Chars from 20 lignite
samples were prepared from two types of original
lignites by multistage removal of inherent metallic species and subsequent
pyrolysis and then were gasified with CO2. A kinetic model,
which assumed the progress of noncatalytic and catalytic gasification
in parallel, quantitatively described the time-dependent changes in
char conversion up to 0.999 for all the chars by employing multicatalytic
species having different initial activities and deactivation kinetics.
A single piecewise linear function, which followed a nucleation–growth
mechanism of the catalysts, showed the relationship between the total
concentration of Na, K, Ca, and Fe and the initial total catalytic
activity (ICA-2) for the chars. The overall rate of catalyst deactivation
(ICD-2) was given by a single linear function of ICA-2 and a factor
for the composition of metallic species. This function was also applicable
to previously reported ICA-2/ICD-2 relationships for chars from lignite
and biomass, showing fast deactivation of Fe catalyst and an important
role of Mg in the promotion of catalyst deactivation.
Potassium (K)-catalyzed CO 2 gasification of lignite char was studied with a particular focus on the change in catalyst activity with the char conversion (X) at 800−900 °C. Char samples were prepared from an Indonesian lignite by a sequence of complete removal of inherent metallic species and mineral matter, K-loading by ion-exchange, and pyrolysis. The catalytic activity of K (k cat ′ ) was defined as the rate of catalytic gasification (after elimination of the rate of non-catalytic gasification and that of K volatilization from total mass release rate from char) per amount of K retained by the gasifying char. k cat ′ increased by a factor of 5− 20 with X over its range up to 0.98−0.99, depending on the initial K concentration in the char (m cat,0 ), ranging 0.16−1.4 wt %-daf. Such significant increase in k cat ′ was due to the change in not the intrinsic reactivity of char but its porous nature, that is, the size and volume of pores that retained the K catalyst. At X < 0.4, the entire portion of the K catalyst was confined in micropores (width <2.0 nm) having relatively small k cat ′ , although it increased gradually. At X > 0.4, the gasification created greater mesopores (width >2.0 nm), providing spaces for growth in the size of the K catalyst and allowing promotion of its activity. However, for low m cat,0 , its major portion continued to stay in micropores with a limited increase in k cat ′ .
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