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ESI-MS Studies and Calculations on Second-Generation Grubbs and Hoveyda-Grubbs Ruthenium Olefin Metathesis Catalysts
其他题名电喷雾质谱结合理论计算研究二代Grubbs 以及 Hoveyda?Grubbs烯烃复分解催化剂
Wang HY(王昊阳); YIM WAILEUNG; Guo YL(郭寅龙); METZGER JUERGEN O
2012
发表期刊Organometallics
ISSN0276-7333
卷号31期号:5页码:1627-1634
摘要Electrospray ionization mass spectrometry (ESI-MS) and subsequent MS/MS methods were used to study second-generation Grubbs catalysts 2 and 3 and first- and second-generation Hoveyda-Grubbs catalysts 4 and 5, respectively, as well as the pyridine-tethered Ru carbene catalyst 6. Direct ESI-MS analyses of Ru catalysts 2-6 showed the corresponding radical cations 2(center dot+)-6(center dot+) and the protonated ligand PCy3 and H(2)IMes, respectively. Alkali metal adduct ions 2.M+ and 3.M+ (M = Li, Na, K, Cs) and 4.M+-6.M+ (M = Li, K) could be easily obtained by mixing the CH2Cl2 solution of catalysts 2-6 with the CH3OH solution of alkali-metal chloride using an online microreactor coupled directly to the electrospray ion source of a quadrupole time-of-flight (Q-TOF) mass spectrometer and were studied by collision-induced dissociation (CID). Remarkably, the alkali metal cationized 14-electron Ru complexes 2a.M+ and 3a.M+ formed by dissociation of phosphine from 2 and 3, respectively, were detected directly from solution. The ratio [2a.M]/[2.M+] increased with decreasing Lewis acidity of M+ from Li+ to Cs+. Moreover, theoretical computations were performed on Ru complexes 2, 5, and 6, showing good agreement with experimental X-ray diffraction data and providing more structural information about the alkali metal adduct ions 2.M+, 5.M+, and 6.M+ (M = Li, K) as well as about the 14-electron species 2a, 5a, and 6a and the respective alkali metal adduct ions.
学科领域分析化学
部门归属中科院上海有机化学研究所; 新加坡Inst High Performance Comp; 德国Carl von Ossietzky Univ Oldenburg
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收录类别SCI
语种英语
WOS记录号WOS:000301331200008
引用统计
被引频次:27[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符http://ir.sioc.ac.cn/handle/331003/28665
专题分析化学研究室
通讯作者METZGER JUERGEN O
推荐引用方式
GB/T 7714
Wang HY,YIM WAILEUNG,Guo YL,et al. ESI-MS Studies and Calculations on Second-Generation Grubbs and Hoveyda-Grubbs Ruthenium Olefin Metathesis Catalysts[J]. Organometallics,2012,31(5):1627-1634.
APA 王昊阳,YIM WAILEUNG,郭寅龙,&METZGER JUERGEN O.(2012).ESI-MS Studies and Calculations on Second-Generation Grubbs and Hoveyda-Grubbs Ruthenium Olefin Metathesis Catalysts.Organometallics,31(5),1627-1634.
MLA 王昊阳,et al."ESI-MS Studies and Calculations on Second-Generation Grubbs and Hoveyda-Grubbs Ruthenium Olefin Metathesis Catalysts".Organometallics 31.5(2012):1627-1634.
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