DOI: 10.1039/c9ta04840e
  • NAID: 120006877259
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Tough double network elastomers reinforced by the amorphous cellulose network (2019)
  • Author(s): Murai Joji、Nakajima Tasuku、Matsuda Takahiro、Tsunoda Katsuhiko、Nonoyama Takayuki、Kurokawa Takayuki、Gong Jian Ping
  • Journal Title: Polymer Volume: 178 Pages: 121686-121686
  • DOI: 10.1016/j.polymer.2019.121686
  • NAID: 120007147245
  • Peer Reviewed
• [Journal Article] Polyelectrolyte complexation via viscoelastic phase separation results in tough and self-recovering porous hydrogels (2019)
  • Author(s): Murakawa Kohei、King Daniel R.、Sun Taolin、Guo Honglei、Kurokawa Takayuki、Gong Jian Ping
  • Journal Title: Journal of Materials Chemistry B Volume: 7 Pages: 5296-5305
  • DOI: 10.1039/c9tb01376h
  • NAID: 120006886030
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Internal Damage Evolution in Double-Network Hydrogels Studied by Microelectrode Technique (2019)
  • Author(s): Guo Honglei、Hong Wei、Kurokawa Takayuki、Matsuda Takahiro、Wu Zi Liang、Nakajima Tasuku、Takahata Masakazu、Sun Taolin、Rao Ping、Gong Jian Ping
  • Journal Title: Macromolecules Volume: 52 Pages: 7114-7122
  • DOI: 10.1021/acs.macromol.9b01308
  • NAID: 120006886033
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Instant Thermal Switching from Soft Hydrogel to Rigid Plastics Inspired by Thermophile Proteins (2019)
  • Author(s): Nonoyama Takayuki、Lee Yong Woo、Ota Kumi、Fujioka Keigo、Hong Wei、Gong Jian Ping
  • Journal Title: Advanced Materials Volume: 32 Pages: 1905878-1905878
  • DOI: 10.1002/adma.201905878
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Shearing-induced contact pattern formation in hydrogels sliding in polymer solution (2019)
  • Author(s): Yashima Shintaro、Hirayama Satoshi、Kurokawa Takayuki、Salez Thomas、Takefuji Haruna、Hong Wei、Gong Jian Ping
  • Journal Title: Soft Matter Volume: 15 Pages: 1953-1959
  • DOI: 10.1039/c8sm02428f
  • NAID: 120006809253
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Designing Responsive Photonic Crystal Patterns by Using Laser Engraving (2019)
  • Author(s): Yue Youfeng、Kurokawa Takayuki
  • Journal Title: ACS Applied Materials & Interfaces Volume: 11 Pages: 10841-10847
  • DOI: 10.1021/acsami.8b22498
  • Peer Reviewed
• [Journal Article] 刺激応答性発色ゲル (2018)
  • Author(s): 堀端修人、中島 祐、グン 剣萍
  • Journal Title: 応用物理学会・有機分子・バイオエレクトロニクス分科会 会誌 Volume: 29 Pages: 232-235
• [Journal Article] Tough and Variable-Band-Gap Photonic Hydrogel Displaying Programmable Angle-Dependent Colors (2018)
  • Author(s): Haque Md. Anamul、Mito Kei、Kurokawa Takayuki、Nakajima Tasuku、Nonoyama Takayuki、Ilyas Muhammad、Gong Jian Ping
  • Journal Title: ACS Omega Volume: 3 Pages: 55-62
  • DOI: 10.1021/acsomega.7b01443
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Water-Triggered Ductile?Brittle Transition of Anisotropic Lamellar Hydrogels and Effect of Confinement on Polymer Dynamics (2017)
  • Author(s): Ilyas Muhammad、Haque Md. Anamul、Yue Youfeng、Kurokawa Takayuki、Nakajima Tasuku、Nonoyama Takayuki、Gong Jian Ping
