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2月, 2017の投稿を表示しています

Alkane Oxidation: Methane Monooxygenases, Related Enzymes, and Their Biomimetics

Vincent C.-C. Wang † ‡ ,  Suman Maji ‡ § ,  Peter P.-Y. Chen ∥ ,  Hung Kay Lee ⊥ ,  Steve S.-F. Yu † , and  Sunney I. Chan * † # ○     †  Institute of Chemistry,  Academia Sinica , 128, Section 2, Academia Road, Nankang, Taipei 11529,  Taiwan §  School of Chemical Engineering and Physical Sciences,  Lovely Professional University , Jalandhar-Delhi G. T. Road (NH-1), Phagwara, Punjab  India  144411 ∥  Department of Chemistry,  National Chung Hsing University , 250 Kuo Kuang Road, Taichung 402,  Taiwan ⊥  Department of Chemistry,  The Chinese University of Hong Kong , Shatin, New Territories,  Hong Kong #  Department of Chemistry,  National Taiwan University , No. 1, Section 4, Roosevelt Road, Taipei 10617,  Taiwan ○  Noyes Laboratory, 127-72,  California Institute of Technology , 1200 East California Boulevard, Pasadena, California 91125,  United States Chem. Rev. , Article ASAP DOI:  10.1021/acs.chemrev.6b00624 Publication Date (Web): February 16, 2017 Copyright

Mechanistic insights into intramolecular ortho-amination/hydroxylation by nonheme FeIV[double bond, length as m-dash]NTs/FeIV[double bond, length as m-dash]O species: the σ vs. the π channels

Bhawana Pandey , a      Madhavan Jaccob a b  and   Gopalan Rajaraman * a    Show Affiliations Chem. Commun. , 2017, Advance Article DOI:  10.1039/C6CC08761B Received 01 Nov 2016, Accepted 11 Feb 2017 First published online 13 Feb 2017 Comparative oxidative abilities of nonheme Fe IV NTs and Fe IV O species using DFT has been explored. Our calculations reveal that the Fe IV NTs is found to be a stronger oxidant in two electron transfer reactions and react exclusively  via  π channels while the Fe IV O species is found to be a stronger oxidant when the σ-pathway is activated such as in HAT reactions. http://pubs.rsc.org/en/content/articlelanding/2017/cc/c6cc08761b#!divAbstract

Substrate and Lewis Acid Coordination Promote O–O Bond Cleavage of an Unreactive L2CuII2(O22–) Species to Form L2CuIII2(O)2 Cores with Enhanced Oxidative Reactivity

Isaac Garcia-Bosch * † ,  Ryan E. Cowley ‡ ,  Daniel E. Díaz § ,  Ryan L. Peterson § ,  Edward I. Solomon * ‡ , and  Kenneth D. Karlin * §   †  Department of Chemistry,  Southern Methodist University , Dallas, Texas 75275,  United States ‡  Department of Chemistry,  Stanford University , Stanford, California 94305,  United States §   Johns Hopkins University , Baltimore, Maryland 21218,  United States J. Am. Chem. Soc. , Article ASAP DOI:  10.1021/jacs.6b12990 Publication Date (Web): February 14, 2017 Copyright © 2017 American Chemical Society * igarciabosch@smu.edu , * edward.solomon@stanford.edu , * karlin@jhu.edu Copper-dependent metalloenzymes are widespread throughout metabolic pathways, coupling the reduction of O 2  with the oxidation of organic substrates. Small-molecule synthetic analogs are useful platforms to generate L/Cu/O 2  species that reproduce the structural, spectroscopic, and reactive properties of some copper-/O 2 -dependent enzymes. La

Second sphere ligand modifications enable a recyclable catalyst for oxidant-free alcohol oxidation to carboxylates

Eric W. Dahl , a      Thomas Louis-Goff a  and   Nathaniel K. Szymczak * a    Show Affiliations Chem. Commun. , 2017, Advance Article DOI:  10.1039/C6CC10206A Received 23 Dec 2016, Accepted 25 Jan 2017 First published online 03 Feb 2017 Modification of the classic terpyridine pincer ligand with pendent NHR (R = mesityl) groups provides enhanced activity and stability in Ru-catalyzed dehydrogenation catalysis. These second sphere modifications furnish highly active catalysts for the oxidant-free dehydrogenative oxidation of primary alcohols to carboxylates and facilitate catalyst recycling. http://pubs.rsc.org/en/content/articlepdf/2017/cc/c6cc10206a