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学科主题: 有机化学
题名: Studies on CH(3)CN-assisted decomposition of 1(st) Grubbs catalyst by electrospray ionization tandem mass spectrometry
其他题名: 电喷雾串联质谱研究乙腈促进的第一代烯烃分解反应催化剂的降解反应
作者: Zhao ZX(赵志雄) ; Wang HY(王昊阳) ; Guo YL(郭寅龙)
通讯作者: 王昊阳 ; 郭寅龙
刊名: Rapid Commun. Mass Spectrom.
发表日期: 2011-01-01
卷: 25, 期:22, 页:3401-3410
收录类别: SCI
部门归属: 中科院上海有机化学研究所
英文摘要: The CH(3)CN-assisted decomposition reaction of the 1(st) Grubbs catalyst (1) was studied using electrospray ionization tandem mass spectrometry (ESI-MS/MS). We detected a series of Ru-intermediates and decomposition products by off-line and on-line ESI-MS(/MS) monitoring of the decomposition process. In particular, an on-line microreactor method was applied with ESI-MS/MS to profile the change and relationship of various Ru-intermediates by controlling the reaction within the first 30 s of its time scale. The main fast decomposition mechanism of Ru-catalyst 1 in the presence of CH(3)CN was similar to that proposed by Grubbs, and this was confirmed by detecting the (PhCH(2)PCy(3))(+) ion at m/z 371 as the major decomposition products with ESI-MS. We also studied the time evolution of the transient reactive Ru-intermediate ions step by step with ESI-MS/MS and detected the C-H bond activation products of toluene - dehydrogenated PCy(3), such as P(Cy)(2)(C(6)H(9)), P(Cy)(2)Ph - by analyzing the decomposition reaction solution by gas chromatography (GC)/MS. The mechanism of another minor decomposition pathway involving the phosphine activation of catalyst 1 was proposed on the basis of the ESI-MS(/MS) interception and characterization of the transient reactive Ru-species in the decomposition reaction solution. Finally the coordination effect of the CH(3)CN in assisting the decomposition and stabilizing the transient Ru-complexes is discussed. Copyright (C) 2011 John Wiley & Sons, Ltd.
语种: 英语
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内容类型: 期刊论文
URI标识: http://ir.sioc.ac.cn/handle/331003/20056
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Recommended Citation:
Zhao ZX,Wang HY,Guo YL. Studies on CH(3)CN-assisted decomposition of 1(st) Grubbs catalyst by electrospray ionization tandem mass spectrometry[J]. Rapid Commun. Mass Spectrom.,2011,25(22):3401-3410.
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