WEKO3
アイテム
Concerted Hydrosilylation Catalysis by Silica-Immobilized Cyclic Carbonates and Surface Silanols
http://hdl.handle.net/10131/0002000040
http://hdl.handle.net/10131/0002000040118a5094-826c-4364-9186-5e8ae56a9b2b
| 名前 / ファイル | ライセンス | アクション |
|---|---|---|
jacsau.3c00306.pdf (2.5 MB)
|
.png)
|
| Item type | 学術雑誌論文 / Journal Article(1) | |||||||||||||||||
|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|
| 公開日 | 2023-09-25 | |||||||||||||||||
| タイトル | ||||||||||||||||||
| タイトル | Concerted Hydrosilylation Catalysis by Silica-Immobilized Cyclic Carbonates and Surface Silanols | |||||||||||||||||
| 言語 | en | |||||||||||||||||
| 言語 | ||||||||||||||||||
| 言語 | eng | |||||||||||||||||
| キーワード | ||||||||||||||||||
| 主題 | concerted catalysis, surface immobilization, heterogeneous organocatalyst, cyclic carbonate, hydrosilylation(en) | |||||||||||||||||
| 資源タイプ | ||||||||||||||||||
| 資源タイプ識別子 | http://purl.org/coar/resource_type/c_6501 | |||||||||||||||||
| 資源タイプ | journal article | |||||||||||||||||
| アクセス権 | ||||||||||||||||||
| アクセス権 | open access | |||||||||||||||||
| アクセス権URI | http://purl.org/coar/access_right/c_abf2 | |||||||||||||||||
| 著者 |
Hasegawa, Shingo
× Hasegawa, Shingo
e-Rad_Researcher
40964804
× Nakamura, Keisuke
× Soga, Kosuke
× Usui, Kei
× Manaka, Yuichi
× Motokura, Ken
e-Rad_Researcher
90444067
|
|||||||||||||||||
| 抄録 | ||||||||||||||||||
| 内容記述タイプ | Abstract | |||||||||||||||||
| 内容記述 | Developing a method for creating a novel catalysis of organic molecules is essential because of the growing interest in organocatalysis. In this study, we found that cyclic carbonates immobilized on a nonporous or mesoporous silica support showed catalytic activity for hydrosilylation, which was not observed for the free cyclic carbonates, silica supports, or their physical mixture. Analysis of the effects of linker lengths and pore sizes on the catalytic activity and carbonate C═O stretching frequency revealed that the proximity of carbonates and surface silanols was crucial for synergistic hydrosilylation catalysis. A carbonate and silanol concertedly activated the silane and aldehyde for efficient hydride transfer. Density functional theory calculations on a model reaction system demonstrated that both the carbonate and silanol contributed to the stabilization of the transition state of hydride transfer, which resulted in a reasonable barrier height of 16.8 kcal mol–1. Furthermore, SiO2/carbonate(C4) enabled the hydrosilylation of an aldehyde with an amino group without catalyst poisoning, owing to the weak acidity of surface silanols, in sharp contrast to previously developed acid catalysts. This study demonstrates that immobilization on a solid support can convert inactive organic molecules into active and heterogeneous organocatalysts. | |||||||||||||||||
| 言語 | en | |||||||||||||||||
| 書誌情報 |
en : JACS Au 巻 3, 号 10, p. 2692-2697, ページ数 6, 発行日 2023-09-15 |
|||||||||||||||||
| ISSN | ||||||||||||||||||
| 収録物識別子タイプ | EISSN | |||||||||||||||||
| 収録物識別子 | 26913704 | |||||||||||||||||
| DOI | ||||||||||||||||||
| 関連タイプ | isIdenticalTo | |||||||||||||||||
| 識別子タイプ | DOI | |||||||||||||||||
| 関連識別子 | https://doi.org/10.1021/jacsau.3c00306 | |||||||||||||||||
| 権利 | ||||||||||||||||||
| 言語 | en | |||||||||||||||||
| 権利情報Resource | https://creativecommons.org/licenses/by-nc-nd/4.0/ | |||||||||||||||||
| 権利情報 | Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International | |||||||||||||||||
| 著者版フラグ | ||||||||||||||||||
| 出版タイプ | VoR | |||||||||||||||||
| 出版タイプResource | http://purl.org/coar/version/c_970fb48d4fbd8a85 | |||||||||||||||||
| 出版者 | ||||||||||||||||||
| 出版者 | American Chemical Society (ACS) | |||||||||||||||||
