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RISS 인기검색어
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- 저자 : Yokoyama Atsutoshi (검색결과 2 건)
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Chromium(IV)–Peroxo Complex Formation and Its Nitric Oxide Dioxygenase Reactivity
Yokoyama, Atsutoshi,Han, Jung Eun,Cho, Jaeheung,Kubo, Minoru,Ogura, Takashi,Siegler, Maxime A.,Karlin, Kenneth D.,Nam, Wonwoo American Chemical Society 2012 JOURNAL OF THE AMERICAN CHEMICAL SOCIETY - Vol.134 No.37
<P>The O<SUB>2</SUB> and NO reactivity of a Cr(II) complex bearing a 12-membered tetraazamacrocyclic <I>N</I>-tetramethylated cyclam (TMC) ligand, [Cr<SUP>II</SUP>(12-TMC)(Cl)]<SUP>+</SUP> (<B>1</B>), and the NO reactivity of its peroxo derivative, [Cr<SUP>IV</SUP>(12-TMC)(O<SUB>2</SUB>)(Cl)]<SUP>+</SUP> (<B>2</B>), are described. By contrast to the previously reported Cr(III)–superoxo complex, [Cr<SUP>III</SUP>(14-TMC)(O<SUB>2</SUB>)(Cl)]<SUP>+</SUP>, the Cr(IV)–peroxo complex <B>2</B> is formed in the reaction of <B>1</B> and O<SUB>2</SUB>. Full spectroscopic and X-ray analysis revealed that <B>2</B> possesses side-on η<SUP>2</SUP>-peroxo ligation. The quantitative reaction of <B>2</B> with NO affords a reduction in Cr oxidation state, producing a Cr(III)–nitrato complex, [Cr<SUP>III</SUP>(12-TMC)(NO<SUB>3</SUB>)(Cl)]<SUP>+</SUP> (<B>3</B>). The latter is suggested to form via a Cr(III)–peroxynitrite intermediate. [Cr<SUP>II</SUP>(12-TMC)(NO)(Cl)]<SUP>+</SUP> (<B>4</B>), a Cr(II)–nitrosyl complex derived from <B>1</B> and NO, could also be synthesized; however, it does not react with O<SUB>2</SUB>.</P><P><B>Graphic Abstract</B> <IMG SRC='http://pubs.acs.org/appl/literatum/publisher/achs/journals/content/jacsat/2012/jacsat.2012.134.issue-37/ja307384e/production/images/medium/ja-2012-07384e_0007.gif'></P><P><A href='http://pubs.acs.org/doi/suppl/10.1021/ja307384e'>ACS Electronic Supporting Info</A></P>
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Yokoyama, Atsutoshi,Han, Jung Eun,Karlin, Kenneth D.,Nam, Wonwoo The Royal Society of Chemistry 2014 Chemical communications Vol.50 No.14
<P>Reaction of a nonheme iron(<SMALL>III</SMALL>)-peroxo complex, [Fe<SUP>III</SUP>(14-TMC)(O<SUB>2</SUB>)]<SUP>+</SUP>, with NO<SUP>+</SUP>, a transformation which is essentially isoelectronic with that for nitric oxide dioxygenases [Fe(<SMALL>III</SMALL>)(O<SUB>2</SUB>&z.rad;<SUP>−</SUP>) + NO], affords an iron(<SMALL>IV</SMALL>)-oxo complex, [Fe<SUP>IV</SUP>(14-TMC)(O)]<SUP>2+</SUP>, and nitrogen dioxide (NO<SUB>2</SUB>), followed by conversion to an iron(<SMALL>III</SMALL>)-nitrato complex, [Fe<SUP>III</SUP>(14-TMC)(NO<SUB>3</SUB>)(F)]<SUP>+</SUP>.</P> <P>Graphic Abstract</P><P>Reaction of a nonheme iron(<SMALL>III</SMALL>)-peroxo complex, [Fe<SUP>III</SUP>(14-TMC)(O<SUB>2</SUB>)]<SUP>+</SUP>, with NO<SUP>+</SUP> affords an iron(<SMALL>IV</SMALL>)-oxo complex, [Fe<SUP>IV</SUP>(14-TMC)(O)]<SUP>2+</SUP>, and nitrogen dioxide (NO<SUB>2</SUB>), followed by conversion to the nitrato complex, [Fe<SUP>III</SUP>(14-TMC)(NO<SUB>3</SUB>)(F)]<SUP>+</SUP>. <IMG SRC='http://pubs.rsc.org/services/images/RSCpubs.ePlatform.Service.FreeContent.ImageService.svc/ImageService/image/GA?id=c3cc48782b'> </P>
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