D. Taulbee, D.P. Patil, B.K. Parekh and R. Honaker University of Kentucky Center for Applied Energy Research Lexington, KY 40514
ABSTRACT
The coal industry usually discards fine-size (-150 microns) coal because of its high moisture content and handling problems. One avenue is to either pelletize or briquette this material. However, industry has not adopted this route due in part to a significant binder cost that would be involved. In an effort to reduce costs, a study was conducted on combining a coarse, 16 x 100-mesh spiral product, with a fine- coal flotation product, both with and without added saw dust. Maximizing packing-density of the coal and wood waste mixture provides a potential for reducing the binder requirements due to a minimization of the void space. Tests were conducted to evaluate the impact of particle-size distributions for different blends of fine and coarse coal, with and without saw dust and a binder. Modified Proctor densities, porosity, and green, one-day, and seven-day compressive strengths were determined for each of these blends
For the coal-only blends, packing density maximized at a relatively high (70 to 80%) coarse-coal content. However, for these blends, packing densities did not correlate with compressive strengths but instead maximized at 100% fine coal and continuously decreased as higher proportions of coarse coal were added. Similar compaction and compressive-strength results were obtained for briquettes prepared with sawdust and varying proportions of coarse and fine coal. With the addition of a binder, the highest strengths were no longer obtained with 100% fine coal but instead maximized between 20%-50% coarse coal addition for one day and became more defined at a 50% coarse product for seven-day strengths.
In a second set of evaluations, a limited number of combustion tests, simulating a traveling grate, were conducted. Three samples of coal/sawdust briquettes were combusted during these tests, one prepared without a binder and two prepared with different binder formulations. The two briquetted samples prepared with a binder exhibited good integrity and burn-out characteristics with one of the binder formulations showing a significant reduction (~32%) in NO x emissions.
1. INTRODUCTION
Kentucky ranks third in coal production with about 150 million tons annually while also producing the largest amount of timber products east of the Mississippi River. A majority of the timber production occurred within or near the coalfields within Kentucky.
Vast quantities of fine, high quality carbon material currently exist in slurry impoundments in Kentucky due to the lack of effective recovery technologies. The fine coal in the waste represents not only a loss of valuable energy resources but also an environmental hazard. Estimates indicate that over 500 million tons of fine coal refuse are currently stored in refuse ponds in the state of Kentucky. Currently, approximately 3 million tons annually of fine clean coal is being lost to the reject stream.
In 1997, the amount of sawdust generated was 35 million cubic feet or about 12% of the total production. Nearly 47% of the sawdust was used as an industrial fuel while the remaining was disposed in landfills. It is a goal of the Industry to utilize 100% of the sawdust for autonomous energy production. The approach described in this proposal will significantly enhance the possibility of reaching this goal.
The goal of the project was to develop a premium fuel from the waste materials created from the production of coal and lumber. A specific objective is to achieve a fuel having an energy value around 9,000 to 10,000 btu/lb from the processed waste material. The fine coal obtained from the fine coal refuse slurry being discarded using advanced separation technologies and then dewatered to lower moisture levels . The coarser size clean coal was collected from the coal preparation plants spiral circuit. The present study was conducted to evaluate the impact of particle-size distributions for blends of 1) fine and coarse coal, 2) fine and coarse coal with saw dust, and 3) fine and coarse coal with saw dust and binder on briquettes quality. The purpose behind the study was to reduce binder costs by maximizing packing density through blending a portion of the spiral product with the ultrafine clean coal. Preliminary combustion testing was conducted of the briquettes using a simulated traveling grate boiler.
