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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Interplay between H- bonding and interpenetration in an aqueous copper( II)- aminoalcoholpyromellitic acid system: self- assembly synthesis, structural features and catalysis
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Interplay between H- bonding and interpenetration in an aqueous copper( II)- aminoalcoholpyromellitic acid system: self- assembly synthesis, structural features and catalysis

机译：在铜（II）水溶液中的H键合和互持续间相互作用 - 氨基醇脲酰基脲酸系统：自组装合成，结构特征和催化

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Two new copper(ii) coordination compounds, [Cu(H(1.5)mdea)(2)](2)(H(2)pma) (1a) and [{Cu-2(-Hmdea)(2)}(2)((4)-pma)](n)2nH(2)O (1b), were self-assembled at different temperatures from the same multicomponent reaction system, comprising copper(ii) nitrate, N-methyldiethanolamine (H(2)mdea), pyromellitic acid (H(4)pma), and potassium hydroxide. Products 1a and 1b were isolated as microcrystalline solids and fully characterized and their structures were established by single-crystal X-ray diffraction. Compound 1a features the bis-aminoalcohol(ate) monocopper(ii) units and H(2)pma(2-) anions that are multiply interconnected by strong H-bonds into a firm 2D H-bonded layer. Compound 1b reveals the bis-aminoalcoholate dicopper(ii) motifs that are interlinked by the (4)-pma(4-) spacers into a 3D + 3D interpenetrated metal-organic framework. From a topological perspective, both networks of 1a and 1b are uninodal and driven by similar 4-connected H(2)pma(2-) or pma(4-) nodes, but result in distinct sql and dia topologies, respectively. Compound 1a was applied as an efficient catalyst for two model cycloalkane functionalization reactions: (1) oxidation by H2O2 to form cyclic alcohols and ketones and (2) hydrocarboxylation by CO/H2O and S2O82- to form cycloalkanecarboxylic acids. The substrate scope, effects of various reaction parameters, selectivity and mechanistic features were also investigated.
机译：两种新的铜（II）配位化合物，[Cu（1.5）MDEA）（2）]（2）（2）（H（2）PMA）（1A）和[{Cu-2（-Hmdea）（2）}（ 2）（（4）-PMA）]（N）2NH（2）O（1B），在来自相同多组分反应体系的不同温度下自组装，其包含铜（II）硝酸N-甲基二乙醇胺（H（2 ）MDEA），吡罗密酸（H（4）PMA）和氢氧化钾。将产物1A和1B分离为微晶固体并充分表征，并通过单晶X射线衍射建立它们的结构。化合物1A具有双氨基醇（ATE）单眼醇（II）单位（II）单位和H（2）PMA（2）个阴离子，其通过强H键与固体2D H键合层乘以互连。化合物1b显示由（4）-pma（4-）间隔物相互连接的双氨基醇二滴体（II）基序列在3D + 3D互渗透金属 - 有机骨架中。从拓扑角度来看，1A和1B的网络都是单向的，并由相似的4连接的H（2）PMA（2-）或PMA（4-）节点驱动，但分别导致不同的SQL和DIA拓扑。将化合物1a作为两种型号环烷烃官能化反应的有效催化剂施用：（1）通过H 2 O 2氧化以形成环状醇和酮通过CO / H 2 O和S2O82-形成环烷基化以形成环烷基羧酸。还研究了基板范围，各种反应参数，选择性和机械特征的效果。

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