Chemically-stable proton-conductive aromatic polymers with high performance and mechanical durability

• Project/Area Number: 18K04746
• Research Category: Grant-in-Aid for Scientific Research (C)
• Allocation Type: Multi-year Fund
• Section: 一般
• Review Section: Basic Section 26040:Structural materials and functional materials-related
• Research Institution: University of Yamanashi
• Principal Investigator: MIYAKE Junpei 山梨大学, 大学院総合研究部, 准教授 (30581409)
• Project Period (FY): 2018-04-01 – 2021-03-31
• Project Status: Completed (Fiscal Year 2020)
• Budget Amount: ¥4,160,000 (Direct Cost: ¥3,200,000、Indirect Cost: ¥960,000); Fiscal Year 2020: ¥1,560,000 (Direct Cost: ¥1,200,000、Indirect Cost: ¥360,000); Fiscal Year 2019: ¥1,300,000 (Direct Cost: ¥1,000,000、Indirect Cost: ¥300,000); Fiscal Year 2018: ¥1,300,000 (Direct Cost: ¥1,000,000、Indirect Cost: ¥300,000)
• Keywords: 高分子合成 / ポリフェニレン / イオノマー / 高分子電解質膜 / 補強膜 / 燃料電池 / 高分子電解質 / 膜 / プロトン伝導

Outline of Final Research Achievements

In the present study, we prepared a novel fluorine-free reinforced aromatic ionomer membrane (SPP-QP-PE), composed of our chemically-stable polyphenylene ionomer (SPP-QP) and a mechanically-flexible porous polyethylene substrate (PE). Compared to the bare SPP-QP membrane, the reinforced membrane (SPP-QP-PE) exhibited improved mechanical toughness, without sacrificing the high proton conductivity and gas impermeability. In addition, the reinforced membrane (SPP-QP-PE) functioned well in fuel cells with high performance and durability.

Academic Significance and Societal Importance of the Research Achievements

ポリフェニレンイオノマーは、その極めて高い化学的安定性ゆえに、各種エネルギーデバイスにおける電解質材料として注目を集めている。しかしながら、高分子主鎖が剛直なフェニレン基のみで構成されているため、硬くて脆い膜になりやすく、機械的強度に富み柔軟であることが求められる隔膜としての利用は難しいとされてきた。本研究は、そのようなポリフェニレンイオノマー膜が有する課題の解決法を提案するものであり、特に、燃料電池や水電解システムへの応用が期待できる。