2. EXPERIMENTAL
The fine refuse slurry was processed using the Jamison flotation cell which provided a very low ash ( ~ 6%) clean coal at more than 90% recovery. The median particle size (D 50 ) of the product was 35 microns. From the same preparation plant a 55-gallon drum of clean coal from the Spiral circuit was collected. The size distribution showed that 90% of the particles are coarser than 297 microns (50 mesh). The sample of the spiral concentrate was first mildly dried in room air to facilitate screening/sampling, and then screened to -8 mesh. Blends of the fine and coarser coal fractions were then prepared in a laboratory blender by varying the proportion of spiral concentrate from 0 to 100% in 10% increments. The initial, wet blends, were subjected to modified Proctor-(packing) density tests and briquetting studies. Each of the blends was then moisture-equilibrated (dry blends) in an environmental chamber for seven days at 80% relative humidity and 22 o C and again subjected to a modified Proctor densities and briquetted. Finally, the same blends were used to study the effects of moisture content, as well as the addition of saw dust and binder on packing density and compressive strength. During these tests, the weight of material that was loaded to the pellet dye was adjusted to compensate for the differences in moisture content between the various blends in an effort to maintain a constant weight of dry material in each briquette.
Modified Proctor densities were obtained by compacting each blend into an approximate one-liter volume with an impact hammer and then recording the weight of material compacted into that fixed volume. These modified Proctor densities will be referred to as packing densities in the following sections. For briquette formation the standard conditions of 4,000 lbs briquetting force, 3-s dwell time, and 22.2 o C cure temperature was utilized. The porosity of the briquettes was determined by measuring the briquette height since the sample weight and briquette diameter were fixed. The compressive strength were measured with the
3. RESULTS AND DISCUSSIONS
Figure 1 shows the packing densities of the coal-only blends (no sawdust or binder) as a function of spiral-product content. The packing density was found to maximize at a relatively high 70-80% spiral- product content which is explained to some extent by the high-density, mineral matter content (20%) of the spiral product that was used in this study.
Packi ng wei ght as a functi on of product stream (coal onl y bl ends) 0.70 0.80 0.90 1.00 1.10 1.20 0 20 40 60 80 100 120 % Spi ral product W e i g h t / L i t e r wet blends dry blends
Figure 1. Packing densities for blends of spiral and flotation product.
Figure 2 shows the compressive strength and porosity of briquettes formed from the wet, coal-only blends (no binder). The green-briquette strengths (day 0) were highest for those briquettes prepared with 100% fine coal (~90 lb f ). Green strengths generally declined with increasing spiral content but did exhibit an inflection or increase at ~50% spiral-product, beyond which compressive strengths declined sharply. In contrast, the compressive strength maximized in the 50:50 blend for the cured briquettes (day 7). Interestingly, cured-briquette compressive strengths were generally declined from day 0 to day 7 for the blends containing higher proportions of fine flotation coal but increased over the same period for those blends containing more of the larger particle size spiral product. As there is a significant amount of water loss over this period, these data suggest a more beneficial role for moisture in the initial binding of the smaller particles but a detrimental role for larger ones. This advantage disappeared as the moisture evaporated.
The height of the fixed diameter briquettes coupled with the skeletal densities of the coal fines were used to calculate porosity values for the briquettes that were formed from the spiral-flotation blends. Porosity minimized at approximately 90% spiral product, much higher than the spiral concentrations in which the maximum 7-day compressive strengths (50% spiral blends) were observed. A somewhat puzzling result of this study is the lack of a clear (inverse) correlation between porosity and briquette strength which had been anticipated when the study was initiated. The reason for this low correlation is not clear but may again be related to the high mineral-matter content of the spiral product as well as the nature of the spiral particles which have a lower surface area to weight than do the smaller flotation particles. Both of these factors would be expected to impact porosity and the strength of the inter- particle attractions in the manner observed.
0.00 20.00 40.00 60.00 80.00 100.00 0 20 40 60 80 100 120 Percent Spiral Product in Briquette S h a t t e r
( l b ) 0 0.05 0.1 0.15 0.2 0.25 0.3 0.35 0.4 P o r o s i t y Shatter Day 0 Shatter Day 7 Porosity Day 7
Figure 2. Compressive strengths and porosities of the coal-only briquettes formed with the wet spiral-flotation blends.
