Beijing National Laboratory for Molecular Sciences (BNLMS), Key Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of Education, College of Chemistry, Peking University, Beijing, 100871, China.
State Key Laboratory of Elemento-Organic Chemistry, Nankai University, Tianjin, 300071, P.R. China.
Angew Chem Int Ed Engl. 2016 Aug 1;55(32):9187-90. doi: 10.1002/anie.201602790. Epub 2016 Jun 15.
The selective construction of P-C bonds directly from P4 and nucleophiles is an ideal and step-economical approach to utilizing elemental P4 for the straightforward synthesis of organophosphorus compounds. In this work, a highly efficient one-pot reaction between P4 and 1,4-dilithio-1,3-butadienes was realized, which quantitatively affords phospholyl lithium derivatives. DFT calculations indicate that the mechanism is significantly different from that of the well-known stepwise cleavage of P-P bond in P4 activation. Instead, a cooperative nucleophilic attack of two Csp2 Li bonds on P4 , leading to simultaneous cleavage of two P-P bonds, is favorable. This mechanistic information offers a new view on the mechanism of P4 activation, as well as a reasonable explanation for the excellent yields and selectivity. This method could prove to be a useful route to P4 activation and the subsequent production of organophosphorus compounds.
直接从 P4 和亲核试剂选择性构建 P-C 键是利用元素 P4 直接合成有机磷化合物的理想且经济的方法。在这项工作中,实现了 P4 和 1,4-二锂-1,3-丁二烯之间的高效一锅反应,定量得到了膦基锂衍生物。DFT 计算表明,该机理与 P4 活化中众所周知的逐步 P-P 键断裂机理显著不同。相反,两个 Csp2 Li 键对 P4 的协同亲核进攻有利于同时断裂两个 P-P 键。这种机理信息为 P4 活化的机理提供了新的视角,也为优异的产率和选择性提供了合理的解释。该方法可能是一种有用的 P4 活化和随后合成有机磷化合物的途径。