38小澤 弘宜33Hironobu OZAWA浅野竜太郎34Ryutaro ASANOノンバイアスでの水の完全分解を可能にするスペーサー導入型酸素生成触媒の創製（2020採択）Development of a Water Oxidation Molecular Catalyst Having a Spacer Unit Enabling Unbiased Overall Water Splitting(Project 2020)グルコース脱水素酵素のスプリット化に基づく新規電気化学イムノセンサ素子の開発（2020採択）Development of a novel electrochemical immunosensor based on split glucose dehydrogenase(Project 2020)icant dedoping of HTM was observed. Notably, this damage could be healed by exposure to short-wavelength light, leading to a partial recovery of the PSC efficiency. Our work exemplifies the robustness of perovskite against EB and the degradation mechanism of the overall PSC performance.ノンバイアスでの光化学的な水の完全分解を駆動できる分子性光電気化学セルの開発には，アノード上におけるTiO2伝導帯から酸素生成触媒への逆電子移動を効果的に抑制することが必要不可欠である．本研究では，アノード上における逆電子移動の抑制を目指したスペーサー導入型酸素生成触媒の創製，およびこれを用いた酸素生成フォトアノードの開発を目指して研究を行った．さらに，光増感サイトと触媒反応サイトを単一分子化した二核錯体の合成，およびこれを修飾したTiO2電極の作製も行った．この修飾電極の電気化学的な酸素生成触媒機能の評価を行い，この二核錯体が酸素生成触媒機能を示すことを明らかにした．本研究において得られた成果は，ノンバイアスでの光化学的な水の完全分解を達成できる分子性光電気化学セルの開発に向けた有用な知見となるものである．In order to develop the molecular-based photoelectrochemical cells promoting overall water splitting even under bias-free conditions, the backward electron transfer from the conduction band of TiO2 to the water oxidation catalyst should be suppressed effectively. In this study, several water oxidation catalysts having spacer units have been synthesized, and the TiO2 electrodes modified with these water oxidation catalysts have been also fabricated for this purpose. Moreover, a dinuclear complex having both the photosensitizing and the catalytic units has been synthesized, and the catalytic activity for the electrochemical water oxidation by the TiO2 elec-trode modified with this dinuclear complex has been evaluated. Several valuable insights into the development of the molecular-based photoelectrochemical cells for overall water splitting have been obtained in this study.本研究では，新たな電気化学イムノセンシング素子を指向した，電極との電子の授受が可能な酸化還元酵素であるグルコース脱水素酵素（GDH）の断片化（スプリット化）を目指した．文献情報等を基に，スプリット化GDHをデザインし，それぞれ大腸菌発現系，および巻き戻し操作を用いて調製した．再会合は，ニッケルイオンとHistagの凝集，およびSpyCatcher/SpyTagシステムを利用して行った．結果，スプリット化させた各断片ではほとんど認められなった酵素活性の再会合後の回復が認められたため，スプリット化GDHの開発に成功したといえる．今後，新たなセンシング素子としての応用に期待が持たれる．In this study, we studied on the construction of a split glucose dehydrogenases (GDH), which is an oxidore-ductase capable of transferring electrons to electrodes as a novel electrochemical immunosensing element. Split GDHs were designed based on previous reports, and prepared using the E. coli expression system with a refolding procedure. Reassociation was carried out using the aggregation of nickel ions and Histag or the SpyCatcher / SpyTag system. As a result, we confirmed successful preparation of the split GDHs, which showed enzymatic activities only after the reassociation. The split GDHs are expected to be applied as novel sensing elements in the future.
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