2019 Fiscal Year Final Research Report
Material Transformation Using Biocatalysts Assisted by External Additives
| Project Area | Precise Formation of a Catalyst Having a Specified Field for Use in Extremely Difficult Substrate Conversion Reactions |
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| Project/Area Number |
15H05806
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| Research Category |
Grant-in-Aid for Scientific Research on Innovative Areas (Research in a proposed research area)
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| Allocation Type | Single-year Grants |
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| Review Section |
Science and Engineering
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| Research Institution | Nagoya University |
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Principal Investigator |
Shoji Osami 名古屋大学, 理学研究科, 教授 (90379587)
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| Project Period (FY) |
2015-06-29 – 2020-03-31
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| Keywords | シトクロムP450 / 酸化反応 / ヘム獲得蛋白質 / 金属錯体 / 結晶構造解析 / ポルフィリン / 緑膿菌 / 擬似基質 |
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| Outline of Final Research Achievements |
We found that cytochrome P450BM3 starts to catalyze hydroxylation of nonnative substrates in the presence of inert dummy substrates (decoy molecules). Recently, we have demonstrated that various carboxylic acids modified with amino acids (N-acyl amino acids) having a completely different structure from fatty acids can serve as decoy molecules. Benzene was more efficiently hydroxylated in the presence of these decoy molecules. We also have demonstrated that the heme acquisition protein HasA secreted by Pseudomonas aeruginosa can accommodate Iron(III)-5,15-diphenylporphyrin and its derivatives including Fe-diaza-DPP without any structural perturbation. Crystal structure analysis revealed that phenyl groups at the meso-position of the porphyrins extend outside of HasA to avoid steric crowding and are exposed to the solvent. Iron(III)- and cobalt(III)-tetraphenylporphycenes, which possess bulky phenyl groups, also can be incorporated into HasA.
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| Free Research Field |
生物無機化学
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| Academic Significance and Societal Importance of the Research Achievements |
酸化酵素の一つであるシトクロムP450BM3は、長鎖脂肪酸の水酸化酵素であり、通常は長鎖脂肪酸以外の基質を水酸化することはできないが、基質類似分子（デコイ分子）を取り込ませることで、様々な基質の水酸化が可能になる。共同研究によって、カルボキシル基を持つ様々な化合物がデコイ分子として機能することを見出した。開発した反応系は、有用物質の生産に利用できると期待される。また、緑膿菌のヘム獲得蛋白質HasAに、ヘムとは構造が大きく異なる合成金属錯体が安定に取り込まれることを明らかにすることができた。合成金属錯体を有する人工金属蛋白質開発が大きく進展した。
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