期刊
CHEMISTRY-A EUROPEAN JOURNAL
卷 24, 期 57, 页码 15178-15184出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201802886
关键词
C-H bond activation; cooperative reductive elimination; cross dehydrogenative coupling; dehydrogenative amination; trinuclear catalysis
资金
- DFG [SFB/TRR 88, PA 2395/2-1]
- COST Action [CA15106]
- ERC [716136: 2O2ACTIVATION]
- CERCA Programme/Generalitat de Catalunya
- MINECO [CTQ2017-87792-R]
- MINECO (Severo Ochoa Excellence Accreditation 2014-2018) [SEV-2013-0319]
- Severo Ochoa predoctoral training fellowship [SVP-2014-068662]
The mechanism of a trinuclear cooperative dehydrogenative C-N bond-forming reaction is investigated in this work, which avoids the use of chelate-assisting directing groups. Two new highly efficient Ru/Cu co-catalyzed systems were identified, allowing orders of magnitude greater TOFs than the previous state of the art. In-depth kinetic studies were performed in combination with advanced DFT calculations, which reveal a decisive rate-determining trinuclear Ru-Cu cooperative reductive elimination step (CRE).
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