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- 저자 : LOTHAR DUNSCH (검색결과 2 건)
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SPECTROELECTROCHEMICAL RECOGNITION OF CHEMICAL DOPANTS IN THE INNER SPACE OF CARBON NANOSTRUCTURES
MARTIN KALBÁČ,LADISLAV KAVAN,MARKÉTA ZUKALOVÁ,LOTHAR DUNSCH 성균관대학교(자연과학캠퍼스) 성균나노과학기술원 2006 NANO Vol.1 No.3
By in situ Raman spectroelectrochemistry the state of chemical dopants in the inner space of potassium vapor treated single-walled carbon nanotubes (SWCNT), double-walled carbon nanotubes (DWCNT) and C60 fullerene peapods was followed. We show that the spectroelectrochemistry is a method of choice to locate the dopant within carbon nanostructures. The presence of potassium inside the carbon nanostructures was found to be associated with a characteristic response of the tangential (TG) mode of SWCNT to electrochemical doping after treatment of the sample with the water. Our study confirmed the presence of residual potassium in peapods even after treatment with water. On the other hand, potassium was not found in the interior of the water-treated DWCNT and SWCNT.
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Popov, Alexey A.,Schiemenz, Sandra,Avdoshenko, Stanislav M.,Yang, Shangfeng,Cuniberti, Gianaurelio,Dunsch, Lothar American Chemical Society 2011 JOURNAL OF PHYSICAL CHEMISTRY C - Vol.115 No.31
<P>While the role of asymmetric nitride clusters on the cage size and symmetry in fullerene-based structures is already well-known, the role of the asymmetric arrangement of metals in nitride clusters on the nitrogen is studied in detail in this work. It is discovered that asymmetric mixed-metal nitride clusters give sufficiently narrow <SUP>14</SUP>N NMR signals to make NMR the method of choice to characterize the endohedral cluster from the inside. In the series of mixed-metal nitride clusterfullerenes Lu<SUB><I>x</I></SUB>Sc<SUB>3–<I>x</I></SUB>N@C<SUB>80</SUB> and Lu<SUB><I>x</I></SUB>Y<SUB>3–<I>x</I></SUB>N@C<SUB>80</SUB> (<I>x</I> = 0–3) the δ(<SUP>14</SUP>N) values are found to be linear functions of <I>x</I> showing that <SUP>14</SUP>N chemical shifts are additive values with specific increment for each kind of metal atoms. Density functional theory calculations are performed to interpret the experimentally measured spectra. To reveal the main factors affecting <SUP>14</SUP>N chemical shifts in nitride clusterfullerenes, shielding tensor components are analyzed in terms of Ramsey theory both in localized and canonical molecular orbitals. <SUP>14</SUP>N chemical shifts in M<SUB>3</SUB>N@C<SUB>80</SUB> and related systems are shown to be determined solely by nitrogen-localized orbitals and in particular by the p<SUB><I>x,y,z</I></SUB> atomic orbitals of nitrogen. As a result, the peculiarities of the nitrogen shielding in nitride clusterfullerenes can be interpreted by the simple analysis of the nitrogen-projected density of states and its variation in different chemical environments.</P><P><B>Graphic Abstract</B> <IMG SRC='http://pubs.acs.org/appl/literatum/publisher/achs/journals/content/jpccck/2011/jpccck.2011.115.issue-31/jp204290f/production/images/medium/jp-2011-04290f_0004.gif'></P>
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