Figure 3 shows the compressive strength and porosity of briquettes formed from the dry, coal-only blends following 5% water addition (note, water had to be added in order to form briquettes that would hold together, i.e., >5 lb f strength). As before, porosity minimized in the 70-90% spiral-product range while green strengths were highest in the 100% flotation product and the maximum 7-day cured- briquette strengths were obtained with the 50:50 blend. However, unlike observed with the wet coal sample, the slope of the strength versus per cent spiral curve was both flatter and generally of a lower magnitude than was observed for the wet blends, particularly at the higher flotation-product concentrations.
0.00 20.00 40.00 60.00 80.00 0 20 40 60 80 100 120 Percent Spiral Product in Briquette S h a t t e r
( l b ) 0 0.05 0.1 0.15 0.2 0.25 0.3 0.35 0.4 P o r o s i t y Shatter Day 0 Shatter Day 7 Porosity
Figure 3. Compressive strengths and porosities of the coal-only briquettes formed with the spiral-flotation blends (dry blends with 5% added water).
The compressive strengths of briquettes formed from the coal/sawdust blends following addition of either 5% or 20% water are shown in Figure 4. For all blends, the addition of 10% saw dust resulted in substantial reduction in both green- and cured-briquette strength relative to the corresponding briquettes prepared without sawdust (Figure 3). For the 5% added-water blends, both green and cured strength were highest in the 100% fine coal/sawdust blends. It is notable that briquettes prepared with 20% added water were stronger that their counterparts that contained 5% added water. This suggests that the additional water may serve as a lubricant which aids particle rearrangement, thereby improving packing efficiency. In addition, for the 20% added water blends, both green and cured strengths maximized in the 20% spiral blends range instead of being highest in the 100% flotation blend as observed with 5% water addition. In all cases, briquette strengths generally exhibited a strong inverse relation with spiral content. The compressive-strength values tended to converge in the higher spiral- content blends regardless of the cure time or the level of water addition. 0 5 10 15 20 25 30 35 0 50 100 150 Percent Spi ral Product S h a t t e r
( l b f ) 5% water( day 0) 20% wate (day 0) 5% water (day 7) 20% water (day 7)
Figure 4. The impact of spiral content and water addition on compressive strengths for coal + saw dust (10%) blends.
Finally, the bulk densities for cured briquettes that were prepared from either coal-only or coal/saw dust feeds are shown in Figure 5. There are two interesting features in Figure 5. First, the density of the briquettes formed from blends containing sawdust exhibited a maximum density near 60-70% spiral content, significantly lower than that of the coal-only blends which maximized at approximately 80% spiral product. Also note that the densities of the briquettes formed with 20% added water were higher than the corresponding briquettes formed with 5% added water. This is despite the fact that these briquettes were allowed to equilibrate under identical conditions for seven days. These observations are favorable from a commercial stance as they suggest that it may not be necessary to radically reduce the moisture content prior to briquetting as the presence of excess water appears to improve packing efficiency, thereby potentially lowering shipping cost since a given weight of product may be contained in a lesser volume. 0.8 0.9 1 1.1 1.2 1.3 1.4 0 50 100 150 Percent Spi ral Product i n Bri quette P a c k i n g
D e n s i t y
( g m / c m 3 )Dried +5% Water Dried +10% SD +5% Water Dried +10% SD +20% Water
Figure 5. Density of briquettes prepared from coal and from coal plus saw dust (10%) following a 7-day cure at room temperature
Repeat compaction experiments: The results of the blending of spiral and flotation products indicated that in fact, higher density briquettes (more efficient packing) could be obtained via blending of the spiral and flotation products. However, the higher packing efficiencies did not equate to a higher - briquette strength, at least not in the absence of a binder. It was speculated that a possible reason for the lack of improvement in strength was a result of the high ash content (~20 weight %) of the spiral product used in the initial blending study and an unusually high proportion of coarse particles in this particular spiral sample. To explore this line of reasoning, the blending/compaction experiments were repeated, only this time using a spiral product that contained less ash as well as fewer coarse particles. The ash content of the spiral product was reduced via gravity separation (lithium metatungstate) at a density of 1.50 g/cm 3 . The unusually high coarse particle content was reduced by splitting the spiral product into +16 and -16 mesh fractions and then recombining at a ratio of 1 part of the +16 mesh fraction and 9 parts of the -16 mesh fraction to simulate a more typical spiral material. These sample preparation steps resulted in a reduction in the ash content from ~20 wt% in the unmodified- to ~9.5% in the modified-spiral sample. In the repeat tests, only the wet flotation/spiral blends were tested and these were tested with and without added sawdust and with and without added binder (GG).
