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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Scandium complexes containing beta-diketiminato ligands with pendant phosphanyl groups: competition between Sc/gamma-C [4+2] cycloaddition and Sc/P frustrated Lewis pair reactions
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Scandium complexes containing beta-diketiminato ligands with pendant phosphanyl groups: competition between Sc/gamma-C [4+2] cycloaddition and Sc/P frustrated Lewis pair reactions

机译：含有糊状磷酸β-二酮氨基硅酸盐配体的钪配合物：sc / gamma-c [4 + 2]环加成和sc / p沮丧的lewis对反应之间的竞争

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摘要

Three cationic scandium aryloxide complexes, i. e., [LScOAr](+)[B(C6F5)(4)]-(Ar = 2,6-tBu(2)C(6)H(3); L = CH3C (2,6-iPr(2)C(6)H(3)N)C(R)C(CH3)(N(CH2)(n)CH2PPh2); 6a: n = 1, R = H; 6b: n = 1, R = CH3; 6c: n = 2, R = C6H5CH2), were prepared by a three-step synthetic route. The reactivities of tridentate NNP ligand supported scandium complexes 6 toward various unsaturated substrates were investigated. Treatment of 6a with non-conjugated small molecules such as phenyl isocyanates, phenyl isothiocyanate, and benzaldehyde resulted in formation of Sc/gamma-C [4 + 2] cycloaddition products 7-9 because of nucleophilic reactivity at the beta-diketiminato gamma-Carbon, with retention of Sc center dot center dot center dot P interactions. Analogous Sc/gamma-C [4 + 2] cycloaddition reactions occurred for complex 6b with phenyl isocyanate and phenyl isothiocyanate, affording complexes 10 and 11, respectively. Complex 6c, with a bulky benzyl substituent at the. position of the beta-diketiminato ligand, showed typical Sc/P frustrated Lewis pair (FLP) reactivity toward phenyl isocyanate to give the 1,2-addition product 12. Complex 6c was efficient in the polymerization of gamma-methy-alpha- methylene-gamma-butyrolactone (MMBL). The corresponding initiating species 13, which was formed by Sc/P FLP-type 1,4-addition, was isolated.
机译：三个阳离子钪氧化物复合物，I。即，[LSCOAR]（+）[B（C6F5）（4）] - （Ar = 2,6-TBU（2）C（6）H（3）; L = CH3C（2,6-IPR（2 ）C（6）H（3）N）C（R）C（CH 3）（N（CH 2）（N）CH 2 PPH2）; 6A：N = 1，R = H; 6B：N = 1，R = CH3; 6C：n = 2，r = C6H5CH2）通过三步合成途径制备。研究了三齿NNP配体的反应性支持朝向各种不饱和底物的钪配合物6。用非缀合的小分子处理如苯基异氰酸酯，苯基异硫氰酸酯，苯基异氰酸酯，导致苯甲酸苯甲酸的形成，导致SC /γ-C [4 + 2]环加入产物7-9，因为β-二酮氨基乙酰γ-碳的亲核反应性，保留SC中心点中心点中心点P相互作用。对于苯基异氰酸酯和苯基异硫氰酸苯酯，分别为苯基异氰酸酯和苯基异硫氰酸酯的复合物10和11分别发生类似SC /γ-C [4 + 2]环加成反应。复合物6C，具有庞大的苄基取代基。 Beta-diketiminato配体的位置，显示典型的SC / P令人沮丧的Lewis对（FLP）反对异氰酸酯的反应性，得到1,2-加成的产物12.复合物6c在γ-甲基 - 甲基聚合中有效γ-丁内酯（MMBL）。分离通过SC / P FLP型1,4-加入形成的相应启动物种13。

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