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Organosilicon compounds meet subatomic physics: Muon spin resonance
West, Robert,Percival, Paul W. Royal Society of Chemistry 2010 Dalton transactions Vol.39 No.39
<P>Silylenes, germylenes and silenes react with muonium atoms, produced from muons generated at a particle accelerator. The resulting radicals can be studied by muon spin resonance spectroscopy, providing unique information about their structure and reactivity.</P> <P>Graphic Abstract</P><P>Stable silylenes, germylenes and silenes capture muonium atoms and are studied by muon spin resonance spectroscopy, with novel results. <IMG SRC='http://pubs.rsc.org/services/images/RSCpubs.ePlatform.Service.FreeContent.ImageService.svc/ImageService/image/GA?id=c0dt00188k'> </P>
Sheberla, Dennis,Tumanskii, Boris,Tomasik, Adam C.,Mitra, Amitabha,Hill, Nicholas J.,West, Robert,Apeloig, Yitzhak Royal Society of Chemistry 2010 Chemical Science Vol.1 No.2
<P>Stable <I>N</I>-heterocyclic carbenes and germylenes were allowed to react with a phosphonyl radical, (<I>i</I>-PrO)<SUB>2</SUB>(O)P&z.rad; (<B>7</B>), generated by photolysis of [(<I>i</I>-PrO)<SUB>2</SUB>(O)P]<SUB>2</SUB>Hg. The products were identified by EPR spectroscopy. An unsaturated carbene (<B>1</B>) and germylene (<B>3</B>) react with <B>7</B> at the divalent atom to give unstable radical products (<I>τ</I><SUB>½</SUB> = 0.2 s). A benzo-annulated carbene (<B>4</B>) and a saturated germylene (<B>6</B>) react with <B>7</B> to give more active radicals. An unsaturated (<B>2</B>) and a saturated silylene (<B>5</B>) undergo rapid reaction (in the dark) with [(<I>i</I>-PrO)<SUB>2</SUB>(O)P]<SUB>2</SUB>Hg to yield unusual silyl phosphites. In these cases only secondary radicals were observed. DFT (PBE0/TZVP//B3LYP/6-31+G(d)) calculations of the radical adducts of the different (C, Si, Ge) unsaturated <I>N</I>-heterocyclic divalent species with the phosphonyl radical show that the unpaired electron is delocalized over the five-membered ring; the spin density on the central atoms decreases in the order C, 39% > Si, 14% > Ge, 2%. These trends can be understood in terms of a zwitterionic structure of the radical adducts. The calculations of the radical adducts of <B>4</B>, <B>5</B> and <B>6</B> with <B>7</B> indicate larger spin density on the central atom, 47%, 58% and 42% on C, Si, Ge, respectively.</P> <P>Graphic Abstract</P><P>The geometry, spin density distribution and reactivity of radical adducts of stable <I>N</I>-heterocyclic carbenes, silylenes and germylenes demonstrate a strong dependence on the nature of the heterocycle and on the central atom. <IMG SRC='http://pubs.rsc.org/services/images/RSCpubs.ePlatform.Service.FreeContent.ImageService.svc/ImageService/image/GA?id=c0sc00143k'> </P>
Zhang, Lingzhi,Lyons, Leslie,Newhouse, Jocelyn,Zhang, Zhengcheng,Straughan, Megan,Chen, Zonghai,Amine, Khalil,Hamers, Robert J.,West, Robert Royal Society of Chemistry 2010 Journal of materials chemistry Vol.20 No.38
<P>Alkylsilane ethers, containing one or three carbon spacer groups between the silicon atom and oligo(ethylene oxide) moiety, were designed and synthesized. These compounds are non-hydrolyzable and less flammable than their alkoxysilane counterparts. A full cell test using them as electrolyte solvents showed good cycling performance in lithium-ion batteries.</P> <P>Graphic Abstract</P><P>Alkylsilane ethers with oligo(ethylene oxide) substituents were designed and synthesized as safe electrolyte solvents which showed good cycling performance doped with LiBOB in lithium-ion cells. <IMG SRC='http://pubs.rsc.org/services/images/RSCpubs.ePlatform.Service.FreeContent.ImageService.svc/ImageService/image/GA?id=c0jm01596b'> </P>