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首页> 外文期刊>Crystal growth & design >Binding of polyatomic anions with protonated ureido-pyridyl ligands
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Binding of polyatomic anions with protonated ureido-pyridyl ligands

机译：多原子阴离子与质子化的脲基-吡啶基配体的结合

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摘要

Two ureido-pyridyl ligands, 1-(4-nitro-phenyl)-3-pyridine-3-ylmethyl-urea (L~1) and 1-pentafluorophenyl-3-pyridine-4-yl-urea (L~2) were synthesized in good yields, and solid-state anion binding studies of (HL~1)~+ and (HL~2)~+ with polyatomic anions such as NO_3~-, AcO~-, ClO_4~-, SO_4~(2-), and SiF_6~(2-) were carried out in detail. Protonation of the pyridyl nitrogen center of L ~1 with HNO_3, HClO_4, and HF in different solvent media yielded crystals of complexes 1 (HL~1 · NO_3), _2 (HL~1 · ClO_4), and 3 (HL~1 · 0.5SiF_6) suitable for single crystal X-ray diffraction studies, respectively. Similarly, protonation of L~2 with HNO_3, CH_3COOH, and H_2SO_4 yielded single crystals of complexes 4 [2(HL~2 · NO_3) ·DMF], 5 (HL ~2 · AcO), and 6 [(HL~2)_2 · SO _4], respectively. X-ray crystallographic analysis of all these six complexes has been carried out and the details of anion binding with the urea functionality of ureido-pyridyl ligands were investigated. In all the complexes, the pyridyl moiety of the ligands is found to be protonated and the binding of anions are observed at the urea functionality of the ligands through the R _2~2(8) hydrogen bonding motif irrespective of sizes and shapes of anions or the electron withdrawing ability of aryl substitutions (p-nitro phenyl vs pentafluoro phenyl) or the position of the pyridyl nitrogen center (protonation site) of the designed ligands.
机译：两个脲基-吡啶基配体是1-（4-硝基-苯基）-3-吡啶-3-基甲基脲（L〜1）和1-五氟苯基-3-吡啶-4-基脲（L〜2） （HL〜1）〜+和（HL〜2）〜+与多原子阴离子如NO_3〜-，AcO〜-，ClO_4〜-，SO_4〜（2- ），并详细进行SiF_6〜（2-）。在不同的溶剂介质中用HNO_3，HClO_4和HF对L〜1的吡啶氮中心进行质​​子化反应，生成了配合物1（HL〜1·NO_3），_ 2（HL〜1·ClO_4）和3（HL〜1· 0.5SiF_6）分别适用于单晶X射线衍射研究。同样，用HNO_3，CH_3COOH和H_2SO_4对L〜2进行质子化处理，生成的复合物为4 [2（HL〜2·NO_3）·DMF]，5（HL〜2·AcO）和6 [（HL〜2） _2·SO _4]。已经对所有这六个络合物进行了X射线晶体学分析，并研究了阴离子与脲基-吡啶基配体的尿素官能团结合的细节。在所有配合物中，发现配体的吡啶基部分被质子化，并且通过R _2〜2（8）氢键基序在配体的尿素官能团处观察到阴离子的结合，而与阴离子的大小和形状无关。芳基取代基（对硝基苯基对五氟苯基）的吸电子能力或所设计配体的吡啶基氮中心位置（质子化位点）。

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