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the coking properties of coal at elevated pressures. - Argonne ...

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Effect <strong>of</strong> Char Loading on Nitric Oxide Reduction<br />

The effect <strong>of</strong> char loading in <strong>the</strong> fluidized bed on NO reduction by char is<br />

illustr<strong>at</strong>ed in Figure 9. As can be seen, <strong>the</strong> reduction <strong>of</strong> NO increases with increase<br />

in char loading. A t bed temper<strong>at</strong>ure <strong>of</strong> 75OoC, <strong>the</strong> effect <strong>of</strong> char loading is most<br />

important around 1 percent where it results in a NO reduction <strong>of</strong> 87 percent. A t<br />

higher char loading, <strong>the</strong> reduction <strong>of</strong> NO is generally higher; however, <strong>the</strong> effect <strong>of</strong> ,<br />

<strong>the</strong> char loading becomes less significant. The same trend can also be observed <strong>at</strong><br />

<strong>the</strong> temper<strong>at</strong>ore range below 75OoC, even though <strong>the</strong> reduction <strong>of</strong> NO falls below<br />

60 percent due to <strong>the</strong> strong temper<strong>at</strong>ure dependence <strong>of</strong> <strong>the</strong> reduction reaction.<br />

Higher char loading in <strong>the</strong> bed may increase <strong>the</strong> chances <strong>of</strong> clinker form<strong>at</strong>ion which<br />

is caused by local temper<strong>at</strong>ure excursion as a consequence <strong>of</strong> <strong>the</strong> poor solid mixing<br />

and <strong>the</strong> inability to dissip<strong>at</strong>e <strong>the</strong> he<strong>at</strong> <strong>of</strong> combustion. In addition, <strong>the</strong> loss <strong>of</strong><br />

unburnt carbon in <strong>the</strong> drained spent-bed m<strong>at</strong>erial may become unacceptable if <strong>the</strong> char<br />

loading in <strong>the</strong> bed becomes too high. However, recent developments in fluidized-bed<br />

combustion technology have indic<strong>at</strong>ed th<strong>at</strong> two-stage combustion systems with <strong>the</strong><br />

increased char loading in <strong>the</strong> first stage enhances <strong>the</strong> overall reduction <strong>of</strong> nitric<br />

oxide emission significantly5.<br />

Prediction <strong>of</strong> NO Reduction by Char 1<br />

Recent experimental studies6 on <strong>the</strong> reduction reaction <strong>of</strong> nitric oxide with char<br />

have concluded th<strong>at</strong> <strong>the</strong> reaction is f irst order with respect to <strong>the</strong> NO concentr<strong>at</strong>ion.<br />

This practice is, hence, adopted in <strong>the</strong> present study. The reaction r<strong>at</strong>e constants<br />

<strong>of</strong> <strong>the</strong> reaction <strong>of</strong> NO with Char 1 <strong>at</strong> <strong>the</strong> corresponding temper<strong>at</strong>ures and char load-<br />

ings were calcul<strong>at</strong>ed based on <strong>the</strong> experimental d<strong>at</strong>a presented <strong>at</strong> Table 3. The<br />

activ<strong>at</strong>ion energy and <strong>the</strong> frequency factor within <strong>the</strong> range <strong>of</strong> oper<strong>at</strong>ing conditions<br />

are 31.7 kcal/mol and 9.66 x 10' sec-' respectively. The r<strong>at</strong>e constants <strong>of</strong> NO-char<br />

plotted as a function <strong>of</strong> inverse temper<strong>at</strong>ures for several experimental studies' are<br />

compared with <strong>the</strong> present results in Figure 10. As can be seen, <strong>the</strong> reaction r<strong>at</strong>e<br />

constants obtained from <strong>the</strong> present experiment show good agreement with previous<br />

investig<strong>at</strong>ions. The NO-char reaction kinetics can be represented by <strong>the</strong> following<br />

correl<strong>at</strong>ion and this was employed in <strong>the</strong> NO emission modeling. In view <strong>of</strong> <strong>the</strong> low<br />

k = 9.66 x loa exp (-<br />

31,700) sec-l ,<br />

RT<br />

superficial velocity, <strong>the</strong> shallow bed, and rel<strong>at</strong>ively small bed diameter, a two-<br />

phase bubble model' with both <strong>the</strong> bubble and emulsion phases tre<strong>at</strong>ed as plug flow<br />

was employed for <strong>the</strong> prediction <strong>of</strong> NO conversion. The NO reduction by Char 1 was<br />

calcul<strong>at</strong>ed using this approach over <strong>the</strong> range <strong>of</strong> experimental conditions. The com-<br />

parison <strong>of</strong> calcul<strong>at</strong>ed versus test d<strong>at</strong>a values may be observed in Table 3, as well<br />

as Figure 7. As can be seen in Figure 7, <strong>the</strong> calcul<strong>at</strong>ed values for NO reduction show<br />

excellent agreement with experimental d<strong>at</strong>a.<br />

Conclusions<br />

Tests to determine <strong>the</strong> NO reduction capability <strong>of</strong> two different chars and a<br />

metallurgic coke were conducted in an electrically he<strong>at</strong>ed, b<strong>at</strong>ch, fluidized-bed<br />

reactor in <strong>the</strong> absence <strong>of</strong> oxygen. Based on <strong>the</strong> experimental results, <strong>the</strong> following<br />

conclusions can be drawn.<br />

o Reduction <strong>of</strong> nitric oxide depends strongly on <strong>the</strong> physical <strong>properties</strong> <strong>of</strong> <strong>the</strong><br />

carbonaceous solids such as specific surface area and pore size distribution;<br />

and, to a lesser extent, on <strong>the</strong> carbon content.<br />

0 Reduction reaction between NO and carbonaceous solids was found to be strongly<br />

influenced by bed temper<strong>at</strong>ure. Within <strong>the</strong> range <strong>of</strong> oper<strong>at</strong>ing conditions, <strong>the</strong><br />

degree <strong>of</strong> NO reduction increases with bed temper<strong>at</strong>ure. However, <strong>the</strong> form<strong>at</strong>ion<br />

<strong>of</strong> <strong>the</strong>rmal NO and <strong>the</strong> unfavorable sulf<strong>at</strong>ion reaction for n<strong>at</strong>ural sorbents in an<br />

278<br />

I<br />

I<br />

r

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