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Crystal structures of TdsC, a dibenzothiophene monooxygenase from the thermophile Paenibacillus sp A11-2, reveal potential for expanding its substrate selectivity
https://repository.lib.tottori-u.ac.jp/records/7243
https://repository.lib.tottori-u.ac.jp/records/72433adf2cc8-dc46-4cfe-a5f2-d0525e873f2b
| 名前 / ファイル | ライセンス | アクション |
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jbc292(38)_15804.pdf (2.9 MB)
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| Item type | 学術雑誌論文 / Journal Article(1) | |||||
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| 公開日 | 2022-07-22 | |||||
| タイトル | ||||||
| タイトル | Crystal structures of TdsC, a dibenzothiophene monooxygenase from the thermophile Paenibacillus sp A11-2, reveal potential for expanding its substrate selectivity | |||||
| 言語 | en | |||||
| 言語 | ||||||
| 言語 | eng | |||||
| 資源タイプ | ||||||
| 資源タイプ | journal article | |||||
| 著者 |
日野, 智也
× 日野, 智也× 鈴木, 宏和× 八木, 寿梓× 大城, 隆× 永野, 真吾× Hamamoto, Haruka |
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| 著者所属（英） | ||||||
| 言語 | en | |||||
| 値 | Department of Chemistry and Biotechnology, Graduate School of Engineering, Tottori University | |||||
| 著者所属（英） | ||||||
| 言語 | en | |||||
| 値 | Department of Chemistry and Biotechnology, Graduate School of Engineering, Tottori University | |||||
| 著者所属（英） | ||||||
| 言語 | en | |||||
| 値 | Department of Chemistry and Biotechnology, Graduate School of Engineering, Tottori University | |||||
| 著者所属（英） | ||||||
| 言語 | en | |||||
| 値 | Department of Chemistry and Biotechnology, Graduate School of Engineering, Tottori University | |||||
| 著者所属（英） | ||||||
| 言語 | en | |||||
| 値 | Department of Chemistry and Biotechnology, Graduate School of Engineering, Tottori University | |||||
| 著者所属（英） | ||||||
| 言語 | en | |||||
| 値 | Department of Chemistry and Biotechnology, Graduate School of Engineering, Tottori University | |||||
| 抄録 | ||||||
| 内容記述タイプ | Other | |||||
| 内容記述 | Sulfur compounds in fossil fuels are a major source of environmental pollution, and microbial desulfurization has emerged as a promising technology for removing sulfur under mild conditions. The enzyme TdsC from the thermophile Paenibacillus sp. A11-2 is a two-component flavin-dependent monooxygenase that catalyzes the oxygenation of dibenzothiophene (DBT) to its sulfoxide (DBTO) and sulfone (DBTO2) during microbial desulfurization. The crystal structures of the apo and flavin mononucleotide (FMN)-bound forms of DszC, an ortholog of TdsC, were previously determined, although the structure of the ternary substrate–FMN–enzyme complex remains unknown. Herein, we report the crystal structures of the DBT–FMN–TdsC and DBTO–FMN–TdsC complexes. These ternary structures revealed many hydrophobic and hydrogen-bonding interactions with the substrate, and the position of the substrate could reasonably explain the two-step oxygenation of DBT by TdsC. We also determined the crystal structure of the indole-bound enzyme because TdsC, but not DszC, can also oxidize indole, and we observed that indole binding did not induce global conformational changes in TdsC with or without bound FMN. We also found that the two loop regions close to the FMN-binding site are disordered in apo-TdsC and become structured upon FMN binding. Alanine substitutions of Tyr-93 and His-388, which are located close to the substrate and FMN bound to TdsC, significantly decreased benzothiophene oxygenation activity, suggesting their involvement in supplying protons to the active site. Interestingly, these substitutions increased DBT oxygenation activity by TdsC, indicating that expanding the substrate-binding site can increase the oxygenation activity of TdsC on larger sulfur-containing substrates, a property that should prove useful for future microbial desulfurization applications. | |||||
| 書誌情報 |
JOURNAL OF BIOLOGICAL CHEMISTRY en : JOURNAL OF BIOLOGICAL CHEMISTRY 巻 292, 号 38, p. 15804-15813, 発行日 2017-09-22 |
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| 出版者 | ||||||
| 出版者 | American Society for Biochemistry and Molecular Biology | |||||
| DOI | ||||||
| 関連タイプ | isIdenticalTo | |||||
| 識別子タイプ | DOI | |||||
| 関連識別子 | 10.1074/jbc.M117.788513 | |||||
| 権利 | ||||||
| 権利情報 | (C) 2017 by The American Society for Biochemistry and Molecular Biology, Inc. Published in the U.S.A. This is an open access article under the CC BY license. | |||||
| 情報源 | ||||||
| 関連名称 | Hino Tomoya, Hamamoto Haruka, Suzuki Hirokazu, et al. Crystal structures of TdsC, a dibenzothiophene monooxygenase from the thermophile Paenibacillus sp A11-2, reveal potential for expanding its substrate selectivity. JOURNAL OF BIOLOGICAL CHEMISTRY. 2017 | |||||
| 関連サイト | ||||||
| 識別子タイプ | URI | |||||
| 関連識別子 | https://www.sciencedirect.com/science/article/pii/S0021925820340461 | |||||
| 関連名称 | https://www.sciencedirect.com/science/article/pii/S0021925820340461 | |||||
| 著者版フラグ | ||||||
| 出版タイプ | VoR | |||||
| EISSN | ||||||
| 値 | 1083351X | |||||
