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首页> 外文期刊>RSC Advances >An unknown component of a selective and mild oxidant: structure and oxidative ability of a double salt-type complex having κ1O-coordinated permanganate anions and three- and four-fold coordinated silver cations
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An unknown component of a selective and mild oxidant: structure and oxidative ability of a double salt-type complex having κ1O-coordinated permanganate anions and three- and four-fold coordinated silver cations

机译：选择性和弱氧化剂的未知成分：具有κ1O配位的高锰酸根阴离子和三倍和四倍配位的银阳离子的双盐型配合物的结构和氧化能力

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Compounds containing redox active permanganate anions and complexed silver cations with reducing pyridine ligands are used not only as selective and mild oxidants in organic chemistry but as precursors for nanocatalyst synthesis in low-temperature solid-phase quasi-intramolecular redox reactions. Here we show a novel compound (4Agpy _(2) MnO _(4) ·Agpy _(4) MnO _(4) ) that has unique structural features including (1) four coordinated and one non-coordinated permanganate anion, (2) κ ~(1) O-permanganate coordinated Ag, (3) chain-like [Ag(py) _(2) ] ~(+) units, (4) non-coordinated ionic permanganate ions and an [Ag(py) _(4) ] ~(+) tetrahedra as well as (5) unsymmetrical hydrogen bonds between pyridine α-CHs and a permanganate oxygen. As a result of the oxidizing permanganate anion and reducing pyridine ligand, a highly exothermic reaction occurs at 85 °C. If the decomposition heat is absorbed by alumina or oxidation-resistant organic solvents (the solvent absorbs the heat to evaporate), the decomposition reaction proceeds smoothly and safely. During heating of the solid material, pyridine is partly oxidized into carbon dioxide and water; the solid phase decomposition end product contains mainly metallic Ag, Mn _(3) O _(4) and some encapsulated carbon dioxide. Surprisingly, the enigmatic carbon-dioxide is an intercalated gas instead of the expected chemisorbed carbonate form. The title compound is proved to be a mild and efficient oxidant toward benzyl alcohols with an almost quantitative yield of benzaldehydes.
机译：含有氧化还原活性高锰酸根阴离子和带有还原吡啶配体的复合银阳离子的化合物不仅在有机化学中用作选择性氧化剂和弱氧化剂，而且还用作低温固相准分子间氧化还原反应中纳米催化剂合成的前体。在这里我们展示了一种新型化合物（4Agpy _（2）MnO _（4）·Agpy _（4）MnO _（4）），它具有独特的结构特征，包括（1）四个配位和一个不配位的高锰酸根阴离子，（2 ）κ〜（1）O-高锰酸盐配位的Ag，（3）链状[Ag（py）_（2）]〜（+）单位，（4）非配位的离子高锰酸盐离子和[Ag（py） _（4）]〜（+）四面体以及吡啶α-CHs和高锰酸盐氧之间的（5）不对称氢键。由于高锰酸根阴离子的还原和吡啶配体的还原，在85°C时发生了放热反应。如果分解热被氧化铝或抗氧化的有机溶剂吸收（溶剂吸收了热量蒸发），则分解反应平稳而安全地进行。在加热固体材料的过程中，吡啶被部分氧化为二氧化碳和水。固相分解终产物主要包含金属Ag，Mn _（3）O _（4）和一些封装的二氧化碳。令人惊讶的是，神秘的二氧化碳是一种插层气体，而不是预期的化学吸附的碳酸盐形式。事实证明该标题化合物是对苄醇的温和而有效的氧化剂，几乎定量地产生了苯甲醛。

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