  • Journal Title: Macromolecules Volume: 50 Pages: 8169-8177
  • DOI: 10.1021/acs.macromol.7b01438
  • Peer Reviewed / Int'l Joint Research
• [Presentation] Robust Phase Separation-induced Rubbery-to -Glassy Transition at Elevating Temperature (2020)
  • Author(s): Takayuki Nonoyama
  • Organizer: 第69回高分子学会年次大会
• [Presentation] バイオミネラルをエネルギー散逸項とするハイドロゲルの強靭化 (2020)
  • Author(s): 野々山貴行
  • Organizer: 日本セラミックス協会第33回秋季シンポジウム
• [Presentation] 生体無機物を犠牲結合としたハイドロゲルの強靭化 (2020)
  • Author(s): 野々山 貴行
  • Organizer: 第69回高分子討論会
• [Presentation] 極限相分離を利用した逆ガラス転移現象 (2020)
  • Author(s): 野々山 貴行
  • Organizer: 知の協奏を目指すソフトおよびナノマテリアル研究会２０２０(SNOWJ2020)
• [Presentation] Quick & Reversible Thermo-Robustizing Hydrogels Exhibiting 1000 Times Modulus Jump (2019)
  • Author(s): Nonoyama Takayuki
  • Organizer: International Symposium on Biopolymer Synthesis and Degradation
  • Int'l Joint Research / Invited
• [Presentation] Hydrogel Possessing Rubbery-to-Glassy Transition at Elevated Temperature (2019)
  • Author(s): Nonoyama Takayuki
  • Organizer: China-Japan Joint Symposium for Young Polymer Scientists
  • Int'l Joint Research / Invited
• [Presentation] Robust Phase-Separation Induced Rubbery-to-Glassy Transition at Elevated Temperature (2019)
  • Author(s): Nonoyama Takayuki
  • Organizer: Seminar at Shaanxi University of Science & Technology
  • Int'l Joint Research / Invited
• [Presentation] 高温で瞬時に弾性率が1000倍以上ジャンプするソフトマテリアル (2019)
  • Author(s): 野々山 貴行
  • Organizer: 第28回ポリマー材料フォーラム
• [Presentation] 多重膜構造を有する機能性微粒子ゲルの創製 (2019)
  • Author(s): 堀端 修人、黒川 孝幸、グン 剣萍
  • Organizer: 第28回ポリマー材料フォーラム
• [Presentation] Deformation of 1D photonic hydrogels with lipid bilayers (2018)
  • Author(s): Jian Ping Gong
  • Organizer: The 4th International Workshop on Soft Machines and Mechanics
  • Int'l Joint Research / Invited
• [Presentation] Study on Contact Pattern Formation at Frictional Interface of Gel (2018)
  • Author(s): Satoshi Hirayama
  • Organizer: The 13th International Symposium on Polymer Physics (PP'2018)
  • Int'l Joint Research
• [Presentation] 多重膜構造を有するジャイアントベシクルゲルの創製 (2018)
  • Author(s): 堀端修人
  • Organizer: 33rd Summer University in Hokkaido・2018年度北海道高分子若手研究会
• [Presentation] Anisotropic Bilayer-hybrid Gels: Fabrication and Water Induced Rubbery-Glassy Transition (2018)
  • Author(s): Muhammad Ilyas
  • Organizer: 第67回高分子討論会
• [Presentation] Tough and Variable-Band-Gap Photonic Hydrogel Displaying Programmable Angle-Dependent Color (2018)
  • Author(s): Md. Anamul Haque
  • Organizer: Fourth Conference of Bangladesh Crystallographic Association
  • Int'l Joint Research
• [Presentation] Water Triggered Ductile-Brittle Transition of Anisotropic Lamellar Hydrogels (2017)
  • Author(s): Muhammad Ilyas
  • Organizer: 第66回高分子討論会
• [Presentation] Tough Functional Hybrid Gel Thin Film (2017)
  • Author(s): Muhammad Ilyas
  • Organizer: ゲルワークショップ イン 松山
• [Remarks] 研究室ホームページ
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• [Remarks] 研究室ホームページ
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