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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Discrete and polymeric cobalt organophosphates: isolation of a 3-D cobalt phosphate framework exhibiting selective CO2 capture
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Discrete and polymeric cobalt organophosphates: isolation of a 3-D cobalt phosphate framework exhibiting selective CO2 capture

机译：离散的和聚合的有机磷酸钴：分离具有选择性CO2捕集能力的3-D磷酸钴骨架

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摘要

Structurally diverse mononuclear, dinuclear, and tetranuclear cobalt organophosphates and a three-dimensional framework based on a D4R cobalt phosphate are reported. The role of auxiliary ligands in determining the nuclearity of the phosphate clusters has further been established. Reaction of cobalt acetate tetrahydrate with 2,6-di-iso-propylphenylphosphate (dippH(2)) in methanol or DMSO in the presence of ancillary N-donor ligands leads to the formation of mononuclear octahedral cobalt phosphate [Co(dippH)(2)(py)(4)] (1), dinuclear octahedral cobalt phosphates [Co(dipp)(NN)(MeOH)(2)](2)center dot 2MeOH (NN = bpy 2; phen 3), tetrahedral cobalt phosphates [Co(dipp)(L)(2)](2)center dot 2(MeOH) (L = imz 4; dmpz 5) and symmetric and asymmetric tetranuclear tetrahedral cobalt phosphates [Co(dipp)(2-apy)](4) (6) and [Co-4(dipp)(4)(2-apy)(3)(DMSO)]center dot(DMSO)center dot(H2O) (7), in nearly quantitative yields. The use of a linear N-donor ditopic linker, 3,6-di(pyridin-4-yl)-1,2,4,5-tetrazine (dptz), as the ancillary ligand leads to the formation of a robust three dimensional, four-fold interpenetrated network based on the D4R platform, {[Co(dipp) (dptz)(0.5)](4)}(n) (8), under ambient conditions. The new compounds have been characterized by analytical, thermo-analytical and spectroscopic techniques. Further, the molecular structures of compounds 1-8 have been established using single crystal X-ray diffraction studies. Compound 1 is a mononuclear complex in which the dippH ligands occupy trans-positions around the octahedral cobalt ion. The core structure of compounds 2-5, a Co2P2O4 ring, resembles the S4R (single-4-ring) SBU of zeolites, whereas the Co4P4O12 inorganic core found in compounds 6 and 7 resembles the D4R (double-4-ring) SBU. Cobalt organophosphate framework 8 shows significant CO2 adsorption at 273 K (7.73 wt% at 1 bar and 18.21 wt% at 15.5 bar) with high selectivity to CO2 uptake over N-2 and H-2 at 273 K. Magnetic studies of these symmetric complexes indicate the presence of weak antiferromagnetic interactions between the metal ions via the phosphate bridging moiety.
机译：据报道，结构不同的单核，双核和四核钴有机磷酸盐以及基于D4R磷酸钴的三维骨架。辅助配体在确定磷酸酯团簇的核中的作用已进一步确立。乙酸钴四水合物与2,6-二异丙基苯基磷酸酯（dippH（2））在甲醇或DMSO中在辅助N供体配体的存在下反应导致单核八面体磷酸钴[Co（dippH）（2 ）（py）（4）]（1），双核八面体钴磷酸盐[Co（dipp）（NN）（MeOH）（2）]（2）中心点2MeOH（NN = bpy 2; phen 3），四面体钴磷酸盐[Co（dipp）（L）（2）]（2）中心点2（MeOH）（L = imz 4; dmpz 5）以及对称和不对称的四核四面体磷酸钴[Co（dipp）（2-apy）]（ 4）（6）和[Co-4（dipp）（4）（2-apy）（3）（DMSO）]中心点（DMSO）中心点（H2O）（7），产量几乎定量。使用线性N供体双位连接体3,6-二（吡啶-4-基）-1,2,4,5-四嗪（dptz）作为辅助配体会导致形成稳固的三维，在环境条件下基于D4R平台的四重互穿网络{[Co（dipp）（dptz）（0.5）]（4）}（n）（8）。新化合物已通过分析，热分析和光谱技术进行了表征。此外，使用单晶X射线衍射研究已经建立了化合物1-8的分子结构。化合物1是单核络合物，其中dippH配体占据八面体钴离子周围的转位。化合物2-5的核心结构是Co2P2O4环，类似于沸石的S4R（单4环）SBU，而化合物6和7中发现的Co4P4O12无机核则类似于D4R（双4环）SBU。有机磷酸钴骨架8在273 K时表现出显着的CO2吸附（1 bar下为7.73 wt％，在15.5 bar下为18.21 wt％），在273 K下对N-2和H-2的CO2吸收选择性高。表示通过磷酸盐桥联部分在金属离子之间存在弱的反铁磁相互作用。

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