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Reaction kinetics and modelling of the gold catalysed glycerol oxidation

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The kinetics of the glycerol oxidation using a carbon supported gold catalyst was studied experimentally in a batch reactor at oxygen pressures up to 10 bar and at temperatures from 25 to 100 °C. The influence of the mass transfer on the reaction was estimated and confirmed with theoretical calculations. A kinetic model has been proposed on the basis of a Langmuir-Hinshelwood mechanism for the experiments carried out in the kinetic regime and the kinetic parameters (reaction rate and adsorption constants as well as activation energies) were calculated.

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Abbreviations

a p :

external area of particles per unit volume of reactor [m2/m3]

C 1 :

glycerol concentration [mol L−1]

C 2 :

dihydroxyacetone concentration [mol L−1]

C 2al :

glyceraldehyde concentration [mol L−1]

C 3 :

glyceric acid concentration [mol L−1]

C 4 :

tartronic acid concentration [mol L−1]

C 5 :

glycolic acid concentration [mol L−1]

C 6 :

oxalic acid concentration [mol L−1]

d :

impeller diameter [cm]

d p :

average catalyst particle diameter [m]

D :

molecular diffusion coefficient [m2/s]

D eff :

effective diffusion coefficient [m2/s]

e :

rate of flow energy supply per unit mass of liquid [m2/s3]

E A :

activation energy [J/mol]

Fr :

Froude number [−]

H i :

Henrýs coefficient [kPa m3/mol]

k 1 ... k6 :

reaction rate constants \({\hbox{[L}}^{{\rm{(n}}_{\rm{i}} + {\rm{ n}}_{{\rm{bi}}} - {\rm{1)}}} {\hbox{/(mol}}^{{\rm{n}}_{\rm{i}} + {\rm{ n}}_{{\rm{bi}}} - {\rm{1}}} {\hbox{ min g)]}}\)

k 01 ... k 06 :

pre-exponential factors \({\hbox{[L}}^{{\rm{(n}}_{\rm{i}} + {\rm{ n}}_{{\rm{bi}}} - {\rm{1)}}} {\hbox{/(mol}}^{{\rm{n}}_{\rm{i}} + {\rm{ n}}_{{\rm{bi}}} - {\rm{1}}} {\hbox{ min g)]}}\)

K 1 ... K 6 :

adsorption equilibrium constants [l/mol]

k l :

gas–liquid mass transfer coefficient [cm/s]

k l a :

volumetric gas–liquid mass transfer coefficient [s−1]

k s :

liquid-solid mass transfer coefficient [cm/s]

n 1 ... n 6 :

reaction order with respect to the educt of step 1 ... 6 [−]

n b :

reaction order with respect to the base concentration [−]

N :

speed of agitation [Hz]

N P :

power number [−]

P :

oxygen pressure [kPa]

r 1 ... r 6 :

reaction rates of respective steps in figure 1 [mol/L min]

Re :

Reynolds number [−]

Sc :

Schmidt number [−]

V :

reaction volume [m3]

V s :

superficial gas velocity [cm/s]

w :

catalyst amount [g]

αl :

ratio chemical reaction/gas–liquid mass transfer [−]

αs :

ratio chemical reaction/liquid–solid mass transfer [−]

Φexp :

Thiele modulus [−]

ε:

catalyst porosity [−]

μ:

viscosity of the liquid [g/cm s]

ν:

kinematic viscosity [cm2/s]

σ:

surface tension [g/s2]

ρ:

density of the liquid [g/cm3]

ψ:

shape factor [−]

τ:

catalyst tortuosity [−]

ω:

ratio catalyst weight to reactor volume [kg/m3]

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Authors and Affiliations

  1. Department of Chemistry, Ernst-Berl-Institute/Chemical Technology II, Darmstadt University of Technology, Petersenstrasse 20, D-64287, Darmstadt, Germany

    S. Demirel, M. Lucas & P. Claus

  2. Laboratory of Industrial Chemistry, Åbo Akademi University, Biskopsgatan 8, 20500, Åbo/Turku, Finland

    J. Wärnå, T. Salmi & D. Murzin

Authors
  1. S. Demirel
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  2. M. Lucas
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  3. J. Wärnå
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  4. T. Salmi
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  5. D. Murzin
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  6. P. Claus
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Correspondence to P. Claus.

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Demirel, S., Lucas, M., Wärnå, J. et al. Reaction kinetics and modelling of the gold catalysed glycerol oxidation. Top Catal 44, 299–305 (2007). https://doi.org/10.1007/s11244-007-0303-y

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