Catalytic routes to transportation fuels utilizing natural gas hydrates

被引:12
作者
Wegrzyn, JE
Mahajan, D [1 ]
Gurevich, M
机构
[1] Brookhaven Natl Lab, Dept Appl Sci, Upton, NY 11973 USA
[2] US DOE, Off Heavy Vehicles Technol, Washington, DC 20585 USA
关键词
partial oxidation; Fischer-Tropsch diesel; dimethylether; MeOH;
D O I
10.1016/S0920-5861(98)00466-0
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
Gas hydrates hold >50% of earth's total combustible carbon. To make this vast but dilute (CH(4)similar to 3.9 wt%) energy source available, an economical three-step route is outlined. A major technological challenge is environmentally-benign mining of gas hydrates that releases "Aqueous CH4" and makes it available at the surface (Step 1). Step 2 involves a cost-effective partial oxidation (POX) with air route that eliminates the O-2-separation plant (conventional POX with O-2) to produce synthesis gas. In Step 3, technologies that affect catalytic conversion of synthesis gas to Fischer-Tropsch (F-T) diesel, MeOH, and dimethylether (DME) transportation fuels are considered. The selection of MeOH and DME energy liquids is justified based on seven criteria: (1) low temperature; (2) low pressure; (3) high gas conversion per pass to eliminate recycle; (4) high spacetime-yield; (5) high product selectivity; (6) robust catalyst; (7) overall high process efficiency. A Ni/Base catalyst system, presently undergoing pilot testing at Brookhaven National Laboratory (BNL), is described that by virtue of its homogeneous liquid phase operation selectively (>95%) produces methanol with unprecedented single pass conversion (>95%) at T<150 degrees C and P=2-5 MPa essentially satisfies these set-forth process requirements. A preliminary kinetic study on the original BNL catalyst system is presented and a limited kinetic rate expression is deduced. Several areas for further research are identified that will allow economical production of MeOH or DR IE in the skid-mounted unit/flexible product option concept applicable to both on-land and off-short: gas hydrates. (C) 1999 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:97 / 108
页数:12
相关论文
共 17 条
[1]   Direct measurement of in situ methane quantities in a large gas-hydrate reservoir [J].
Dickens, GR ;
Paull, CK ;
Wallace, P .
NATURE, 1997, 385 (6615) :426-428
[2]   CLATHRATE HYDRATES [J].
ENGLEZOS, P .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 1993, 32 (07) :1251-1274
[3]  
FLEISCH TH, 1995, DIESEL PROG ENGINE D, P43
[4]   PRODUCTION OF SYNGAS BY DIRECT CATALYTIC-OXIDATION OF METHANE [J].
HICKMAN, DA ;
SCHMIDT, LD .
SCIENCE, 1993, 259 (5093) :343-346
[5]   MECHANISTIC ASPECTS OF THE FORMATION OF HYDROCARBONS AND ALCOHOLS FROM CO HYDROGENATION [J].
HINDERMANN, JP ;
HUTCHINGS, GJ ;
KIENNEMANN, A .
CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 1993, 35 (01) :1-127
[6]   MASS-TRANSFER CHARACTERISTICS OF GASES IN METHANOL AND ETHANOL UNDER ELEVATED PRESSURES AND TEMPERATURES [J].
KONERIPALLI, N ;
TEKIE, Z ;
MORSI, BI ;
CHANG, MY .
CHEMICAL ENGINEERING JOURNAL AND THE BIOCHEMICAL ENGINEERING JOURNAL, 1994, 54 (02) :63-77
[7]  
Lee S., 1990, METHANOL SYNTHESIS T
[8]   DIRECT CATALYTIC CONVERSION OF METHANE TO ACETIC-ACID IN AN AQUEOUS-MEDIUM [J].
LIN, M ;
SEN, A .
NATURE, 1994, 368 (6472) :613-615
[9]  
Mahajan D, 1990, U. S. Patent, Patent No. [4,935,395, 4935395]
[10]  
MAHAJAN D, UNPUB