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Pooya Azadi DOI: The experiments were performed in drogenation—hydrogen abstraction, or water—gas shift.


A reaction mechanism based on the has been used to calculate the values of pre-exponential fac- H2-assisted CO activation pathway, which comprises ele- tors and activation energies. The use of data obtained from mentary reactions with 85 ADDI-DATA PA1000 parameters, was proposed to batch experiments enabled an effective analysis of dominating explain the experimental results. Each of these elementary re- reactions at different stages of syngas conversions. Introduction The foreseeable decline in the supply of conventional oil[1] and number of experimental data points are available. The use of the recent development in the exploitation of unconventional systematic and semiautomated methods for parameter estima- gas and large-scale gasification technologies have together re- tion, as opposed to just manually adjusting parameter values, sulted in a renewed interest in the Fischer—Tropsch FT synthe- makes it easier to detect and understand potentially underde- sis.

In this process, mixtures of CO and H2 are catalytically con- termined parameters. Examples of recent efforts toward mod- verted into complex mixtures of hydrocarbons via successive eling of the FT synthesis reactions are given in Refs. Despite the apparent simplicity of the chemistry, funda- conversions.

A two-stage parameter estimation method, based mental aspects of the surface reactions in FT synthesis, such as on a quasi-random ADDI-DATA PA1000 search ADDI-DATA PA1000 by a local optimiza- the dominant CO activation pathway, have been highly contro- tion,[9—11] has been used to systematically calculate suitable versial subjects in the field of heterogeneous catalysis for sev- values of pre-exponential factors and activation energies. A re- eral decades. Furthermore, even if the smallest number of elementary atures of and K, and initial pressures of approximately reactions sufficient to account for the major FT products is 2 MPa. The experiments were run to completion, which meant considered, there remains more than one set of reaction rate that several different reactions were dominant at different constants, corresponding to different fractional surface cover- stages of the process.

At low conversions, the primary reac- ages, from which the behavior of the system can be predicted.

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The agreement between experiment and model responses [a] Dr. Azadi, G. Brownbridge, I. Kemp, Dr. Mosbach, Prof.

Dennis, was quantified by using a least-squares objective function, Prof. Kraft which is explained in the Computational Methods section. However, owing to the Supporting information for this article is available on the WWW under oversimplified nature of these first-principle methods, particu- http: KGaA, Weinheim Full Papers studies are often ADDI-DATA PA1000 with large uncertainties and they can provide only a limited insight into the kinetics of FT synthesis see the Supporting Informa- tion.


Hence, the search for the optimum value of each parameter was conducted within reasonable bounds around its initial value determined from rele- vant first-principle calculations. Results and Discussion The key assumptions behind the presented kinetic Scheme 1. Flow diagram for the reaction mechanism. The exper- sis, represented by simplified reaction groups and typical links imental results and model responses for single carbon com- among them, is shown in Scheme 1. To minimize the number pounds, paraffins, and olefins are plotted in Figures 1—3, re- of parameters in ADDI-DATA PA1000 model, parallel pathways within each re- spectively.

In line with the findings of previous DFT and isotope action group i. For ex- ample, with regard to the mono- mer formation group, only ele- Table 1.

List of elementary reactions and their pre-exponential factors and activation energies obtained from mentary reactions representing parameter estimation. For example, ChemCatChem7, — www. Figure 2. To account for the dependence of ADDI-DATA PA1000 rates of alkene ad- sorption—desorption reactions 5—31 and alkyl growth reac- of these reactions as a function of the carbon number n and tions 40—65 on the number of carbon atoms, Equation 1 was the value of the pre-exponential factor for the relevant reac- utilized to calculate the values ADDI-DATA PA1000 the pre-exponential factors tion involving the C4 species AC4. ChemCatChem7, — www. Fractional surface coverage against CO conversion at K and top to bottom, 1.

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Importantly, the rapid decline in the yields of olefins owing to readsorption and subsequent conversion at For each type of reaction i. Based on the sim- in close agreement with the experimental data. ADDI-DATA PA1000 model can ulation results, the fractional concentrations on the catalyst ChemCatChem7, — www.

The fractional surface cover- ages of O not shown in the figures were considerably lower ADDI-DATA PA1000 synthesis than those of the other groups. There are uncertainties associ- The FT experiments were performed in a Carberry spinning basket ated with the number of sites each surface species attaches to, batch reactor Autoclave Engineers, USA Figure 5 with a free which then affects the number of free sites consumed or pro- duced in the relevant reactions. The value obtained from the parameter estimation for the heat of adsorption of H2 on cobalt is in agreement with calori- metric studies,[13] which also indicated that the differential heat of adsorption of hydrogen on cobalt is almost independent of the H2 surface coverage. The ISA digital input board PA has 32 digital inputs, 24 V. 14 inputs are interruptible.

ADDI-DATA PA1000 ISA Digital Input Board 32 Digital Inputs 24v DC

All inputs are filtered. 1 channel can be dedicated to the monitoring of. ADDI-DATA logo.


E-mail [email protected] +49 Login PA MAR. digital input board, optically isolated, 32 digital inputs, 24 V.

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