Ruthenium nanoparticles supported on magnesium oxide: A versatile and recyclable dual-site catalyst for hydrogenation of mono- and poly-cyclic arenes, N-heteroaromatics, and S-heteroaromatics

被引:101
作者
Fang, Minfeng
Sanchez-Delgado, Roberto A. [1 ]
机构
[1] CUNY Brooklyn Coll, Dept Chem, Brooklyn, NY 11210 USA
关键词
Hydrogenation; Ru nanoparticles; Magnesium oxide; Aromatics; N-heteroaromatics; S-heteroaromatics; Heterolytic hydrogen splitting; Ionic hydrogenation mechanism; Dual-site; IMIDAZOLIUM IONIC LIQUIDS; METAL NANOPARTICLES; AMMONIA-SYNTHESIS; STABILIZED RUTHENIUM; MILD CONDITIONS; METHYLATED CYCLODEXTRINS; AROMATIC HYDROGENATION; RU/AL2O3; CATALYSTS; RU/MGO CATALYSTS; SUPERB CATALYST;
D O I
10.1016/j.jcat.2013.12.017
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 development of catalysts capable of promoting hydrogenation of aromatics while being resistant to poisoning by nitrogen- and sulfur-containing species is of much interest in connection with hydrotreating of fossil fuels. We report a catalyst composed of ruthenium nanoparticles supported on magnesia, designed to promote heterolytic hydrogen splitting and surface ionic hydrogenation pathways. The catalyst, prepared through a one-pot procedure, promotes the hydrogenation of mono- and poly-cyclic arenes, as well as N- and S-heteroaromatics representative of fossil fuels components. Of particular significance are the superior activity and wider substrate scope of the catalyst, in relation to other known supported noble metals, and the excellent recyclability and long catalyst lifetime. Based on our experimental data, a dual-site catalyst structure and an associated dual-pathway mechanism are proposed, which may have interesting implications for the development of new poison-tolerant noble metal catalytic systems. (C) 2014 Elsevier Inc. All rights reserved.
引用
收藏
页码:357 / 368
页数:12
相关论文
共 91 条
  • [1] Organometallic approach for the synthesis of nanostructures
    Amiens, Catherine
    Chaudret, Bruno
    Ciuculescu-Pradines, Diana
    Colliere, Vincent
    Fajerwerg, Katia
    Fau, Pierre
    Kahn, Myrtil
    Maisonnat, Andre
    Soulantica, Katerina
    Philippot, Karine
    [J]. NEW JOURNAL OF CHEMISTRY, 2013, 37 (11) : 3374 - 3401
  • [2] [Anonymous], 2010, WORLD ENERGY OUTLOOK
  • [3] [Anonymous], 2011, TRENDS REN EN CONS E
  • [4] [Anonymous], 2004, POWD DIFFR FIL CARD
  • [5] [Anonymous], ANN EN OUTL 2010 PRO
  • [6] [Anonymous], 1995, Handbook of X-ray Photoelectron Spectroscopy. A Reference Book of Standard Spectra for Identification and Interpretation of XPS Data
  • [7] MgO powders: interplay between adsorbed species and localisation of basic sites
    Ardizzone, S
    Bianchi, CL
    Vercelli, B
    [J]. APPLIED SURFACE SCIENCE, 1998, 126 (1-2) : 169 - 175
  • [8] Acid/base and surface features of pure phase magnesia powders
    Ardizzone, S
    Bianchi, CL
    Vercelli, B
    [J]. COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS, 1998, 144 (1-3) : 9 - 17
  • [9] Nanoparticles as recyclable catalysts: The frontier between homogeneous and heterogeneous catalysis
    Astruc, D
    Lu, F
    Aranzaes, JR
    [J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2005, 44 (48) : 7852 - 7872
  • [10] Astruc D., 2008, NANOPARTICLES CATALY