1,721,040 research outputs found

    Ruthenium‐Catalyzed Remote‐Difunctionalization of Nonactivated Alkenes for Double meta‐C(sp2)−H/C‐6(sp3)−H Functionalization

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    Twofold distal C−H functionalization was accomplished by difunctionalization of nonactivated alkenes to provide rapid access to multifunctionalized molecules. The multicomponent ruthenium-catalyzed remote 1,n-difunctionalization (n=6,7) of nonactivated alkenes with fluoroalkyl halides and heteroarenes in a modular manner is reported. The meta-C(sp2)−H/C-6(sp3)−H distal functionalization featured mild conditions, unique selectivity, and broad substrate scope with a domino process for twofold remote C(sp2)−H/C(sp3)−H activation of the sequential formation of three different carbon-centered radicals. A plausible mechanism was proposed based on detailed experimental and computational studies.European Research Council http://dx.doi.org/10.13039/501100000781DFG http://dx.doi.org/10.13039/501100001659Alexander von Humboldt-Stiftung http://dx.doi.org/10.13039/100005156China Sponsorship Council http://dx.doi.org/10.13039/50110000454

    Ruthenaphoto-catalyzed ortho-C−H alkylation with secondary alkyl halides: SET-enabled ruthenium(II/III/IV) manifold

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    http://dx.doi.org/10.13039/100019180 HORIZON EUROPE European Research Councilhttp://dx.doi.org/10.13039/501100001659 German Research Foundationhttp://dx.doi.org/10.13039/501100004543 China Scholarship Councilhttp://dx.doi.org/10.13039/501100000781 European Research Councilhttp://dx.doi.org/10.13039/100005156 Alexander von Humboldt-Stiftun

    )−H‐Funktionalisierung

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    Abstract Die zweifache distale C−H‐Funktionalisierung wurde durch Difunktionalisierung von nicht aktivierten Alkenen erreicht, um einen schnellen Zugang zu hochfunktionalisierten Molekülen zu ermöglichen. Wir berichten hier über die Mehrkomponten‐Ruthenium‐katalysierte 1,n‐Ferndifunktionalisierung ( n =6,7) von nicht aktivierten Alkenen mit Fluoralkylhalogeniden und Heteroarenen in modularer Weise. Die distale meta ‐C(sp 2 )−H/C‐6(sp 3 )−H‐Funktionalisierung zeichnete sich durch milde Bedingungen, einzigartige Selektivität und einen breiten Substratbereich mit einem Domino‐Prozess für die zweifache C(sp 2 )−H/C(sp 3 )−H‐Fernaktivierung der sequentiellen Bildung von drei verschiedenen kohlenstoff‐zentrierten Radikalen aus. Auf der Grundlage detaillierter experimenteller und rechnerischer Studien wurde ein plausibler Mechanismus vorgeschlagen.European Research Council https://doi.org/10.13039/501100000781Deutsche Forschungsgemeinschaft https://doi.org/10.13039/501100001659Alexander von Humboldt-Stiftung https://doi.org/10.13039/100005156China Scholarship Council https://doi.org/10.13039/50110000454

    Elektrooxidative Rhodium‐katalysierte [5+2]‐Anellierung durch C‐H/O‐H‐Aktivierung

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    DFG http://dx.doi.org/10.13039/501100001659Alexander von Humboldt-Stiftung http://dx.doi.org/10.13039/100005156China Sponsorship Council (CN

    Photo‐Induced Ruthenium‐Catalyzed Double Remote C(sp(2))−H / C(sp(3))−H Functionalizations by Radical Relay

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    Distal C(sp(2))−H and C(sp(3))−H functionalizations have recently emerged as step‐economical tools for molecular synthesis. However, while the C(sp(2))−C(sp(3)) construction is of fundamental importance, its formation through double remote C(sp(2))−H/C(sp(3))−H activation has proven elusive. By merging the ruthenium‐catalyzed meta‐C(sp(2))−H functionalization with an aliphatic hydrogen atom transfer (HAT) process, we, herein, describe the catalyzed twofold remote C(sp(2))−H/C(sp(3))−H functionalizations via photo‐induced ruthenium‐mediated radical relay. Thus, meta‐C(sp(2))−H arene bonds and remote C(sp(3))−H alkane bonds were activated by a single catalyst in a single operation. This process was accomplished at room temperature by visible light—notably without exogenous photocatalysts. Experimental and computational theory studies uncovered a manifold comprising ortho‐C−H activation, single‐electron‐transfer (SET), 1,n‐HAT (n=5–7) and σ‐activation by means of a single ruthenium(II) catalyst
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