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Fukuzumi, Shunichi,Kobayashi, Takeshi,Suenobu, Tomoyoshi American Chemical Society 2010 JOURNAL OF THE AMERICAN CHEMICAL SOCIETY - Vol.132 No.5
<P><B>Graphic Abstract</B> <IMG SRC='http://pubs.acs.org/appl/literatum/publisher/achs/journals/content/jacsat/2010/jacsat.2010.132.issue-5/ja910349w/production/images/medium/ja-2009-10349w_0005.gif'> <P>A heterodinuclear iridium−ruthenium complex [Ir<SUP>III</SUP>(Cp*)(H<SUB>2</SUB>O)(bpm)Ru<SUP>II</SUP>(bpy)<SUB>2</SUB>](SO<SUB>4</SUB>)<SUB>2</SUB> {<B>1</B>(SO<SUB>4</SUB>)<SUB>2</SUB>, Cp* = η<SUP>5</SUP>-pentamethylcyclopentadienyl, bpm = 2,2′-bipyrimidine, bpy = 2,2′-bipyridine} acts as the most effective catalyst for selective production of hydrogen from formic acid in an aqueous solution at ambient temperature among catalysts reported so far. An unusually large tunneling effect was observed for the first time for the catalytic hydrogen production in H<SUB>2</SUB>O vs D<SUB>2</SUB>O.</P></P><P><A href='http://pubs.acs.org/doi/suppl/10.1021/ja910349w'>ACS Electronic Supporting Info</A></P>
Fukuzumi, Shunichi,Mase, Kentaro,Ohkubo, Kei,Fu, Zhen,Karnas, Elizabeth,Sessler, Jonathan L.,Kadish, Karl M. American Chemical Society 2011 JOURNAL OF THE AMERICAN CHEMICAL SOCIETY - Vol.133 No.19
<P>Disproportionation of dipyrrolylquinoxaline radical anions occurs via hydrogen atom transfer from the pyrrole moiety to the quinoxaline moiety to produce monodeprotonated dipyrrolylquinoxaline anions and monohydrodipyrrolylquinoxaline anions. In contrast, simple quinoxaline radical anions without pyrrole moieties are stable, and disproportionation occurs only in the presence of external protons.</P><P><B>Graphic Abstract</B> <IMG SRC='http://pubs.acs.org/appl/literatum/publisher/achs/journals/content/jacsat/2011/jacsat.2011.133.issue-19/ja200925e/production/images/medium/ja-2011-00925e_0002.gif'></P><P><A href='http://pubs.acs.org/doi/suppl/10.1021/ja200925e'>ACS Electronic Supporting Info</A></P>
Mononuclear Copper Complex-Catalyzed Four-Electron Reduction of Oxygen
Fukuzumi, Shunichi,Kotani, Hiroaki,Lucas, Heather R.,Doi, Kaoru,Suenobu, Tomoyoshi,Peterson, Ryan L.,Karlin, Kenneth D. American Chemical Society 2010 JOURNAL OF THE AMERICAN CHEMICAL SOCIETY - Vol.132 No.20
<P><B>Graphic Abstract</B> <IMG SRC='http://pubs.acs.org/appl/literatum/publisher/achs/journals/content/jacsat/2010/jacsat.2010.132.issue-20/ja100538x/production/images/medium/ja-2010-00538x_0002.gif'> <P>A mononuclear Cu<SUP>II</SUP> complex acts as an efficient catalyst for four-electron reduction of O<SUB>2</SUB> to H<SUB>2</SUB>O. Its reduction by a ferrocene derivative (Fc*) and reaction with O<SUB>2</SUB> leads to the formation of a peroxodicopper(II) complex; this is subsequently reduced by Fc* in the presence of protons to regenerate the Cu<SUP>II</SUP> complex.</P></P><P><A href='http://pubs.acs.org/doi/suppl/10.1021/ja100538x'>ACS Electronic Supporting Info</A></P>
Formation of Ground State Triplet Diradicals from Annulated Rosarin Derivatives by Triprotonation
Fukuzumi, Shunichi,Ohkubo, Kei,Ishida, Masatoshi,Preihs, Christian,Chen, Bo,Borden, Weston Thatcher,Kim, Dongho,Sessler, Jonathan L. American Chemical Society 2015 JOURNAL OF THE AMERICAN CHEMICAL SOCIETY - Vol.137 No.31
<P>Annulated rosarins, β,β′-bridged hexaphyrin(1.0.1.0.1.0) derivatives <B>1</B>–<B>3</B>, are formally 24 π-electron antiaromatic species. At low temperature, rosarins <B>2</B> and <B>3</B> are readily triprotonated in the presence of trifluoroacetic acid in dichloromethane to produce ground state triplet diradicals, as inferred from electron paramagnetic resonance (EPR) spectral studies. From an analysis of the fine structure in the EPR spectrum of triprotonated rosarin <B>H</B><SUB><B>3</B></SUB><B>3</B><SUP><B>3+</B></SUP>, a distance of 3.6 Å between the two unpaired electrons was estimated. The temperature dependence of the singlet–triplet equilibrium was determined by means of an EPR titration. Support for these experimental findings came from calculations carried out at the (U)B3LYP/6-31G* level, which served to predict a very low-lying triplet state for the triprotonated form of a simplified model system <B>1</B>.</P><P><B>Graphic Abstract</B> <IMG SRC='http://pubs.acs.org/appl/literatum/publisher/achs/journals/content/jacsat/2015/jacsat.2015.137.issue-31/jacs.5b05309/production/images/medium/ja-2015-05309k_0008.gif'></P><P><A href='http://pubs.acs.org/doi/suppl/10.1021/ja5b05309'>ACS Electronic Supporting Info</A></P>
