SUITABILITY OF FEEDSTOCKS FOR THE SASOL-LURGI FIXED BED DRY BOTTOM GASIFICATION PROCESS “Gasification Technologies 2001, San Francisco, California, October 7-10, 2001” JC van Dyk∗, MJ Keyser, JW van Zyl Sasol Technology, R&D Division, Department of Carbon to Syngas Research, P. O. Box 1, Sasolburg, 1947, South Africa Abstract Coal is a crucial feedstock for South Africa’s unique synfuels and petrochemicals industry and it is used by Sasol as a feedstock to produce synthesis gas (CO and H2) via the Sasol-Lurgi fixed bed dry bottom gasification process. A detailed knowledge of coal characteristics is essential to predict gasification behavior when a specific coal source is to be gasified. The principle aim of this paper is to highlight and discuss those specific coal characteristics, which affect gasification behavior and stability. In order to determine the suitability of a coal source for gasification purposes, the coal is characterized and the results compared with historical data. Benchmark data, obtained when the gasifiers are operating without problems and with relatively high stability, is used as a reference. Coal from sources with extreme properties (e.g. ash content <10% to as high as 35% or “brown coal” with moisture content of approximately 30%) can be gasified in a Sasol-Lurgi fixed bed dry bottom gasifier provided that certain operational changes are implemented. Other properties, like high caking propensity for example, require blending to acceptable levels and /or mechanical modifications. The coal characteristics discussed in this paper are not the only properties affecting gasifier stability, but are those properties which are easily measurable on laboratory scale and can be related to gasifier performance. Interpretation of coal characterization data gives an indication of expected gasifier performance, and the suitability of a specific coal source for Sasol/Lurgi Fixed Bed Gasification. Data on a number of coal sources will be discussed. Keywords: Sasol-Lurgi fixed bed dry bottom gasification, coal characteristics, South African coal sources, other feedstocks. 1. INTRODUCTION Coal is used as main feedstock for South Africa’s unique synfuels and petrochemicals industry and it is used by Sasol as a feedstock to produce synthesis gas (CO + H2) via the Sasol-Lurgi fixed bed gasification process. South Africa, as well as many other countries in the world, will for many years to come rely on its abundant coal resources for energy and petrochemical products. The Sasol plants located in Secunda and Sasolburg (South Africa) gasify approximately 30 million tons of bituminous coal to synthesis gas, which is converted to fuels and chemicals via the Fischer-Tropsch process. A total of 97 fixed bed dry bottom gasifiers, 17 at Sasolburg and 80 at Secunda, have a combined production capacity of approximately 5.1 x 106 m3n/h dry crude gas, which is equivalent to approximately 3.6 x 106 m3n/h pure synthesis gas. These production rates are well in excess of the design capacity and were achieved by continuous debottlenecking and optimization. ∗ Corresponding author. Tel.: +27 16 960 4375; fax.: +27 11 522 4806; e-mail: johan.vandyk@sasol.com The coal from the sources used by Sasol vary substantially in terms of chemical and physical properties and this directly relates to gasifier behaviour. The ability of fixed bed gasifiers to handle a variety of different feedstocks is seen as a significant advantage over other gasification technologies. At the Schwarze Pumpe site in the former East Germany, 7 fixed bed dry bottom Lurgi gasifiers are utilized for treatment of solid wastes, such as plastics, sewage sludge, rubber, contaminated wood, paint residues and household wastes [10]. Other distinct characteristics of fixed bed gasifiers are the following: • It uses lump coal and limited grinding is required. Coal used for fixed bed gasification is mined, crushed down to <70mm and screened at a bottom size of 5-8mm. • Coal with a high ash content can be gasified without severe losses in thermal efficiency, since the ash is not extracted in the molten state. • High “cold gas” thermal efficiency is achieved through counter-current operation, which allows the gas and solid product streams to exit at relatively low temperatures. • Low oxidant requirements due to the high thermal efficiency. • Valuable co-products like tars, pitches, oils and chemicals are produced. • A H2/CO ratio of 1.7 to 2.0 is produced directly which is suitable for Fischer-Tropsch synthesis without the need for additional water-gas shift conversion to adjust the H2/CO ratio. The Sasol-Lurgi gasifiers has some limitations, e.g.: • Limited ability to handle excessive fine coal or coal with a high caking propensity. • Broad particle size distributions can lead to excessive coal segregation, which in turn may cause channel burning and unstable gasifier operation. • Pressure drop can limit gas throughput in certain instances. • Relatively high steam consumption. The principle aim of this paper is to highlight and discuss those specific coal or feedstock characteristics, which affect gasification behavior and stability. Due to the large variation in coal properties from various sources, detail coal and feedstock characteristics are essential to predict gasification performance when a specific coal source is to be gasified. 