Itoh Group Literature Review

Linus Chiang   † ,  Khrystyna Herasymchuk   † ,  Fabrice Thomas   § , and  Tim Storr   * † †  Department of Chemistry,  Simon Fraser University , Burnaby, British Columbia V5A 1S6,  Canada §  Département de Chimie Moléculaire, Chimie Inorganique Redox (CIRE), UMR-5250,  Université Grenoble Alpes , BP 53, 38041 Grenoble Cedex 9,  France Inorg. Chem. , Article ASAP DOI:  10.1021/acs.inorgchem.5b00783 Publication Date (Web): May 27, 2015 Copyright © 2015 American Chemical Society *E-mail:  tim_storr@sfu.ca . Synopsis Nickel ( Ni(Sal CF3 ) ) and copper ( Cu(Sal CF3 ) ) complexes of an electron-deficient salen ligand were prepared, and their one-electron oxidized counterparts were studied using an array of experimental and theoretical methods.  Ni(Sal CF3 )  undergoes ligand oxidation to afford a delocalized ligand radical, while  Cu(Sal CF3 ) exhibits metal-based oxidation to afford a Cu III  species. 電子求引基をサレンにつけることで、配位子が電子不足になり酸化されにくくなる。これにより、錯体の一電子過程において配位子ではな

Brenda Nataly Sanchez-Eguia ,     Marcos Flores-Álamo ,   Maylis Orio  and     Ivan Castillo    Chem. Commun. , 2015, Accepted Manuscript DOI:  10.1039/C5CC02332G Received 19 Mar 2015, Accepted 28 May 2015 First published online 28 May 2015 http://pubs.rsc.org/en/content/articlelanding/2015/cc/c5cc02332g#!divAbstract Abstract   Copper complexes with N 3 S donors inspired on the Cu M  site of copper monooxygenases react with O 2  affording side-on cupric-superoxo complexes capable of H-abstraction from dihydroanthracene and THF. Spectroscopic and DFT data of the Cu-superoxos support a spin triplet ground state for the side-on complexes, as well as a hemilabile thioether.                                        

Scott D. McCann   and  Shannon S. Stahl   * Department of Chemistry,  University of Wisconsin-Madison , 1101 University Avenue, Madison, Wisconsin 53706,  United States Acc. Chem. Res. , Article ASAP DOI:  10.1021/acs.accounts.5b00060 Publication Date (Web): May 28, 2015 Copyright © 2015 American Chemical Society http://pubs.acs.org/doi/ abs/10.1021/acs.accounts.5b00060 Abstract Conspectus Selective oxidation reactions have extraordinary value in organic chemistry, ranging from the conversion of petrochemical feedstocks into industrial chemicals and polymer precursors to the introduction of heteroatom functional groups into pharmaceutical and agrochemical intermediates. Molecular oxygen (O 2 ) would be the ideal oxidant for these transformations. Whereas many commodity-scale oxidations of simple hydrocarbon feedstocks employ O 2  as an oxidant, methods for selective oxidation of more complex molecules bearing diverse functional groups are often incompatib

Kosuke Ono   † § ,  Kohei Johmoto   ‡ § ,  Nobuhiro Yasuda   ∥ ,  Hidehiro Uekusa   ‡ § ,  Shintaro Fujii   † ,  Manabu Kiguchi   † , and  Nobuharu Iwasawa   * † § † Department of Chemistry,  ‡ Department of Chemistry and Materials Science,  Tokyo Institute of Technology and  § JST-CREST, O-okayama, Meguro-ku, Tokyo 152-8551,  Japan ∥   Japan Synchrotron Radiation Research Institute/SPring-8 , 1-1-1 Kouto, Sayo-cho, Sayo-gun, Hyogo 679-5198,  Japan J. Am. Chem. Soc. , Article ASAP DOI:  10.1021/jacs.5b02716 Publication Date (Web): May 18, 2015 Copyright © 2015 American Chemical Society http://pubs.acs.org/doi/abs/10.1021/jacs.5b02716 * niwasawa@chem.titech.ac.jp Abstract By use of the reversible trimerization of boronic acids, the series of boroxine cages  3-mer ,  6-mer , and  12-mer  were constructed from rationally designed diboronic acids whose bond angles between two C–B bonds are 60°, 84°, and 117°, respectively. Boroxine cages  6-mer  and  12-mer  have 1

