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A neutral germanium/phosphorus frustrated Lewis pair: Synthesis and reactivity
Journal of Organometallic Chemistry ( IF 2.1 ) Pub Date : 2021-09-07 , DOI: 10.1016/j.jorganchem.2021.122071
Qian Yang 1 , Liliang Wang 1 , Yinhuan Li 1 , Linqun Zhou 1 , Zhifang Li 1
Affiliation  

A novel germinal germanium/phosphorus frustrated Lewis pair, Cl3GeCH2PtBu2 1, was prepared through the metathesis reaction of tBu2PCH2Li with tetrachlorogermanium. This neutral germanium-based frustrated Lewis pair 1 exhibits higher reactivity toward a series of small molecules. When 1 was treated with an excess amount of tetrachloromethane (2.3equiv) yielding a zwitterionic adduct 2, Cl4GeCH2P(Cl)tBu2. The cycloaddition of dimethyl but-2-ynedioate with 1 was took place smoothly at room temperature, and afforded a zwitterionic cyclic vinyl 3 in good yields. The reaction of 1 with furan-2,5-dione has also been performed giving the corresponding cycloaddition 4 in high yields. The additions of C=Ch (Ch = O, and S) units involving 1-isocyanato-4-methylbenzene and isothiocyanatobenzene with 1 have been also carried out at ambient temperature in which the five-membered GeCPCO(S)-ring products 5a and 5b were furnished, respectively. All these above-mentioned compounds 1-5 were fully characterized by multinuclear NMR spectroscopy, high-resolution mass spectrometry (HRMS), and the structures of 1 and 3 were also determined by single-crystal X-ray diffraction.



中文翻译:

中性锗/磷受挫路易斯对:合成和反应性

通过t Bu 2 PCH 2 Li与四氯锗的复分解反应制备了一种新型的锗/磷受挫Lewis对Cl 3 GeCH 2 P t Bu 2 1。这种基于中性锗的受挫路易斯对1对一系列小分子表现出更高的反应性。当1用过量的四氯甲烷(2.3当量)处理时产生两性离子加合物2,Cl 4 GeCH 2 P(Cl) t Bu 2。丁-2-炔二酸二甲酯与1在室温下顺利进行,并以良好的产率得到两性离子环状乙烯基31与呋喃-2,5-二酮的反应也已进行,以高产率得到相应的环加成4。涉及 1-异氰酸根合-4-甲基苯和异硫氰酸根合苯与1的 C=Ch(Ch=O,和 S)单元的加成也在室温下进行,其中五元 GeCPCO(S)-环产物5a和分别配备了5b。所有上述化合物1-5均通过多核 NMR 光谱、高分辨率质谱 (HRMS) 和结构图 1和图3也通过单晶 X 射线衍射测定。

更新日期:2021-09-16
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