【摘要】 2014年,我们设计合成了一类结构独特的螺环稠合六元环-氮杂卡宾配体(SNHC),并初步证明了该配体比一般的咪唑型五元环氮杂卡宾具有更强的亲核能力和配位能力.在温和条件下, SNHC配体与Ir(Ⅰ)发生快捷的氧化还原配位,生成了含有两个Ir–C共价键的Ir(Ⅲ)钳形有机金属氢化物SNIr-H,产率高达91%.该类配合物在催化C–H活化/C–Si、C–C键形成反应中具有较高的活性和区域选择性,因此有必要合成更多的类似物和衍生物,进一步拓宽并深化该类配合物催化性质研究.本文通过扩展配体类型和Ir–C共价键的杂化模式,进一步转化和衍生该类金属有机配合物.这些化合物为开发新的金属有机试剂、新的催化反应性质提供了物质基础.更多还原

【Abstract】 In 2014, we designed and synthesized a unique spiro-fused six-membered N-heterocyclic carbene(SNHC),and preliminarily proved that it has stronger nucleophilic nature than the widely reported five-membered carbenes.Taking the advantage of these features of SNHC ligand, we have further succeeded in the convenient synthesis of a series of new and maybe more active Ir(Ⅲ) pincer organometallics 2–5 through conventional transformations. Many complexes derived from complex 1 have high catalytic activity in the C–H activation/C–C bond formation reaction. This paper will introduce the conversion and synthesis of organometallic complexes containing multiple Ir–C covalent bonds.These compounds and their analogues will be helpful to develop new organometallic alkylation reagents or new organometallic catalytic reactions. This case is considerably different from the typical coordination strategies and thus provides an alternative synthetic methodology of organometallics.更多还原