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首页> 外文期刊>Chemistry: A European journal >New insights into cinchonine-aluminium complexes and their application as chiral building blocks: Unprecedented ligand-exchange processes in the presence of ZnR _2 compounds
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New insights into cinchonine-aluminium complexes and their application as chiral building blocks: Unprecedented ligand-exchange processes in the presence of ZnR _2 compounds

机译：辛可宁-铝络合物及其作为手性构件的应用的新见解：存在ZnR _2化合物时空前的配体交换过程

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Previous studies have demonstrated that [(CN) _2AlCl] and [R _2Al(μ-CN)] _2 (CN=deprotonated cinchonine) complexes can effectively act as chiral, semirigid, N,N-ditopic metalloligands for Zn-containing nodes, and provide viable means for constructing new, homochiral, heterometallic, coordination polymers of zigzag and helical topologies. These findings have prompted further investigations on the organometallic analogues of the formula [(CN) _2AlR], anticipating their utility as N,N-metalloligands for ZnR _2 units. Surprisingly, reactions of [(CN) _2AlMe]-type metalloligands with ZnR _2 compounds (R=Me or Et) revealed unprecedented ligand-exchange processes, including zinc-to-aluminium and aluminium-to-zinc transmetalations of alkyl groups. The molecular and crystal structure of the resulting compounds was determined by X-ray diffraction analysis. From the reaction of [(CN) _2AlMe] with ZnMe _2 a new pseudopolymorphic form of a noncovalent porous material based on [Me _2Al(μ-CN)] _2 molecules was isolated. Strikingly, the analogous reaction involving ZnEt _2 led to the generation of a new chiral 4N-tetratopic heterometalloligand [(CN)EtAl(μ-CN) _2ZnEt]. The latter unit was successfully connected by alkyl-exchanged ZnMe 2 nodes to give an original homochiral heterometallic {[(CN)EtAl(μ-CN) _2ZnEt]ZnMe _2} n coordination polymer adopting a snake 1D motif. The outcome of the revealed reactions indicates the complicated multistep reaction route that involves redistribution of cinchonine and alkyl ligands among the Al and Zn centers, and a general reaction scheme is proposed. The results are in strong contrast with the previously studied inorganic-organic [(CN) _2AlCl/ZnCl _2] system, which exclusively affords a helical coordination polymer based on ZnCl _2 nodes and (CN) _2AlCl metalloligands and lacks the exchange of CN ligands.
机译：先前的研究表明，[（CN）_2AlCl]和[R _2Al（μ-CN）] _2（CN =去质子化的辛可宁）络合物可以有效地充当含锌节点的手性，半刚性，N，N-异位金属配体，并且为构建新的，锯齿形和螺旋形拓扑结构的同手性，杂金属，配位聚合物提供了可行的方法。这些发现促进了对式[（CN）_2AlR]的有机金属类似物的进一步研究，预计它们可用作ZnR _2单元的N，N-金属配体。出乎意料的是，[（CN）_2AlMe]型金属配体与ZnR _2化合物（R = Me或Et）的反应显示出空前的配体交换过程，包括烷基的锌到铝和铝到锌的转金属。通过X射线衍射分析确定所得化合物的分子和晶体结构。从[（CN）_2AlMe]与ZnMe _2的反应中，分离出一种新的基于[Me _2Al（μ-CN）] _2分子的非共价多孔材料的假多晶型。引人注目的是，涉及ZnEt _2的类似反应导致了新的手性4N-四位异金属配体[（CN）EtAl（μ-CN）_2ZnEt]的产生。后一个单元通过烷基交换的ZnMe 2节点成功连接，得到具有蛇1D图案的原始同手性异金属{[（CN）EtAl（μ-CN）_2ZnEt] ZnMe _2} n配位聚合物。揭示的反应结果表明复杂的多步反应路线涉及在Al和Zn中心之间重新分布辛可宁和烷基配体，并提出了一种通用的反应方案。结果与先前研究的无机-有机[（CN）_2AlCl / ZnCl _2]系统形成鲜明对比，该系统仅提供基于ZnCl _2节点和（CN）_2AlCl金属配体的螺旋配位聚合物，并且缺乏CN配体的交换。

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