期刊
NATURE CATALYSIS
卷 2, 期 2, 页码 114-122出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/s41929-018-0207-1
关键词
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资金
- University of Strasbourg
- French National Research Agency ('Investments for the future' programme of the IdEx Unistra framework)
- FRC & LabEx Chemistry of Complex Systems
- Polish National Science Centre [2016/20/T/ST5/00494]
- European Union (Marie Curie Actions) through the Campus France [PCOFUND-GA-2013-609102, PRESTIGE-2017-4-0022]
- Polish Ministry of Science and Higher Education [1672/l/MOB/V/l 7/2018/0]
- Foundation for Polish Science [START-036.2018]
Catalytic reactions occur readily at the sites of starting materials that are both innately reactive and sterically accessible, or that are predisposed by a functional group amenable to direct a catalyst. However, selective reactions at unbiased sites of substrates remain challenging and typically require additional preactivation steps or the use of highly reactive reagents. Here we report dual-catalytic transition metal systems that merge a reversible activation cycle with a functionalization cycle, which together enable the functionalization of substrates at their inherently unreactive sites. By engaging the Ru-or Fe-catalysed equilibrium between an alcohol and an aldehyde, methods for Pd-catalysed beta-arylation of aliphatic alcohols and Rh-catalysed gamma-hydroarylation of allylic alcohols were developed. The mild conditions, functional group tolerance and broad scope (81 examples) demonstrate the synthetic applicability of the dual-catalytic systems. This work highlights the potential of the multicatalytic approach to address challenging transformations to circumvent multistep procedures and the use of highly reactive reagents in organic synthesis.
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