Research Products

• [Journal Article] リチャージャブル燃料電池 (2021)
  • Author(s): 宮武 健治、小柳津 研一、三宅 純平
  • Journal Title: 水素エネルギーシステム Volume: 46 Pages: 6-11
• [Journal Article] Proton Exchange Membranes Containing Densely Sulfonated Quinquephenylene Groups for High Performance and Durable Fuel Cells (2020)
  • Author(s): Z. Long; J. Miyake; K. Miyatake
  • Journal Title: J. Mater. Chem. A Volume: 8 Issue: 24 Pages: 12134-12140
  • DOI: 10.1039/d0ta03435e
  • Peer Reviewed
• [Journal Article] Rechargeable proton exchange membrane fuel cell containing an intrinsic hydrogen storage polymer (2020)
  • Author(s): Junpei Miyake; Yasunari Ogawa; Toshiki Tanaka; Jinju Ahn; Kouki Oka; Kenichi Oyaizu; Kenji Miyatake
  • Journal Title: Communications Chemistry Volume: 3 Issue: 1 Pages: 138-138
  • DOI: 10.1038/s42004-020-00384-z
  • Peer Reviewed / Open Access
• [Journal Article] Ladder-type Sulfonated Poly(arylene perfluoroalkylene)s for High Performance Proton Exchange Membrane Fuel Cells (2020)
  • Author(s): Z. Long; J. Miyake; K. Miyatak
  • Journal Title: RSC Adv. Volume: 10 Issue: 67 Pages: 41058-41064
  • DOI: 10.1039/d0ra08630d
  • Peer Reviewed / Open Access
• [Journal Article] Structural Investigation of Sulfonated Polyphenylene Ionomers for the Design of Better Performing Proton-Conductive Membranes (2020)
  • Author(s): K. Shiino; T. Otomo; T. Yamada; H. Arima; K. Hiroi; S. Takata; J. Miyake; K. Miyatake
  • Journal Title: ACS Appl. Polym. Mater. Volume: 2 Issue: 12 Pages: 5558-5565
  • DOI: 10.1021/acsapm.0c00895
  • Peer Reviewed / Open Access
• [Journal Article] Differences in the Synthetic Method Affected Copolymer Sequence and Membrane Properties of Sulfonated Polymers (2020)
  • Author(s): Hosaka Ibuki、Sawano Takatoshi、Kimura Taro、Matsumoto Akinobu、Miyake Junpei、Miyatake Kenji
  • Journal Title: Bulletin of the Chemical Society of Japan Volume: 93 Issue: 3 Pages: 393-398
  • DOI: 10.1246/bcsj.20190309
  • NAID: 130007808668
  • Peer Reviewed
• [Journal Article] Sulfonated Poly(arylene perfluoroalkylene) Terpolymers as Novel Proton Exchange Membranes for High Performance Fuel Cells (2020)
  • Author(s): Long Zhi、Miyake Junpei、Miyatake Kenji
  • Journal Title: Bulletin of the Chemical Society of Japan Volume: 93 Issue: 3 Pages: 338-344
  • DOI: 10.1246/bcsj.20190351
  • NAID: 130007808651
  • Peer Reviewed
• [Journal Article] アニオン導電性高分子薄膜の設計とアルカリ形燃料電池への展開 (2020)
  • Author(s): 三宅純平、宮武健治
  • Journal Title: 高分子 Volume: 69/3 Pages: 110-111
• [Journal Article] Sublayered Structures of Hydrated Nafion^® Thin Film Formed by Casting on Pt Substrate Analyzed by X-ray Absorption Spectroscopy under Ambient Conditions and Neutron Reflectometry at Temperature of 80°C and Relative Humidity of 30–80% (2019)
  • Author(s): KAWAMOTO Teppei、AOKI Makoto、KIMURA Taro、CHINAPANG Pondchanok、MIZUSAWA Takako、YAMADA Norifumi L.、NEMOTO Fumiya、WATANABE Takeshi、TANIDA Hajime、MATSUMOTO Masashi、IMAI Hideto、MIYAKE Junpei、MIYATAKE Kenji、INUKAI Junji
  • Journal Title: Electrochemistry Volume: 87 Issue: 5 Pages: 270-275
  • DOI: 10.5796/electrochemistry.19-00042
  • NAID: 130007702969
  • ISSN: 1344-3542, 2186-2451
  • Year and Date: 2019-09-05
  • Peer Reviewed
• [Journal Article] Quaternized poly(arylene perfluoroalkylene)s (QPAFs) for alkaline fuel cells - a perspective (2019)
  • Author(s): Miyake Junpei、Miyatake Kenji
  • Journal Title: Sustainable Energy & Fuels Volume: 3 Issue: 8 Pages: 1916-1928
  • DOI: 10.1039/c9se00106a
  • Peer Reviewed
• [Journal Article] Highly stable polyphenylene ionomer membranes from dichlorobiphenyls (2019)
  • Author(s): Shiino Keisuke、Miyake Junpei、Miyatake Kenji
