Hydrogen production from formate by a hydride biocatalyst

• Project/Area Number: 18H02091
• Research Category: Grant-in-Aid for Scientific Research (B)
• Allocation Type: Single-year Grants
• Section: 一般
• Review Section: Basic Section 37010:Bio-related chemistry
• Research Institution: Kyushu University
• Principal Investigator: Yoon Ki-Seok 九州大学, カーボンニュートラル・エネルギー国際研究所, 准教授 (50701497)
• Project Period (FY): 2018-04-01 – 2021-03-31
• Project Status: Completed (Fiscal Year 2020)
• Budget Amount: ¥17,550,000 (Direct Cost: ¥13,500,000、Indirect Cost: ¥4,050,000); Fiscal Year 2020: ¥4,420,000 (Direct Cost: ¥3,400,000、Indirect Cost: ¥1,020,000); Fiscal Year 2019: ¥4,420,000 (Direct Cost: ¥3,400,000、Indirect Cost: ¥1,020,000); Fiscal Year 2018: ¥8,710,000 (Direct Cost: ¥6,700,000、Indirect Cost: ¥2,010,000)
• Keywords: エネルギー変換系 / 水素酸化反応 / ヒドロゲナーゼ / ギ酸デヒドロゲナーゼ / 生体触媒 / 水素発生 / 二酸化炭素の水素化 / 水素生成 / エネルギー変換反応 / 融合型酵素反応 / 水素 / 二酸化炭素 / ギ酸 / 人工融合酵素

Outline of Final Research Achievements

Efficient hydrogen evolution from formate using biocatalysts is an attractive mean to produce an environmentally clean energy source. However, the biocatalysts for formate oxidation and hydrogen evolution are extremely oxygen-labile. We present an excellent model system for hydrogen evolution from formate using enzymatic reaction by the encapsulated cytoplasmic membrane of Citrobacter sp. S-77 containing O2-stable [NiFe]-hydrogenase and [Mo]-formate dehydrogenase immobilized on Ketjenblack EC-600JD with sodium alginate. The immobilized biocatalysts lead to stabilization of hydrogen production from formate. Notably, its catalytic H2 production showed a remarkable O2-stability, maintaining its catalytic activity even after air exposure.

Academic Significance and Societal Importance of the Research Achievements

微生物によるバイオマスを原料とした水素生成では、ギ酸を基質とすることも可能である。実際、様々な通性嫌気性細菌による、ギ酸を基質とした水素生成法がこれまでに報告されている。しかし、酸素安定性酵素を導電性のカーボンブラックに担持し、酵素電極によるギ酸からの水素生成のエネルギー変換系を構築するのは、本研究が初めての例となる。本研究は、異なる生体触媒をカーボン担体に固定することで、水溶性エネルギー変換系を創成するものであり、貴金属触媒を持たない高効率なエネルギー変換系の研究開発に大きく貢献するものである。

