Department of Chemistry and Biochemistry, Florida International University, Miami, Florida 33199, USA.
J Org Chem. 2010 Dec 3;75(23):8199-212. doi: 10.1021/jo101848f. Epub 2010 Nov 10.
The trichlorophenyl-, dichlorodiphenyl-, and chlorotriphenylgermanes undergo Pd-catalyzed cross-couplings with aryl bromides and iodides in the presence of tetrabutylammonium fluoride in toluene with addition of the measured amount of water. One chloride ligand on the Ge center allows efficient activation by fluoride to promote transfer of one, two, or three phenyl groups from the organogermanes. The corresponding chlorophenylstannanes were found to be more reactive than chlorophenylsilanes, which in turn were more effective than chlorophenylgermanes. One chloride ligand on the Ge or Si center allows efficient activation by fluoride to promote transfer of up to three aryl groups from germane or silicon. However, no haloligand was necessary to be present on the Sn center, since tetraphenyltin efficiently transferred up to four phenyl groups during fluoride-promoted couplings with aryl halides. (19)F NMR studies suggested formation of the fluorophenylgermanes and the hypervalent germanate species as possible intermediates.
三氯苯基、二氯二苯基和氯三苯基锗在四丁基氟化铵存在下,在甲苯中与芳基溴化物和碘化物发生 Pd 催化交叉偶联反应,并加入适量的水。锗中心上的一个氯配体允许氟化物有效活化,促进从有机锗中转移一个、两个或三个苯基。发现相应的氯苯基锡烷比氯苯基硅烷更具反应性,而氯苯基硅烷又比氯苯基锗更有效。锗或硅中心上的一个氯配体允许氟化物有效活化,从而促进从锗或硅中转移多达三个芳基基团。然而,锡中心上不需要存在卤配体,因为四苯基锡在氟化物促进的与芳基卤化物的偶联反应中能够有效地转移多达四个苯基。(19)F NMR 研究表明,形成氟苯基锗和高价锗酸盐作为可能的中间体。