2. COAL MINING AT SASOL The coal used by Sasol for Sasol-Lurgi fixed bed dry bottom gasification in South African has a low rank, is inertinite rich, and has properties which may vary significantly from one mine to the next. Sasol Mining (Pty) Ltd. is responsible for coal mining in the Sasolburg and Secunda regions and supplies coal to Sasol’s synthetic fuels and chemical plants. The division operates regional operations comprising the Sigma Colliery and Wonderwater strip mining operations at Sasolburg and the Secunda Collieries, which consist of six underground operations and a strip mine near Trichardt. The combined run-of-mine output from the Sasolburg and Secunda operations increased from a total production of ±20 million tons in the ten year period 1954 – 1964, to almost 51 million tons 2 per annum in 2000. Supplies to the Sasol Chemical Industries (Sasol 1) plant in Sasolburg are supplemented with external purchases of 0.9 million tons in 2000. During the 2000 financial year, the company supplied 46.7 million tons of saleable coal from the 50.9 million tons of coal extracted to the operations of Sasol Synthetic Fuels (SSF) at Secunda and the Sasol Chemical Industries (SCI) at Sasolburg. The company commenced its coal export operations at Secunda during the 1997 financial year and produced 3.2 million tons of export quality coal, which was exported mainly to Europe, during the 2000 financial year [8]. TABLE 1 SASOL MINING (Pty) Ltd. PRODUCTION HIGHLIGHTS [8] 1999 Production (millions of tons) 2000 50,9 49,0 Total production Sigma Colliery including Wonderwater 5,1 5,5 Secunda Collieries: 6,5 Bosjesspruit Colliery 7,4 Brandspruit Colliery 8,7 8,6 Middelbult Colliery 9,0 8,8 Twistdraai Colliery 5,6 5,9 Twistdraai Export Colliery 6,0 5,1 Syferfontein (underground and strip) 9,1 8,6 Colliery Saleable production from all mines 49,4 47,0 External coal purchases from other mines 0,9 0,7 Total sales excluding exports 49,9 49,0 Sales to SCI (Sasol 1), Sasolburg 6,2 6,5 Sales to SSF, Secunda 40,5 39,4 International sales 3,2 3,1 3. COAL CHARACTERISTICS PERFORMANCE AND THE EFFECT ON GASIFIER New coal sources and areas under exploration for utilization in Sasol-Lurgi fixed bed dry bottom gasification are characterized in detail and the results compared with historical data in order to determine the suitability of a coal source for gasification purposes. Benchmark data, obtained when it was possible to operate the gasifier without problems and with relatively high stability, is used as a reference. The following tests are conducted on coal sources to determine suitability for gasification purposes: • Proximate analysis • Ultimate analysis • CO2 gasification reactivity • Particle size distribution • Ash melting properties and ash composition • Caking properties under 26 bar pressure • Thermal fragmentation (atmospheric pressure) • Mechanical fragmentation • Fischer Assay 3 • • • Total sulphur Heating value Maceral analysis and rank Data obtained on a number of coal will be discussed. 3.1 Proximate analysis Ash content gives an indication of the amount of inorganic material in the coal from a source and includes mineral matter inherent in the coal structure, as well as out-of-seam inorganic contamination. The measurement of ash content is used by Sasol Mining as an operating tool to prepare blends with an ash content within the agreed limits and with a relatively small variation in ash content over time. The budgeted ash content of the coal blend requested by gasification at SSF in Secunda is ±28 % (air dry basis). Gasification at the Sasolburg plant operates on a coal blend with an ash content exceeding 32 % during certain periods. FIGURE 1 VARIATION IN ASH CONTENT (air dried basis) 50 % Ash (average - air dried basis) 45 Secunda Biological sludge 40 35 30 25 20 15 10 5 0 A 3.2 Non SouthAfrican Sasolburg B C D E F I II a b c d e CO2 reactivity CO2 reactivity is determined in order to get an indication of the expected rate of the gasification reactions. Reactivity is expressed as a mass loss per time at 50% burn-off under a CO2 atmosphere. The reactivity of coal from the various sources used by Sasol vary between 2-5 hr-1, although coal sources with lower and higher reactivities have been gasified in the past. Some of the non South-African coal sources tested for gasification purposes have showed reactivities of as low as 0.5 hr-1 and also as high as 9 hr-1. However, it is uncertain what the lower limit for reactivity is below which the gasification reactions will become too slow for complete conversion. 4 3.3 Particle size distribution Particle size distributions of coal blends are determined in order to estimate or predict which size distributions are more likely to cause unstable operation due to pressure drop effects. Pressure drop problems manifest themselves in a variety of ways, and include grate traction loss (due to bed fluidization), channel burning (leading to unacceptable gas outlet temperatures) and solids elutriation (carry-over). Probably the best known estimation method for pressure drop is the Ergun equation, which gives pressure drop as a function of bed voidage ε , viscosity µ, fluid density ρ, superficial velocity Us and particle diameter dp [2]: (1 − ε ) µ U s + 1 . 