Research Products

• [Journal Article] A NiRhS Fuel Cell Catalyst-Lessons from Hydrogenase. (2020)
  • Author(s): Ogo, Seiji;* Ando, Tatsuya; Thi Minh, Le Tu; Mori, Yuki; Matsumoto, Takahiro; Yatabe, Takeshi; Yoon, Ki-Seok; Sato, Yukio; Hibino, Takashi; Kaneko, Kenji.
  • Journal Title: Chemical Communucations Volume: 56 Issue: 79 Pages: 11787-11790
  • DOI: 10.1039/d0cc04789a
  • Peer Reviewed
• [Journal Article] Biochemical and structural characterization of a thermostable Dps protein with His‐type ferroxidase centers and outer metal‐binding sites (2020)
  • Author(s): Minato Takuo、Teramoto Takamasa、Kakuta Yoshimitsu、Ogo Seiji、Yoon Ki‐Seok
  • Journal Title: FEBS Open Bio Volume: - Issue: 7 Pages: 1219-1229
  • DOI: 10.1002/2211-5463.12837
  • Peer Reviewed / Open Access
• [Journal Article] NiFe], [FeFe], and [Fe] Hydrogenase Models from Isomers (2020)
  • Author(s): Ogo, Seiji; Kishima, Takahiro; Yatabe, Takeshi; Miyazawa, Keishi; Yamasaki, Ryunosuke; Matsumoto, Takahiro; Ando, Tatsuya; Kikkawa, Mitsuhiro; Isegawa, Miho; Yoon, Ki-Seok; Hayami, Shinya
  • Journal Title: Sci. Adv. Volume: 6 Issue: 24
  • DOI: 10.1126/sciadv.aaz8181
  • Peer Reviewed / Open Access
• [Journal Article] Glyceraldehyde-3-phosphate Dehydrogenase of Citrobacter sp. S-77 is Post-translationally Modified by CoA (Protein CoAlation) under Oxidative Stress (2019)
  • Author(s): Tsuji, Kohsei; Yoon, Ki-Seok; Ogo, Seiji.
  • Journal Title: FEBS Open Bio Volume: 9 Pages: 53-73
  • Peer Reviewed / Open Access
• [Journal Article] Redox-dependent conformational changes of a proximal [4Fe-4S] cluster in Hyb-type [NiFe]-hydrogenase to protect the active site from O2 (2018)
  • Author(s): N. D. M. Noor, H. Matsuura, K. Nishikawa, H. Tai, S. Hirota, J. Kim, J. Kang, M. Tateno, K-S. Yoon, S. Ogo, S. Kubota, Y. Shomura and Y. Higuchi
  • Journal Title: Chemical Communications Volume: 54 Issue: 87 Pages: 12385-12388
  • DOI: 10.1039/c8cc06261g
  • Peer Reviewed / Open Access
• [Journal Article] Oxidation of Guanosine Monophosphate with O2 via a Ru-peroxo Complex in Water (2018)
  • Author(s): Takenaka, Makoto; Kikkawa, Mitsuhiro; Matsumoto, Takahiro; Yatabe, Takeshi; Ando, Tatsuya; Yoon, Ki-Seok; Ogo, Seiji
  • Journal Title: Chem. Asian J. Volume: 13 Issue: 21 Pages: 3180-3184
  • DOI: 10.1002/asia.201801267
  • Peer Reviewed
• [Journal Article] Multifunctional Catalysts for H2O2-resistant Hydrogen Fuel Cells (2018)
  • Author(s): Mori, Yuki; Ando, Tatsuya; Matsumoto, Takahiro; Yatabe, Takeshi; Kikkawa, Mitsuhiro; Yoon, Ki-Seok; Ogo, Seiji
  • Journal Title: Angew. Chem. Int. Ed. Volume: 57 Issue: 48 Pages: 34-36
  • DOI: 10.1002/anie.201810270
  • Peer Reviewed
• [Journal Article] A MnI Model for the Photoinhibited Species of Oxygen-Evolving Complex. (2018)
  • Author(s): Yatabe, Takeshi; Tokunaga, Taisuke; Matsumoto, Kikkawa, Mitsuhiro; Tatsuya; Yoon, Ki-Seok; Ogo, Seiji.
  • Journal Title: Chem. Lett. Volume: 47 Issue: 1 Pages: 34-36
  • DOI: 10.1246/cl.170869
  • NAID: 130006302110
  • Peer Reviewed
• [Presentation] New [NiFe]hydrogenases running between H2 and O2 molecules (2018)
  • Author(s): Ki-Seok Yoon, Seiji Ogo
  • Organizer: The 20th Biocatalysis Symposium of Japan
  • Int'l Joint Research
• [Presentation] Exploring new biocatalysts for hydrogen activation (2018)
  • Author(s): Ki-Seok Yoon, Seiji Ogo
  • Organizer: The 4th Korea-Japan Symposium on Hydrogen in Materials
  • Int'l Joint Research / Invited
• [Presentation] New insights of naturally occurring O2-tolerant [NiFe]hydrogenase (2018)
  • Author(s): Ki-Seok Yoon, Seiji Ogo
  • Organizer: International Congress on Pure & Applied Chemistry 2018 (ICPAC2018)
  • Int'l Joint Research / Invited
• [Presentation] A diversity of Naturally Occurring O2-tolerant [NiFe]hydrogenase (2018)
  • Author(s): Ki-Seok Yoon, Tahahiro Matsumoto, Seiji Ogo
  • Organizer: International Conference on Coordination Chemistry 2018 (ICCC2018)
  • Int'l Joint Research
• [Presentation] Structural genes and hydrogen activation of [NiFe]hydrogenase from Citrobacter sp. S-77 (2018)
  • Author(s): Ki-Seok Yoon, Seiji Ogo
  • Organizer: The 70th The Society for Biotechnology, Annual Meeting 2018
• [Presentation] Redox-regulation of glyceraldehyde-3-phosphate dehydrogenase from Citrobacter sp. S-77 by coenzyme A (2018)
  • Author(s): Kohsei Tsuji, Ki-Seok Yoon, Seiji Ogo
  • Organizer: The 91st Annual Meeting of the Japanese Biochemical Society