For the coal-only blends, packing density maximized at about 60% spiral product (Figure 6) compared to a maximum density at ~70-80% spiral product observed earlier with the higher ash-content spiral product. The packing density for this blend was approximately 15% greater than was achieved with the 100% flotation product. Similarly, the packing density of the coal/sawdust blends maximized around 55% float and 45% spiral product. The inclusion of the spiral product in this mix increased packing density by 7% relative to the equivalent 100% flotation/sawdust blend. The addition of sawdust resulted in a shift in the maximum packing-density to a higher proportion of float product relative to the coal- only blends, indicating that the smaller flotation particles appear to pack more efficiently in the presence of the larger sawdust particles.
0.75 0.79 0.83 0.87 0.91 0.95 0 20 40 60 80 100 % spi ral product d e n s i t y
Figure 6 a. Packing densities for spiral/flotation blends using a reduced ash content spiral product (coal-only blends).
0.76 0.8 0.84 0.88 0.92 0 20 40 60 80 100 120 % Spi ral product d e n s i t y
Figure 6 b. Packing densities for spiral/flotation blends using a reduced ash content spiral product (coal/sawdust blends).
Briquette Strength: Next, briquettes were formed from the coal-only blends for compressive-strengths determinations. In the initial tests, compressive strengths were measured for the coal-only blends without an added binder. As before, the highest compressive strengths were recorded for the briquettes containing 100% flotation product. However, the decline in strength was relatively minor up to the addition of approximately 50% spiral product.
Next, compressive strength measurements were made for coal/sawdust blends that were briquetted both with and without binder (1% GG). Again, when no binder was used, the higher strengths were obtained in the 100% flotation blend with a steady decline in both the initial and 7-day strength observed as a function of spiral content. However, with the addition of a binder, the highest green strengths were no longer clearly obtained with 100% flotation product but were essentially the same for blends containing between 0 and 50% spiral product (Figure 7). A shift in the maximum-strength to higher proportions of spiral became even more pronounced as the briquettes cured. Compressive strengths appeared to maximize at a mix between 20%-50% spiral product on day 1 and became more defined at a 50% spiral product content on day 7. Briquettes formed from blends of flotation and spiral product were also more durable in terms of shatter resistance (drop tests) in which the most durable briquettes were obtained for mixes containing nearly 60% spiral product (Figure 8). Thus, it would appear that when a binder is employed, it may be possible to make stronger briquettes for a given binder addition when the coal fines are blended with a larger particle size spiral products.
0 20 40 60 80 100 120 140 160 180 200 0 20 40 60 80 100 120 % Spiral Product C o m p r e s s i o n
S t r e n g t h Green Strength 1-Day Strength 7-Day Strength
Figure 7. Briquette strengths for coal/sawdust blends as a function of spiral product content when using a binder.
0 2 4 6 8 10 12 14 16 0 20 40 60 80 100 120 % Spiral Product A v e .