Cooper Citek   † ,  J. Brannon Gary   † ,  Erik C. Wasinger   ‡ , and  T. Daniel P. Stack   * † †  Department of Chemistry,  Stanford University , Stanford, California 94305,  United States ‡  Department of Chemistry and Biochemistry,  California State University , Chico, California 95929,  United States J. Am. Chem. Soc. , Article ASAP DOI:  10.1021/jacs.5b02157 Publication Date (Web): May 28, 2015 Copyright © 2015 American Chemical Society http://pubs.acs.org/doi/abs/10.1021/jacs.5b02157 * stack@stanford.edu Abstract The mechanisms of dioxygen activation and methane C−H oxidation in particulate methane monooxygenase (pMMO) are currently unknown. Recent studies support a binuclear copper site as the catalytic center. We report the low-temperature assembly of a high-valent dicopper(III) bis(μ-oxide) complex bearing marked structural fidelity to the proposed active site of pMMO. This unprecedented dioxygen-bonded Cu(III) species with exclusive biological ligat

Edge Article  Significant improvement of oxidase activity through the genetic incorporation of a redox-active unnatural amino acid Yang Yu , c      Qing Zhou , b      Li Wang , a b      Xiaohong Liu , b      Wei Zhang , b    Meirong Hu , b      Jianshu Dong , b      Jiasong Li , a b      Xiaoxuan Lv , b    Hanlin Ouyang , c      Han Li , b      Feng Gao , b      Weimin Gong , b    Yi Lu * c  and     Jiangyun Wang * b    Show Affiliations Chem. Sci. , 2015, Advance Article DOI:  10.1039/C5SC01126D Received 29 Mar 2015, Accepted 13 Apr 2015 First published online 13 Apr 2015 While nature employs various covalent and non-covalent strategies to modulate tyrosine (Y) redox potential and p K a  in order to optimize enzyme activities, such approaches have not been systematically applied for the design of functional metalloproteins. Through the genetic incorporation of 3-methoxytyrosine (OMeY) into myoglobin, we replicated important features of cytochrome c oxidase (CcO)

Chemistry - A European Journal  by Li Ji, Abayomi S. Faponle, Matthew G. Quesne, Mala A. Sainna, Jing Zhang, Alicja Franke, Devesh Kumar, Rudi van Eldik, Weiping Liu, Sam P. de Visser  /   25d   //   keep unread  //   hide   //   preview Abstract Cytochrome P450 enzymes are highly versatile biological catalysts in our body that react with a broad range of substrates. Key functions in the liver include the metabolism of drugs and xenobiotics. One particular metabolic pathway that is poorly understood relates to the P450 activation of aliphatic groups leading to either hydroxylation or desaturation pathways. A DFT and QM/MM study has been carried out on the factors that determine the regioselectivity of aliphatic hydroxylation over desaturation of compounds by P450 isozymes. The calculations establish multistate reactivity patterns, whereby the product distributions differ on each of the spin-state surfaces; hence spin-selective product formation was found. The electronic and

Pablo Garrido-Barros † , Ignacio Funes-Ardoiz † , Samuel Drouet † , Jordi Benet-Buchholz † , Feliu Maseras * † ‡ , and Antoni Llobet * † ‡ † Institute of Chemical Research of Catalonia (ICIQ) , Avgda. Països Catalans, 16, 43007 Tarragona, Spain ‡ Departament de Química, Universitat Autònoma de Barcelona , 08193 Bellaterra, Spain J. Am. Chem. Soc. , Article ASAP DOI: 10.1021/jacs.5b03977 Publication Date (Web): May 18, 2015 Copyright © 2015 American Chemical Society Abstract A new family of tetra-anionic tetradentate amidate ligands, N 1 , N 1 ′-(1,2-phenylene)bis( N 2 -methyloxalamide) (H 4 L1), and its derivatives containing electron-donating groups at the aromatic ring have been prepared and characterized, together with their corresponding anionic Cu(II) complexes, [(L Y )Cu] 2– . At pH 11.5, the latter undergoes a reversible metal-based III/II oxidation process at 0.56 V and a ligand-based pH-dependent electron-transfer process at 1.25 V, a