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首页> 外文期刊>Chemistry: A European journal >Alkene Metalates as Hydrogenation Catalysts
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Alkene Metalates as Hydrogenation Catalysts

机译：烯烃金属作为氢化催化剂

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摘要

First-row transition-metal complexes hold great potential as catalysts for hydrogenations and related reductive reactions. Homo- and heteroleptic arene/alkene metalates(1-) (M=Co, Fe) are a structurally distinct catalyst class with good activities in hydrogenations of alkenes and alkynes. The first syntheses of the heteroleptic cobaltates [K([18]crown-6)][Co(η~4-cod)(η~2-styrene)_2] (5) and [K([18]crown-6)][Co(η~4-dct)(η~4-cod)] (6), and the homoleptic complex [K(thf)_2][Co(η~4-dct)_2] (7; dct=dibenzo[a,e]cyclooctatetraene, cod=1,5-cyclooctadiene), are reported. For comparison, two cyclopentadienylferrates(1-) were synthesized according to literature procedures. The isolated and fully characterized monoanionic complexes were competent precatalysts in alkene hydrogenations under mild conditions (2 bar H_2, r.t., THF). Mechanistic studies by NMR spectroscopy, ESI mass spectrometry, and poisoning experiments documented the operation of a homogeneous mechanism, which was initiated by facile redox-neutral π-ligand exchange with the substrates followed by H_2 activation. The substrate scope of the investigated precatalysts was also extended to polar substrates (ketones and imines).
机译：一排型过渡金属配合物作为氢化和相关还原反应的催化剂具有巨大潜力。同源和异烯芳烃/烯烃金属酸盐（1-）（M = CO，Fe）是具有良好的烯烃和炔烃的良好活性的结构上不同的催化剂类。异钴酸盐的第一合成[K（[18]冠-6）] [CO（η〜4-COD）（η〜2-苯乙烯）_2]（5）和[k（[18]冠-6） [Co（η〜4-DCT）（η〜4-cod）]（6）和杂种复合物[K（THF）_2] [CO（η〜4-DCT）_2]（7; DCT = Dibenzo据报道[A，E]环辛法，COD = 1,5-环辛二烯）。为了比较，根据文献程序合成了两个环戊二烯基酯（1-）。分离的和完全表征的单壬酸酯复合物在温和条件下的烯烃氢化（2巴H_2，R.T.，THF）下是烯烃氢化的竞争力。通过NMR光谱，ESI质谱和中毒实验的机械研究记录了均匀机理的操作，其通过与基材的体内氧化还原 - 中性π-配体交换引发，然后通过H_2活化引发。研究的预催化剂的衬底范围也延伸到极性底物（酮和亚胺）。

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