#
o f
D r o p s
Figure 8. Shatter resistance for briquettes formed from coal/sawdust/binder blends 3.1 COMBUSTION TESTING OF BRIQUETTES:
A series of combustions tests firing of three different briquettes in a stoker simulator were conducted at the Pennsylvania State Universitys Energy Institute The objectives of the tests were to note combustion stability and emissions when firing the briquettes, which were produced from the feed coal without any binder and two produced by adding additives (labeled LMR and GG). The flue gas from the stoker simulator was sampled and analyzed, per EPA test protocol, for CO 2 , CO, SO 2 , and NO x , emissions. A schematic diagram of the stoker combustor apparatus is shown in Figure 2. Combustion air to the stoker simulator was supplied from the bottom of the chamber through a distributor plate. The air flow rate was varied during a test to simulate the variable air flow rate in an operating stoker boiler. During the 45-minute test, the air flow rate for the first 10 minutes was set at 3.5 standard cubic feet per minute (scfm), then changed to 5 scfm for the next 20 minutes and then lowered to 4 scfm for the last 15 minutes. The bed was purged with nitrogen after the 45-minute test period to ensure that further combustion of the bed does not occur after the test was completed; assist in cooling the bed quickly in order for it to be removed; and mimic the bed dropping into an ash pit where, theoretically, no further combustion occurrs. The variation of air with time is shown in Figure 1. During the peak combustion period at an air flow rate of 5 scfm, the cold air velocity through the grate is approximately 1 ft/s. Although this velocity is lower than the conventional velocity of 1.2 to 1.5 ft/s, it is consistent with the trend of reducing the combustion air flow rate through the grate and increasing the over fire air flow rate to minimize pollutant emissions.
35.25 T T T T T P 3.27" 3.49" 3.19" 4.36" 20 Gage s.s. Grating with 1/16" Holes 1.75" 2.62" 3.49" 7.86" 10.91" 2" 3 Kw Heating Cone Ignition Elements Coal Charge 3.93"
Figure 2. Schematic diagram of the modified stoker simulator.
The fuel analyses are listed in Table 1. The briquettes made with the LMR additive contained a larger concentration of inorganic constituents (i.e., it contained 30% more ash) and also had a very high calorific value. A summary of the combustion tests is provided in Table 2, which contains the average level of O 2 in flue gas during the 20 minute period of maximum air flow, and average emissions normalized to 3% O 2 .
Feed Briquettes
Two tests were performed using the Feed briquettes and are labeled A and B in Table 2. The results from the tests are similar in that the bed burnout was approximately 87% for both tests, although the average level of O 2 in the flue gas was higher for Test B than Test A, i.e., 6.9 as compared to 4.0%, respectively. The CO and CO 2 emissions, normalized to 3% O 2 , were identical for the tests with SO 2 and NO x slightly lower in Test A than Test B. This type of variability is common for batch testing in the stoker simulator. The higher NO x emissions in Test B may be the result of the higher overall O 2
concentration during the test as NO x formation is a function of both O 2 concentration and temperature. The sulfur content in the ash was measured to determine if sulfur capture by the bed could be related to SO 2 emissions. No apparent trend was evident as the sulfur content in the bed ash from Test A was 0.64% while the sulfur content in the bed ash from Test B was 0.75%.
Table 1. Fuel Analyses Fuel Type Feed GG LMR Moisture (%, as received) 1.4 0.7 0.9
Heating Value As-fired 13,468 12,647 12,737 Dry 13,655 13,165 13,289
Table 2. Summary of the Stoker Combustion Tests Average Emissions @ 3% O 2 Test Code Coal Type Bed Burnout (%) Test O 2
Level (%) CO (ppm) CO 2
(%) SO 2
(ppm) NO x
(ppm) A Feed 87.3 4.0 242 15.5 671 168 B Feed 87.3 6.9 241 15.4 739 203
C GG 85.5 4.7 261 16.1 444 145 D GG 83.4 4.6 294 15.8 685 141 E GG 86.5 4.9 254 15.5 632 201
F LMR 98.3 1.2 >6,000 a 15.5 671 168 G LMR 97.6 1.0 N.R. b 15.4 885 75 H LMR 96.0 c 5.4 233 15.6 682 126
a CO emissions were off-scale, which is greater than 6,000 ppm. b Not reported. As can be observed from Figure 10, CO emissions were off-scale (i.e., >6,000 ppm) for a portion of the test period.
