Chemoenzymatic cascades mediated by in situ generated H2O2.

2021 Fiscal Year Final Research Report

• Project/Area Number: 20K15393
• Research Category: Grant-in-Aid for Early-Career Scientists
• Allocation Type: Multi-year Fund
• Review Section: Basic Section 37010:Bio-related chemistry
• Research Institution: Tohoku University
• Principal Investigator: Okamoto Yasunori 東北大学, 学際科学フロンティア研究所, 助教 (50843405)
• Project Period (FY): 2020-04-01 – 2022-03-31
• Keywords: 生体触媒化学

Outline of Final Research Achievements

Enzymatic cascades enable multistep chemical transformations in a high space-time yield under environmentally friendly reaction conditions. Integrating synthetic catalysts into enzyme cascades is expected to increase the number of synthesizable molecules. However, the reaction conditions of synthetic catalysts and those of biocatalysts are very different. This project aims to construct a cascade reaction, which does not require sacrificial reagents or coenzymes, by combining a synthetic catalyst that works under the conditions relevant to enzymatic reaction with an enzyme driven by the product of the synthetic catalyst.
In the first year, a synthetic catalyst found through screening was synthesized. In the second year, we prepared a modified heme protein based on previous reports. These were concurrently used in a reaction vessel, leading to slight absorption changes that may be derived from the final product.

Free Research Field

生体触媒化学

Academic Significance and Societal Importance of the Research Achievements

複数の酵素 (生体触媒) を同時利用した酵素カスケードでは、酵素反応の利点である温和な反応条件と高い選択性に加え、中間体の単離・精製を省略可能なため、高い空間時間収率も期待できる。　このように低環境負荷型の物質変換技術として、酵素カスケードは有望である。　酵素カスケードに合成触媒を統合できれば、合成可能な分子の種類が飛躍的に増大する。本研究では、合成触媒反応の生成物によって駆動する天然酵素を組み合わせることで、犠牲試薬や高価な補酵素を必要としない合成-生体触媒カスケードの構築をめざしており、低環境負荷型の物質変換技術に資するものである。