Fukuzumi, Shunichi,Morimoto, Yuma,Kotani, Hiroaki,Naumov, Pan?e,Lee, Yong-Min,Nam, Wonwoo Nature Publishing Group, a division of Macmillan P 2010 Nature chemistry Vol.2 No.9
Critical biological electron-transfer processes involving high-valent oxometal chemistry occur widely, for example in haem proteins [oxoiron(IV); Fe<SUP>IV</SUP>(O)] and in photosystem II. Photosystem II involves Ca<SUP>2+</SUP> as well as high-valent oxomanganese cluster species. However, there is no example of an interaction between metal ions and oxoiron(IV) complexes. Here, we report new findings concerning the binding of the redox-inactive metal ions Ca<SUP>2+</SUP> and Sc<SUP>3+</SUP> to a non-haem oxoiron(IV) complex, [(TMC)Fe<SUP>IV</SUP>(O)]<SUP>2+</SUP> (TMC?=?1,4,8,11-tetramethyl-1,4,8,11-tetraazacyclotetradecane). As determined by X-ray diffraction analysis, an oxo-Sc<SUP>3+</SUP> interaction leads to a structural distortion of the oxoiron(IV) moiety. More importantly, this interaction facilitates a two-electron reduction by ferrocene, whereas only a one-electron reduction process occurs without the metal ions. This control of redox behaviour provides valuable mechanistic insights into oxometal redox chemistry, and suggests a possible key role that an auxiliary Lewis acid metal ion could play in nature, as in photosystem II.
Fukuzumi, Shunichi,Kobayashi, Takeshi,Suenobu, Tomoyoshi WILEY‐VCH Verlag 2011 Angewandte Chemie Vol.123 No.3
<P><B>3 Metalle, 2 Elektronen, 1 H</B><SUB><B>2</B></SUB><B>:</B> Ein Aquarhodiumkomplex und ein Iridium‐Ruthenium‐Komplex (siehe Bild) wirken als effektive Katalysatoren für die photokatalytische Zwei‐Elektronen‐Reduktion von Protonen. Wasserstoff wird mithilfe eines Photosensibilisators und eines Elektronendonors erzeugt, indem die um ein Elektron reduzierten Metallkomplexe disproportionieren.</P>
Fukuzumi, Shunichi,Kobayashi, Takeshi,Suenobu, Tomoyoshi American Chemical Society 2010 JOURNAL OF THE AMERICAN CHEMICAL SOCIETY - Vol.132 No.34
<P>A heterodinuclear iridium−ruthenium complex [Ir<SUP>III</SUP>(Cp*)(H<SUB>2</SUB>O)(bpm)Ru<SUP>II</SUP>(bpy)<SUB>2</SUB>](SO<SUB>4</SUB>)<SUB>2</SUB> (Cp* = η<SUP>5</SUP>-pentamethyl-cyclopentadienyl, bpm = 2,2′-bipyrimidine, bpy = 2,2′-bipyridine) acts as an effective catalyst for removal of dissolved O<SUB>2</SUB> by the four-electron reduction of O<SUB>2</SUB> with formic acid in water at an ambient temperature.</P><P><B>Graphic Abstract</B> <IMG SRC='http://pubs.acs.org/appl/literatum/publisher/achs/journals/content/jacsat/2010/jacsat.2010.132.issue-34/ja104486h/production/images/medium/ja-2010-04486h_0007.gif'></P><P><A href='http://pubs.acs.org/doi/suppl/10.1021/ja104486h'>ACS Electronic Supporting Info</A></P>
Fukuzumi, S.,Karlin, K.D. Elsevier Publishing Company 2013 Coordination chemistry reviews Vol.257 No.1
The kinetics and thermodynamics of formation of Cu(II)-superoxo (Cu-O<SUB>2</SUB>) complexes by the reaction of Cu(I) complexes with dioxygen (O<SUB>2</SUB>) and the reduction of Cu(II)-superoxo complexes to dinuclear Cu-peroxo complexes are discussed. In the former case, electron transfer from a Cu(I) complex to O<SUB>2</SUB> occurs concomitantly with binding of O<SUB>2</SUB><SUP>?-</SUP>to the corresponding Cu(II) species. This is defined as an inner-sphere Cu(II) ion-coupled electron transfer process. Electron transfer from another Cu(I) complex to preformed Cu(II)-superoxo complexes also occurs concomitantly with binding of the Cu(II)-peroxo species with the Cu(II) species to produce the dinuclear Cu-peroxo (Cu<SUB>2</SUB>-O<SUB>2</SUB>) complexes. The kinetics and thermodynamics of outer-sphere electron-transfer reduction of Cu<SUB>2</SUB>-O<SUB>2</SUB> complexes are also been discussed in light of the Marcus theory of outer-sphere electron transfer.