Crossed Regio- and Enantioselective Iron-Catalyzed [4+2]-Cycloadditions of Unactivated Dienes

非活化二烯的交叉区域选择性和对映选择性铁催化[4+2]环加成反应

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Abstract

The cyclohexene motif is ubiquitous in nature and specialty chemicals. A straightforward selective access to chiral cyclohexenes from unactivated dienes and dienophiles is not feasible by classical Diels-Alder reaction and constitutes an unsolved synthetic challenge. We report a mild and enantioselective iron-catalyzed cross-[4+2]-cycloaddition of unactivated dienes providing access to chiral 1,3-substituted vinyl-cyclohexenes. The development of bis-dihydroisoquinoline ligands was vital to obtain iron complexes that display high reactivities and excellent chemo-, regio- and enantioselectivities towards the targeted cyclohexenes. A range of diene substrates is well accommodated including feedstocks like butadiene, isoprene and myrcene. The structures of different iron complexes are mapped by X-ray crystallographic analysis and linked to their performance.

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