CO Oxidation by N2O Homogeneously Catalyzed by Ruthenium Hydride Pincer Complexes Indicating a New Mechanism

被引:61
作者
Zeng, Rong [1 ]
Feller, Moran [1 ]
Diskin-Posner, Yael [2 ]
Shimon, Linda J. W. [2 ]
Ben-David, Yehoshoa [1 ]
Milstein, David [1 ]
机构
[1] Weizmann Inst Sci, Dept Organ Chem, IL-7610001 Rehovot, Israel
[2] Weizmann Inst Sci, Dept Chem Res Support, IL-7610001 Rehovot, Israel
基金
欧洲研究理事会;
关键词
METAL-LIGAND COOPERATION; OXYGEN-ATOM TRANSFER; NITROUS-OXIDE N2O; N BOND-CLEAVAGE; CARBON-MONOXIDE; HYDROGENATION; CHEMISTRY; ALCOHOLS; ACTIVATION; REDUCTION;
D O I
10.1021/jacs.8b03927
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Both CO and N2O are important, environmentally harmful industrial gases. The reaction of CO and N2O to produce CO2 and N-2 has stimulated much research interest aimed at degradation of these two gases in a single step. Herein, we report an efficient CO oxidation by N2O catalyzed by a (PNN)Ru-H pincer complex under mild conditions, even with no added base. The reaction is proposed to proceed through a sequence of O-atom transfer (OAT) from N2O to the Ru-H bond to form a Ru-OH intermediate, followed by intramolecular OH attack on an adjacent CO ligand, forming CO2 and N-2. Thus, the Ru-H bond of the catalyst plays a central role in facilitating the OAT from N2O to CO, providing an efficient and novel protocol for CO oxidation.
引用
收藏
页码:7061 / 7064
页数:4
相关论文
共 56 条
  • [1] Direct Hydrogenation of Amides to Alcohols and Amines under Mild Conditions
    Balaraman, Ekambaram
    Gnanaprakasam, Boopathy
    Shimon, Linda J. W.
    Milstein, David
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2010, 132 (47) : 16756 - 16758
  • [2] PNN Ruthenium Pincer Complexes Based on Phosphinated 2,2′-Dipyridinemethane and 2,2′-Oxobispyridine. Metal-Ligand Cooperation in Cyclometalation and Catalysis
    Barrios-Francisco, Rigoberto
    Balaraman, Ekambaram
    Diskin-Posner, Yael
    Leitus, Gregory
    Shimon, Linda J. W.
    Milstein, David
    [J]. ORGANOMETALLICS, 2013, 32 (10) : 2973 - 2982
  • [3] KINETICS OF CO OXIDATION BY N2O OVER RH(111)
    BELTON, DN
    SCHMIEG, SJ
    [J]. JOURNAL OF CATALYSIS, 1992, 138 (01) : 70 - 78
  • [4] REACTIONS OF DINITROGEN OXIDE (NITROUS-OXIDE) WITH DICYCLOPENTADIENYLTITANIUM COMPLEXES INCLUDING A REACTION IN WHICH CARBON-MONOXIDE IS OXIDIZED
    BOTTOMLEY, F
    LIN, IJB
    MUKAIDA, M
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1980, 102 (16) : 5238 - 5242
  • [5] Depletion of the Ozone Layer in the 21st Century
    Dameris, Martin
    [J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2010, 49 (03) : 489 - 491
  • [6] Ligand Cooperation in the Formal Hydrogenation of N2O Using a PCsp2P Iridium Pincer Complex
    Doyle, Lauren E.
    Piers, Warren E.
    Borau-Garcia, Javier
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2015, 137 (06) : 2187 - 2190
  • [7] HOMOGENEOUS CATALYTIC REDUCTION OF NITROUS AND NITRIC OXIDES TO DINITROGEN BY CARBON-MONOXIDE
    FANG, WP
    CHENG, CH
    [J]. JOURNAL OF THE CHEMICAL SOCIETY-CHEMICAL COMMUNICATIONS, 1986, (07) : 503 - 504
  • [8] Fogg P.G. T., 1992, Solubility Data Series - Carbon Dioxide in Non-aqueous Solvents at Pressures Less Than 200 kP, V50
  • [9] System with Potential Dual Modes of Metal-Ligand Cooperation: Highly Catalytically Active Pyridine-Based PNNH-Ru Pincer Complexes
    Fogler, Eran
    Garg, Jai Anand
    Hu, Peng
    Leitus, Gregory
    Shimon, Linda J. W.
    Milstein, David
    [J]. CHEMISTRY-A EUROPEAN JOURNAL, 2014, 20 (48) : 15727 - 15731
  • [10] Zero-Valent Amino-Olefin Cobalt Complexes as Catalysts for Oxygen Atom Transfer Reactions from Nitrous Oxide
    Gianetti, Thomas L.
    Rodriguez-Lugo, Rafael E.
    Harmer, Jeffrey R.
    Trincado, Monica
    Vogt, Matthias
    Santiso-Quinones, Gustavo
    Grutzmacher, Hansjoerg
    [J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2016, 55 (49) : 15323 - 15328