75 (1 − ε ) pU ∆P = 150 L ε 3 d p2 ε 3d p 2 2 s …(1) When dealing with particle size distributions instead of uniformly sized particles, the particle size dp has to be replaced by φ d p , where φ is the particle sphericity and d p the average particle size reflecting the mean surface area (also referred to as the Sauter mean diameter). The Sauter diameter of a coal sample with a specific particle size distribution is calculated as follows: 1 dp = …(2) xi ∑i d p ,i where i = screen number xi = fraction (mass %) on screen i dp,i = diameter (mm) of screen i Experience has shown that d p is a useful parameter for predicting which PSD’s are more likely to result in gasifier instability. Extensive research on the effect of coal types and PSD on pressure drop and how the data fit the Ergun equation have been conducted, but will not be reported here. The value of d p is extremely sensitive to the smaller particle sizes, or the so-called “tail” of the PSD. As illustrated in Table 2, a 10% change to the coarser side resulted in a change of only 3% in the Sauter diameter, while a 10% change in particle size to the finer fraction resulted in a 7% change. Extensive operating experience has shown that size distributions with a Sauter diameter below a specific value can result in unstable gasifier operation. Inefficient screening due to screen overload causes misplacement of fine coal, which can easily reduce the Sauter diameter to unacceptably low values resulting in highly unstable gasifier operation. 5 TABLE 2 EFFECT OF CHANGE IN PARTICLE SIZE ON SAUTER DIAMETER Fraction (mm) Standard Coarser Finer composition fraction fraction -5.8 42.1 52.1 42.1 -3.7 33.3 23.3 23.3 -2.8 24.6 24.6 34.6 % Change in 3 7 Sauter diameter 3.4 Thermal fragmentation It is known that when lump coal from certain origins (e.g. South-African low rank inertinite rich coals) is exposed to high temperatures (700oC), it will tend to undergo fragmentation (primary and secondary fragmentation)[1]. Primary fragmentation occurs during devolatilization, while secondary fragmentation occurs during combustion of the char by burnout of carbon bridges connecting parts of the particle. In the case of fixed bed gasification, fine material formed in the gasifier may lead to the same kind of hydrodynamic problems as was described previously. Thermal fragmentation of coal is measured by placing a sample with a specific predetermined size distribution into a pre-heated muffle oven at 100oC under atmospheric pressure [9]. The coal is then heated to 700oC (final temperature) at a rate of ±12oC/min. The experiments are conducted under nitrogen with a reaction time of 60 minutes at the final temperature. After the sample is cooled under nitrogen and screened again, the change in size distribution is calculated. The percentage thermal fragmentation of coal is given as a percentage decrease in Sauter diameter. The smaller the percentage decrease, the better the thermal stability. Thermal fragmentation is defined as: % Thermal fragmentation = d p before test − d after test p d p before test x 100 …(3) As illustrated in Figure 2, weathering / oxidation and moisture content affect the thermal fragmentation of coal sources. An extensive study revealed that the effect of moisture contributes to ±75% of the thermal fragmentation of coal [1]. This is not only surface moisture, but a combination of surface moisture and inherent moisture captured within the pores and the coal structure. Although moisture contributes significantly towards fragmentation, it is also affected by a complex interaction with other factors. 6 FIGURE 2 THERMAL FRAGMENTATION OF COAL SOURCES (effect of moisture and weathering) 70 % Thermal fragmentation Secunda Sasolburg 60 50 % Thermal fragmentation (dry) % Thermal fragmentation (w et) 40 30 20 10 0 A 3.5 B C D E F1 F2 F3 I & II Caking Caking of coal particles can be described as the softening or plasticity property of coal, which cause particles to melt or sinter together to form larger particles when heated. Caking of coal within the gasifier can cause pressure drop fluctuations and channel burning, resulting in unstable gasifier operation. In severe cases oxygen break-through can occur, which can be a safety hazard due to the possibility of downstream explosions. The caking propensity of coal is determined by pyrolizing a coal sample with a specific predetermined size distribution in an argon atmosphere at the typical gasifier pressure, i.e. ±26 bar. The sample is screened afterwards and the increase (if any) in particle size determined. This test is unique and was developed in-house by Sasol for characterizing coal under conditions similar to those prevail within the gasifier. Pressure significantly influences the caking propensity of coal. Coal with a medium to low caking propensity shows no caking at atmospheric conditions, and a highly caking coal will have a much lower caking propensity at atmospheric conditions than at 26 bar. Atmosphere (i.e. nitrogen, CO2, etc.) does not have a significant effect on the caking propensity of coal. According to previous experience, coal from sources with a relatively high caking propensity resulted in unstable gasifier operation and are therefore mixed with other coal sources having a low caking propensity to obtain an acceptable blend. Normal blends used for gasification at Secunda have a caking property of ±20 % and coal blends used in the Sasolburg plant have no or a very little caking. The variation in caking properties between the different coal sources used for gasification in Secunda and Sasolburg, as well as non-South African coal sources tested, are given in Figure 4. 