GG Briquettes
Three tests were performed using the GG briquettes and are labeled C, D and E in Table 2. The third test (Test E) was performed because of the large discrepancy in SO 2 emissions between Tests C and D, which averaged 444 and 685 ppm (@ 3% O 2 ), respectively.
In Tests C and D, the bed burnouts were similar (86 and 84%, respectively) as were the gaseous emissions other than SO 2 . The sulfur in the bed ash was higher in Test C (0.70%) than in Test D (0.59%), which would indicate increased sulfur capture in the bed and less sulfur in the flue gas.
In Test E, the average SO 2 emissions were 632 ppm (corrected to 3% O 2 ), which are slightly less than the emissions observed in Test D. The sulfur content in the bed ash for Test E was 0.64%. A trend of decreasing SO 2 emissions with increased sulfur retained in the bed ash was observed with this fuel series. The NO x emissions in Test E were slightly higher than those observed in Tests C/D, i.e., 201 ppm as compared to 145/141 ppm, respectively.
LMR Briquettes
The LMR briquettes burned with such intensity that the system was starved of oxygen and CO emissions were excessive. Burnout ranged from 96 to 98% (see Table 2). Increasing air flow was helpful for the first twenty minutes, however, it became too excessive and the bed of coal/ash was blown off of the grate. As a final test, Test H, the coal charge was reduced from 800 g (1.76 lb or a firing density of 26.7 lb/ft 2 ) to 600 g (1.32 lb or a firing density of 20.0 lb/ft 2 ) while maintaining the same air flow/time periods. This test was successfully performed and the emissions results are summarized in Table 2 with the emissions profile shown in Figure 7.
Sulfur contents in the bed ash were also analyzed. They were 0.35, 0.34, and 0.33%, respectively, for Tests F, G, and H,
4. CONCLUSIONS
Blending of spiral and flotation products provided higher density (more efficient packing), however, it did not provided higher briquette strength, at least not in the absence of a binder. Packing densities reached maximum at ~70% spiral product ; with a low ash spiral product the maximum density reached at 60%, this was 15% higher than that achieved with 100% flotation product Packing density of coal/sawdust maximized at about 55% flotation and 45% spiral product. It is possible to make stronger briquettes for a given binder addition when coal fines are blended with larger size spiral product. Highest compressive strength obtained with 100% flotation product, the decline in strength was relatively minor up to addition of approx. 50% spiral product. Briquetts formed from blends of flotation and spiral products (60%) were more durable in terms of shatter resistance (drop tests) For the briquettes made with the feed material the bed burnout was about 87.3%. CO and CO2 emissions were 240 ppm and 15.5%, respectively. Average SO2 and NOx were 705 ppm and 186 ppm, respectively For the GG briquettes the bed burn out was about 85%; the CO and SO2 emissions were 257 ppm and 658 ppm, respectively. The NOx emission averaged 185 ppm. There was no reduction observed in SO2 and NOx emissions. The LMR briquettes burned with high intensity and starved the system of oxygen resulting in high CO emission. The bed burnout was about 97%. There was no significant reduction in CO or SO2 emissions, however, the NOx emission was reduced by about 32%.
ACKNOWLEDGEMENT:
Financial assistance for the project provided by the U.S.Department of Energy through the Kentucky Division of Energy under the State Industries of the Future program. Assistance provided by Dr. V. Oszever and S. Li is acknowledged. Industrial partners were James River Coal, Cook & Sons Coal Company, Pine Mountain Lumber, H & S Lumber, Kentucky Timber Association and Global Energy.