Binding and Activation of N2O at Transition-Metal Centers: Recent Mechanistic Insights

被引：216
作者：
Tolman, William B. [1 ,2 ]
机构：
[1] Univ Minnesota, Dept Chem, Ctr Met Biocatalysis, Minneapolis, MN 55410 USA
[2] Univ Minnesota, Ctr Sustainable Polymers, Minneapolis, MN 55410 USA
来源：
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2010年 / 49卷 / 06期
关键词：
catalysis; N2O activation; nitrogen oxides; reaction mechanisms; transition metals; NITROUS-OXIDE REDUCTASE; CU-Z CLUSTER; SPIN-FORBIDDEN REACTION; BRIDGED IRON SITES; GAS-PHASE; ELECTRONIC-STRUCTURE; ACHROMOBACTER-CYCLOCLASTES; ORGANOMETALLIC CHEMISTRY; COMPREHENSIVE DFT; DINITROGEN OXIDE;
D O I：
10.1002/anie.200905364
中图分类号：
O6 [化学];
学科分类号：
0703 ;
摘要：
No laughing matter, nitrous oxide's role in stratospheric ozone depletion and as a greenhouse gas has stimulated great interest in developing and understanding its decomposition, particularly through the use of transition-metal promoters. Recent advances in our understanding of the reaction pathways for N2O reduction by metal ions in the gas phase and in heterogeneous, homogeneous, and biological catalytic systems have provided provocative ideas about the structure and properties of metal N2O adducts and derived intermediates. These ideas are likely to inform efforts to design more effective catalysts for N2O remediation. © 2010 Wiley-VCH Verlag GmbH & Co. KGaA,.
引用
收藏
页码：1018 / 1024
页数：7
相关论文
共 100 条
[11]   O-atom transport catalysis by atomic cations in the gas phase:: Reduction of N2O by CO [J].
Blagojevic, V ;
Orlova, G ;
Bohme, DK .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2005, 127 (10) :3545-3555
[12]   Gas-phase catalysis by atomic and cluster metal ions:: The ultimate single-site catalysts [J].
Böhme, DK ;
Schwarz, H .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2005, 44 (16) :2336-2354
[13]   MODE OF BONDING OF DINITROGEN OXIDE (NITROUS-OXIDE) IN (DINITROGEN OXIDE)PENTAAMMINERUTHENIUM [J].
BOTTOMLEY, F ;
BROOKS, WVF .
INORGANIC CHEMISTRY, 1977, 16 (02) :501-502
[14]  
Brown K, 2000, NAT STRUCT BIOL, V7, P191
[15]   Revisiting the catalytic CuZ cluster of nitrous oxide (N2O) reductase -: Evidence of a bridging inorganic sulfur [J].
Brown, K ;
Djinovic-Carugo, K ;
Haltia, T ;
Cabrito, I ;
Saraste, M ;
Moura, JJG ;
Moura, I ;
Tegoni, M ;
Cambillau, C .
JOURNAL OF BIOLOGICAL CHEMISTRY, 2000, 275 (52) :41133-41136
[16]   Kinetic study of the reactions of gas phase Pd(a1S0), Ag(5s 2S1/2), Au(6s 2S1/2), Cd(5s2 1S0), and Hg(6s2 1S0) atoms with nitrous oxide [J].
Campbell, ML .
JOURNAL OF PHYSICAL CHEMISTRY A, 2003, 107 (17) :3048-3053
[17]   X-X Through-Cage Bonding in Cu, Ni, and Cr Complexes with M3X2 Cores (X = S, As) [J].
Carrasco, Rosa ;
Aullon, Gabriel ;
Alvarez, Santiago .
CHEMISTRY-A EUROPEAN JOURNAL, 2009, 15 (02) :536-546
[18]   N2O reduction by the μ4-sulfide-bridged tetranuclear CuZ cluster active site [J].
Chen, P ;
Gorelsky, SI ;
Ghosh, S ;
Solomon, EI .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2004, 43 (32) :4132-4140
[19]   Spectroscopic and electronic structure studies of the μ4-sulfide bridged tetranuclear Cuz cluster in N2O reductase:: Molecular insight into the catalytic mechanism [J].
Chen, P ;
Cabrito, I ;
Moura, JJG ;
Moura, I ;
Solomon, EI .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2002, 124 (35) :10497-10507
[20]   Electronic structure description of the μ4-sulfide bridged tetranuclear Cuz center in N2O reductase [J].
Chen, P ;
George, SD ;
Cabrito, I ;
Antholine, WE ;
Moura, JJG ;
Moura, I ;
Hedman, B ;
Hodgson, KO ;
Solomon, EI .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2002, 124 (05) :744-745
12345678910