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Title: An Ab Initio Approach Towards Engineering Fischer-Tropsch Surface Chemistry

One of the greatest societal challenges over the next decade is the production of cheap, renewable energy for the 10 billion people that inhabit the earth. This will require the development of various different energy sources potentially including fuels derived from methane, coal, and biomass and alternatives sources such as solar, wind and nuclear energy. One approach will be to synthesize gasoline and other fuels from simpler hydrocarbons such as CO derived from methane or other U.S. based sources such as coal. Syngas (CO and H{sub 2}) can be readily converted into higher molecular weight hydrocarbons through Fischer-Tropsch synthesis. Fischer-Tropsch synthesis involves the initiation or activation of CO and H{sub 2} bonds, the subsequent propagation steps including hydrogenation and carbon-carbon coupling, followed by chain termination reactions. Commercially viable catalysts include supported Co and Co-alloys. Over the first two years of this project we have used ab initio methods to determine the adsorption energies for all reactants, intermediates, and products along with the overall reaction energies and their corresponding activation barriers over the Co(0001) surface. Over the third year of the project we developed and advanced an ab initio-based kinetic Monte Carlo simulation code to simulate Fischer Tropsch synthesis. This reportmore » details our work over the last year which has focused on the derivation of kinetic parameters for the elementary steps involved in FT synthesis from ab initio density functional theoretical calculations and the application of the kinetic Monte Carlo algorithm to simulate the initial rates of reaction for FT over the ideal Co(0001) surface. The results from our simulations over Co(0001) indicate the importance of stepped surfaces for the activation of adsorbed CO. In addition, they demonstrate that the dominant CH{sub x}* surface intermediate under steady state conditions is CH*. This strongly suggests that hydrocarbon coupling occurs through reaction with the adsorbed CH*.« less
Authors:
;
Publication Date:
OSTI Identifier:
882888
DOE Contract Number:
FG26-01NT41275
Resource Type:
Technical Report
Research Org:
University of Virginia
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
01 COAL, LIGNITE, AND PEAT; 02 PETROLEUM; 03 NATURAL GAS; 09 BIOMASS FUELS; 29 ENERGY PLANNING, POLICY AND ECONOMY; ADSORPTION; ALGORITHMS; BIOMASS; CATALYSTS; CHEMISTRY; COAL; ENERGY SOURCES; FISCHER-TROPSCH SYNTHESIS; FUNCTIONALS; GASOLINE; HYDROCARBONS; HYDROGENATION; KINETICS; METHANE; MOLECULAR WEIGHT; NUCLEAR ENERGY; PROGRESS REPORT; STEADY-STATE CONDITIONS; SYNTHESIS