Iridium catalyzed hydrogenation of CO2 under basic conditions-Mechanistic insight from theory

被引：94
|
作者：
Ahlquist, Marten S. G. [1 ]
机构：
[1] Royal Inst Technol, Sch Biotechnol, Dept Theoret Chem, SE-10691 Stockholm, Sweden
来源：
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL | 2010年 / 324卷 / 1-2期
关键词：
DFT; Carbon dioxide; Iridium; Catalysis; Hydrogenation; Reduction; Formate; Base; Transition metal; Homogeneous; CONTINUUM DIELECTRIC THEORY; SOLVATION FREE-ENERGIES; CARBON-DIOXIDE; THERMOCHEMISTRY; DENSITY; MODEL; WATER;
D O I：
10.1016/j.molcata.2010.02.018
中图分类号：
O64 [物理化学（理论化学）、化学物理学];
学科分类号：
070304 ; 081704 ;
摘要：
The iridium(III) catalyzed hydrogenation of carbon dioxide under basic conditions was studied with density functional theory. It was found that the insertion of CO2 into an Ir-H bond proceeds via a two-step mechanism. The rate-limiting step was calculated to be the regeneration of the iridium(III) trihydride intermediate, and the overall barrier for the reaction was calculated to 26.1 kcal mol(-1). The formation of the iridium trihydride proceeds via formation of a cationic Ir(H)(2)(H-2) complex at which the base abstracts a proton from the dihydrogen ligand. (C) 2010 Elsevier B.V. All rights reserved.
引用
收藏
页码：3 / 8
页数：6
相关论文
共 50 条
  • [31] Insight into the electronic effect of phosphine ligand on Rh catalyzed CO2 hydrogenation by investigating the reaction mechanism
    Ni, Shao-Fei
    Dang, Li
    PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2016, 18 (06) : 4860 - 4870
  • [32] Heterogeneously Catalyzed Hydrogenation of Supercritical CO2 to Methanol
    Kommoss, Bjoern
    Klemenz, Sebastian
    Schmitt, Fabian
    Hocke, Elisabeth
    Vogel, Kevin
    Drochner, Alfons
    Albert, Barbara
    Etzold, Bastian
    Vogel, Herbert G.
    CHEMICAL ENGINEERING & TECHNOLOGY, 2017, 40 (10) : 1907 - 1915
  • [33] Iron catalyzed CO2 hydrogenation to liquid hydrocarbons
    Fiato, RA
    Iglesia, E
    Rice, GW
    Soled, SL
    ADVANCES IN CHEMICAL CONVERSIONS FOR MITIGATING CARBON DIOXIDE, 1998, 114 : 339 - 344
  • [34] CO and CO2 hydrogenation under mechanochemical treatment
    Morozova, OS
    Streletskii, AN
    Berestetskaya, IV
    Borunova, AB
    CATALYSIS TODAY, 1997, 38 (01) : 107 - 113
  • [35] Shape and Surface Morphology of Copper Nanoparticles under CO2 Hydrogenation Conditions from First Principles
    Muller, Andreas
    Comas-Vives, Aleix
    Coperet, Christophe
    JOURNAL OF PHYSICAL CHEMISTRY C, 2021, 125 (01): : 396 - 409
  • [36] Effective Fixation of CO2 by Iridium-Catalyzed Hydrosilylation
    Lalrempuia, Ralte
    Iglesias, Manuel
    Polo, Victor
    Sanz Miguel, Pablo J.
    Fernandez-Alvarez, Francisco J.
    Perez-Torrente, Jesus J.
    Oro, Luis A.
    ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2012, 51 (51) : 12824 - 12827
  • [37] Asymmetric transfer hydrogenation of aromatic ketones catalyzed by the iridium hydride complex under ambient conditions
    Chen, JS
    Li, YY
    Dong, ZR
    Li, BZ
    Gao, JX
    TETRAHEDRON LETTERS, 2004, 45 (45) : 8415 - 8418
  • [38] Mechanistic insights into PtN/MoS2 catalyzed CO2 hydrogenation to methanol: A first-principles study
    Yuan, Yongning
    Gao, Zhuxian
    Guo, Tuo
    Li, Caihu
    Yang, Panpan
    Zhang, Jianli
    Zhu, Yun
    He, Yurong
    Hu, Xiude
    Guo, Qingjie
    INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 2025, 98 : 139 - 147
  • [39] Iridium-Catalyzed Hydrogenation and Dehydrogenation of N-Heterocycles in Water under Mild Conditions
    Wang, Shengdong
    Huang, Haiyun
    Bruneau, Christian
    Fischmeister, Cedric
    CHEMSUSCHEM, 2019, 12 (11) : 2350 - 2354
  • [40] The mechanism for production of abiogenic formate from CO2 and lactate from glycerine: uncatalyzed transfer hydrogenation of CO2 with glycerine under alkaline hydrothermal conditions
    Shen, Zheng
    Gu, Minyan
    Zhang, Min
    Sang, Wenjing
    Zhou, Xuefei
    Zhang, Yalei
    Jin, Fangmin
    RSC ADVANCES, 2014, 4 (29) : 15256 - 15263
12345