Alcohol Amination with Ammonia Catalyzed by an Acridine-Based Ruthenium Pincer Complex: A Mechanistic Study
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- 作者：Xuan Ye ; Philipp N. Plessow ; Marion K. Brinks ; Mathias Schelwies ; Thomas Schaub ; Frank Rominger ; Rocco Paciello ; Michael Limbach ; Peter Hofmann
- 刊名：Journal of the American Chemical Society
- 出版年：2014
- 出版时间：April 23, 2014
- 年：2014
- 卷：136
- 期：16
- 页码：5923-5929
- 全文大小：519K
- 年卷期：v.136,no.16(April 23, 2014)
- ISSN：1520-5126
文摘
The mechanistic course of the amination of alcohols with ammonia catalyzed by a structurally modified congener of Milstein鈥檚 well-defined acridine-based PNP-pincer Ru complex has been investigated both experimentally and by DFT calculations. Several key Ru intermediates have been isolated and characterized. The detailed analysis of a series of possible catalytic pathways (e.g., with and without metal鈥搇igand cooperation, inner- and outer-sphere mechanisms) leads us to conclude that the most favorable pathway for this catalyst does not require metal鈥搇igand cooperation.