Catalytic alkane metathesis by tandem alkane dehydrogenation olefin metathesis

被引:500
作者
Goldman, AS [1 ]
Roy, AH
Huang, Z
Ahuja, R
Schinski, W
Brookhart, M
机构
[1] Rutgers State Univ, Dept Chem & Biol Chem, Piscataway, NJ 08854 USA
[2] Univ N Carolina, Dept Chem, Chapel Hill, NC 27599 USA
[3] Chevron Res & Technol Co, Richmond, CA 94802 USA
关键词
D O I
10.1126/science.1123787
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
With petroleum supplies dwindling, there is increasing interest in selective methods for transforming other carbon feedstocks into hydrocarbons suitable for transportation fuel. We report the development of highly productive, well-defined, tandem catalytic systems for the metathesis of n-alkanes. Each system comprises one molecular catalyst ( a "pincer''-ligated iridium complex) that effects alkane dehydrogenation and olefin hydrogenation, plus a second catalyst ( molecular or solid-phase) for olefin metathesis. The systems all show complete selectivity for linear (n-alkane) product. We report one example that achieves selectivity with respect to the distribution of product molecular weights, in which n-decane is the predominant high-molecular-weight product of the metathesis of two moles of n-hexane.
引用
收藏
页码:257 / 261
页数:5
相关论文
共 23 条
[1]   The metathesis reactions: from a historical perspective to recent developments [J].
Astruc, D .
NEW JOURNAL OF CHEMISTRY, 2005, 29 (01) :42-56
[2]   Primary products and mechanistic considerations in alkane metathesis [J].
Basset, JM ;
Copéret, C ;
Lefort, L ;
Maunders, BM ;
Maury, O ;
Le Roux, E ;
Saggio, G ;
Soignier, S ;
Soulivong, D ;
Sunley, GJ ;
Taoufik, M ;
Thivolle-Cazat, J .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2005, 127 (24) :8604-8605
[3]   MECHANISM AND POISONING OF MOLECULAR REDISTRIBUTION REACTION OF ALKANES WITH A DUAL-FUNCTIONAL CATALYST SYSTEM [J].
BURNETT, RL ;
HUGHES, TR .
JOURNAL OF CATALYSIS, 1973, 31 (01) :55-64
[4]   High quality diesel via the Fischer-Tropsch process - a review [J].
Dry, ME .
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY, 2002, 77 (01) :43-50
[5]   Mechanistic studies of the transfer dehydrogenation of cyclooctane catalyzed by iridium bis(phosphinite) p-XPCP pincer complexes [J].
Göttker-Schnetmann, I ;
Brookhart, M .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2004, 126 (30) :9330-9338
[6]   Iridium bis(phosphinite) p-XPCP pincer complexes:: Highly active catalysts for the transfer dehydrogenation of alkanes [J].
Göttker-Schnetmann, I ;
White, P ;
Brookhart, M .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2004, 126 (06) :1804-1811
[7]   Olefin metathesis [J].
Grubbs, RH .
TETRAHEDRON, 2004, 60 (34) :7117-7140
[8]   Catalytic dehydrogenation of cycloalkanes to arenes by a dihydrido iridium P-C-P pincer complex [J].
Gupta, M ;
Hagen, C ;
Kaska, WC ;
Cramer, RE ;
Jensen, CM .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1997, 119 (04) :840-841
[9]   A highly active alkane dehydrogenation catalyst: Stabilization of dihydrido rhodium and iridium complexes by a P-C-P pincer-ligand [J].
Gupta, M ;
Hagen, C ;
Flesher, RJ ;
Kaska, WC ;
Jensen, CM .
CHEMICAL COMMUNICATIONS, 1996, (17) :2083-2084
[10]   What will come after petroleum? [J].
Levenspiel, O .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2005, 44 (14) :5073-5078