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Formation of unprecedented actinide carbon triple bonds in uranium methylidyne molecules
Lyon, Jonathan T. ; Hu, Han-Shi ; Andrews, Lester ; Li, Jun
2010-05-06 ; 2010-05-06
关键词actinide multiple bond heavy element laser ablation matrix isolation relativistic quantum chemistry TRANSITION-METAL-COMPLEXES INFRARED-SPECTRA ELECTRON LOCALIZATION MOLYBDENUM ATOMS STABLE COMPOUND QUINTUPLE BOND LOW-COORDINATE W ATOMS CHEMISTRY INTERCONVERSION Multidisciplinary Sciences
中文摘要Chemistry of the actinide elements represents a challenging yet vital scientific frontier. Development of actinide chemistry requires fundamental understanding of the relative roles of actinide valence-region orbitals and the nature of their chemical bonding. We report here an experimental and theoretical investigation of the uranium methylidyne molecules X3U CH (X = F, Cl, Br), F2ClU CH, and F3U CF formed through reactions of laser-ablated uranium atoms and trihalomethanes or carbon tetrafluoride in excess argon. By using matrix infrared spectroscopy and relativistic quantum chemistry calculations, we have shown that these actinide complexes possess relatively strong U C triple bonds between the U 6d-5f hybrid orbitals and carbon 2s-2p orbitals. Electron-withdrawing ligands are critical in stabilizing the U(VI) oxidation state and sustaining the formation of uranium multiple bonds. These unique U C-bearing molecules are examples of the long-sought actinide-alkylidynes. This discovery opens the door to the rational synthesis of triple-bonded actinide-carbon compounds.
语种英语 ; 英语
出版者NATL ACAD SCIENCES ; WASHINGTON ; 2101 CONSTITUTION AVE NW, WASHINGTON, DC 20418 USA
内容类型期刊论文
源URL[http://hdl.handle.net/123456789/10586]  
专题清华大学
推荐引用方式
GB/T 7714
Lyon, Jonathan T.,Hu, Han-Shi,Andrews, Lester,et al. Formation of unprecedented actinide carbon triple bonds in uranium methylidyne molecules[J],2010, 2010.
APA Lyon, Jonathan T.,Hu, Han-Shi,Andrews, Lester,&Li, Jun.(2010).Formation of unprecedented actinide carbon triple bonds in uranium methylidyne molecules..
MLA Lyon, Jonathan T.,et al."Formation of unprecedented actinide carbon triple bonds in uranium methylidyne molecules".(2010).
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