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Formation of macrocyclic ring systems by carbonylation of trifunctional P/B/B frustrated Lewis pairs†
Chemical Science ( IF 7.6 ) Pub Date : 2017-12-14 00:00:00 , DOI: 10.1039/c7sc04394e Long Wang 1 , Shunxi Dong 1 , Constantin G Daniliuc 1 , Lei Liu 2 , Stefan Grimme 2 , Robert Knitsch 3 , Hellmut Eckert 3, 4 , Michael Ryan Hansen 3 , Gerald Kehr 1 , Gerhard Erker 1
Chemical Science ( IF 7.6 ) Pub Date : 2017-12-14 00:00:00 , DOI: 10.1039/c7sc04394e Long Wang 1 , Shunxi Dong 1 , Constantin G Daniliuc 1 , Lei Liu 2 , Stefan Grimme 2 , Robert Knitsch 3 , Hellmut Eckert 3, 4 , Michael Ryan Hansen 3 , Gerald Kehr 1 , Gerhard Erker 1
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The trifunctional P/B/B frustrated Lewis pairs 11a–c featuring bulky aryl groups at phosphorus [Dmesp (a), Tipp (b), Mes* (c)] react with H2 by heterolytic hydrogen splitting followed by cleavage of HB(C6F5)2 to give the zwitterionic six-membered heterocyclic PH phosphonium/borate products 14a–c. Compounds 11a,b react with carbon monoxide by means of a Lewis acid induced CO insertion/rearrangement sequence that eventually results in the formation of the macrocyclic dimers 17a,b. The respective carbonylation reaction of the Mes*P/B/B FLP gives the macrocyclic trimer 18c. The new products were characterized spectroscopically and by X-ray diffraction and the reaction mechanism was analyzed by DFT calculations.
中文翻译：
通过三官能 P/B/B 受阻路易斯对的羰基化形成大环系统†
三官能 P/B/B 受阻的路易斯对11a–c在磷上具有庞大的芳基 [Dmesp ( a ), Tipp ( b ), Mes* ( c )] 与 H 2通过异解氢裂解反应，然后裂解 HB( C 6 F 5 ) 2得到两性离子六元杂环 PH 鏻/硼酸盐产物14a–c。化合物11a、b通过路易斯酸诱导的CO插入/重排顺序与一氧化碳反应，最终形成大环二聚体17a、b。Mes*P/B/B FLP的各自的羰基化反应得到大环三聚体18c。对新产物进行了光谱和X射线衍射表征，并通过DFT计算分析了反应机理。
更新日期：2017-12-14
中文翻译：
通过三官能 P/B/B 受阻路易斯对的羰基化形成大环系统†
三官能 P/B/B 受阻的路易斯对11a–c在磷上具有庞大的芳基 [Dmesp ( a ), Tipp ( b ), Mes* ( c )] 与 H 2通过异解氢裂解反应，然后裂解 HB( C 6 F 5 ) 2得到两性离子六元杂环 PH 鏻/硼酸盐产物14a–c。化合物11a、b通过路易斯酸诱导的CO插入/重排顺序与一氧化碳反应，最终形成大环二聚体17a、b。Mes*P/B/B FLP的各自的羰基化反应得到大环三聚体18c。对新产物进行了光谱和X射线衍射表征，并通过DFT计算分析了反应机理。
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