  • Journal Title: Chemical Communications Volume: 55 Issue: 49 Pages: 7073-7076
  • DOI: 10.1039/c9cc02475a
  • Peer Reviewed
• [Journal Article] Effect of Alkanediol Additives on the Properties of Polyphenylene-Based Proton Exchange Membranes (2019)
  • Author(s): Long Zhi、Zhang Yaojian、Miyake Junpei、Miyatake Kenji
  • Journal Title: Industrial & Engineering Chemistry Research Volume: 58 Issue: 23 Pages: 9915-9920
  • DOI: 10.1021/acs.iecr.9b01564
  • Peer Reviewed
• [Journal Article] プロトン導電性高分子薄膜の設計と燃料電池への応用 (2019)
  • Author(s): 三宅純平、宮武健治
  • Journal Title: 化学と工業 Volume: 72/8 Pages: 665-667
• [Journal Article] In-plane distribution of water inside Nafion; thin film analyzed by neutron reflectivity at temperature of 80 °C and relative humidity of 30%-80% based on 4- layered structural model (2019)
  • Author(s): Teppei Kawamoto, Makoto Aoki, Taro Kimura, Takako Mizusawa, Norifumi L. Yamada, Junpei Miyake, Kenji Miyatake, and Junji Inukai
  • Journal Title: Japanese Journal of Applied Chemistry Volume: 58 Issue: SI Pages: SIID01-SIID01
  • DOI: 10.7567/1347-4065/ab0c7c
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Partially Fluorinated Polyphenylene Ionomers as Proton Exchange Membranes for Fuel Cells: Effect of Pendant Multi-Sulfophenylene Groups (2019)
  • Author(s): Long Zhi、Miyake Junpei、Miyatake Kenji
  • Journal Title: ACS Applied Energy Materials Volume: 2 Issue: 10 Pages: 7527-7534
  • DOI: 10.1021/acsaem.9b01513
  • Peer Reviewed
• [Journal Article] Structurally Well-Defined Anion-Exchange Membranes Containing Perfluoroalkyl and Ammonium-Functionalized Fluorenyl Groups (2018)
  • Author(s): Ozawa Mizuki、Kimura Taro、Otsuji Kanji、Akiyama Ryo、Miyake Junpei、Uchida Makoto、Inukai Junji、Miyatake Kenji
  • Journal Title: ACS Omega Volume: 3 Issue: 11 Pages: 16143-16149
  • DOI: 10.1021/acsomega.8b02742
  • Peer Reviewed / Open Access
• [Journal Article] 革新的な芳香族系電解質膜の開発 (2018)
  • Author(s): 三宅純平、宮武健治
  • Journal Title: クリーンエネルギー Volume: 9 Pages: 24-28
• [Presentation] Properties and Fuel Cell Performance of Reinforced Aromatic Ionomer Membranes (2020)
  • Author(s): Miyake Junpei、Watanabe Takayuki、Miyatake Kenji
  • Organizer: 第69回高分子学会年次大会
• [Presentation] 全固体高分子形リチャージャブル燃料電池の原理実証研究 (2020)
  • Author(s): 三宅 純平、小川 泰誠、田中 俊貴、アン ジンジュ、岡 弘樹、小柳津 研一、宮武 健治
  • Organizer: 第69回高分子討論会
• [Presentation] 芳香族系電解質：プロトン伝導膜の高性能化・高耐久化 (2019)
  • Author(s): 三宅純平
  • Organizer: 第144回燃料電池研究会セミナー
  • Invited
• [Presentation] 汎用的なNi化合物を用いたプロトン導電性芳香族高分子の合成と物性 (2019)
  • Author(s): 保坂伊吹、澤野貴俊、日下部正人、三宅純平、宮武健治
  • Organizer: 第68回高分子学会年次大会
• [Presentation] Effect of the Multi Sulfophenylene Groups on the Properties of Poly(arylene perfluoroalkylene) (SPAF) Membranes (2019)
  • Author(s): Long Zhi、三宅純平、宮武健治
  • Organizer: 第68回高分子学会年次大会
• [Presentation] スルホン酸化ポリフェニレン電解質薄膜の合成、構造と物性 (2019)
  • Author(s): 椎野佳祐、木村太郎、大友季哉、山田武、有馬寛、廣井孝介、高田慎一、三宅純平、犬飼潤治、宮武健治
  • Organizer: 第68回高分子討論会
• [Presentation] 芳香族系高分子電解質膜の高性能化・高耐久化 (2018)
  • Author(s): 三宅純平、Zhang Yaojian、秋山良、清水瞭、内田誠、宮武健治
  • Organizer: 第25回燃料電池シンポジウム
• [Presentation] スルホン酸化ポリフェニレンの合成 (2018)
  • Author(s): 椎野佳祐、三宅純平、宮武健治
  • Organizer: 第67回高分子学会年次大会
• [Presentation] フルオレニル基を有する部分フッ素化アニオン導電性高分子の合成と物性 (2018)
  • Author(s): 小澤美月、三宅純平、宮武健治
  • Organizer: 第67回高分子学会年次大会
• [Presentation] 芳香族系アニオン導電性高分子薄膜における化学的安定性の向上 (2018)
  • Author(s): 横田尚樹、三宅純平、宮武健治
  • Organizer: 第67回高分子討論会
• [Remarks] 山梨大学クリーンエネルギー研究センター
  • URL: http://www.clean.yamanashi.ac.jp/
• [Remarks] 山梨大学燃料電池ナノ材料研究センター
  • URL: https://fc-nano.yamanashi.ac.jp/
• [Remarks] 山梨大学燃料電池ナノ材料研究センター
  • URL: http://fc-nano.yamanashi.ac.jp/