Gold-Catalyzed Cyclizations of 4-Alkyl-2-yn-1-yl (Oxy)cyclohexa-2,5-dien-1-ones (1) to Develop Two Cyclizations via π-Alkyne versus π-Allene Activations

金催化4-烷基-2-炔-1-基(氧代)环己-2,5-二烯-1-酮(1)的环化反应,通过π-炔烃活化和π-丙二烯活化开发两种环化反应

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Abstract

This work reports two new gold-catalyzed cyclizations of 4-alkyl-2-yn-1-yl (oxy)cyclohexa-2,5-dien-1-ones (1) via gold-π-allene versus gold-π-alkyne routes, The π-allene route involves a [3.3] Claisen rearrangement of 1-alloxyallene intermediates to enable a 1,3-group migration, ultimately affording 2-substituted 3-formylbenzofurans (2). Density functional theory (DFT) calculations support this proposed mechanism in which water plays a key role. An alternative π-alkyne route contains cocatalyst PhNH(2) (10 mol %), leading to the formation of C(3,4)-fused tetrahydrobenzofuran-5(4H)-ones (3) stereoselectively.

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