7 FIGURE 3 CAKING PROPERTIES OF SASOL’S COAL COURCES Secunda Sasolburg 100 Non SouthAfrican 90 High risk 80 % Caking 70 60 50 40 Uncertain area 30 20 Safe operating region 10 0 A 3.6 B C D E F1 F2 F3 I & II a b d Ash fusion temperatures and ash composition The ash fusion temperature (AFT) of a coal source gives an indication to what extent ash agglomeration and ash clinkering is likely to occur within the gasifier. Ash clinkering inside the gasifier can cause channel burning, pressure drop problems and unstable gasifier operation. The results of an AFT analysis consist of four temperatures, namely the initial deformation temperature, softening temperature, hemispherical temperature and flow temperature. Ideal gasifier operation is to operate at a temperature above the initial deformation temperature in order to obtain enough agglomeration to improve bed permeability, but to operate below the ash melting temperature to prevent excessive clinkering. Ideal coal sources will thus have a big difference between the initial deformation temperature and the melting temperature. Secunda and Sasolburg coal sources currently used for gasification have an ash melting temperature > 1350oC and an initial deformation temperature of >1300oC. Non South-African coal sources tested (China, India and Ethiopia) have ash fusion temperatures similar to the Sasol coal sources. This does not imply that coal sources with lower ash fusion temperatures are not suitable for the Sasol-Lurgi gasification process, provided that gasifier operation is adopted accordingly. The ash composition, specifically the Ca and Fe content in the coal, gives a fair indication of the expected ash fusion behaviour. A Ca and/or Fe rich coal source normally has a low ash fusion temperature due to the fluxing properties of the Ca and Fe minerals. Although the standard AFT analysis is currently used as the only prediction tool for ash fusion temperatures of coal, literature studies have showed that this may not represent the actual flow temperature of certain minerals and mineral phases [6]. Fe, for example, in a specific phase can slag at temperatures as low as 700oC and then solidify again. This is not reflected by a standard AFT analysis. Sasol Technology, R&D Division, is currently investigating this issue. Visual investigation of actual ash produced from a fixed bed gasifier showed that the coarse and fine ash is sometimes extracted from the gasifier with the important middle fraction being absent. This can possibly be explained by the fact that some minerals already slag and clinker at low temperatures. 8 4. MAXIMUM THEORETICAL PURE GAS YIELD In order to compare the maximum theoretical pure gas yield of different coal sources, a detailed experimental evaluation, together with thermodynamic modeling, is conducted on the coal to simulate the gasification process. The theoretical pure gas yield predictions are subject to certain assumptions: • The thermodynamic model calculates the theoretical pure gas yield of the remaining fixed C after pyrolysis. • Experimental data for pyrolysis gas production and composition is added afterwards to obtain the maximum theoretical pure gas yield. Inputs in model: • Coal composition from proximate analysis. • Pyrolysis product yields. • Composition of pyrolysis gas. Assumptions made in model: • Percentage unconverted C reporting in the ash is 3% of total amount of C in the coal feed, but can be adjusted according to experimental data. • CH4 and water-gas shift reactions are at chemical equilibrium. CH4 formation and water-gas shift approach to equilibrium can be adjusted to match actual CH4 production figures and H2/CO ratios. • No kinetic, hydrodynamic or particle segregation effects are taken into account. This means that the model is not affected by load, particle size, coal reactivity, diffusion effects, heat and mass transfers. All of these factors may have an effect on the actual carbon conversion and yield predictions. Examples of theoretical PG yield predictions for a few South African coal sources and one non South-African source are shown in Figure 4. Exact agreement between predictions and plant data are normally not obtained, but experience showed that the predicted trends are valid (e.g. if blend composition changes and an increase in yield is predicted, then an increase is measured on the plant). 9 FIGURE 4 COMPARISON OF MAXIMUM THEORETICAL PURE GAS YIELD BETWEEN COAL SOURCES Pure Gas Yield (Nm 3/t DAF) 1700 1650 1600 1550 1500 1450 1400 1350 I & II X I & II plus 15% X Y Non South African 5. CONCLUSIONS The coal characteristics discussed in this paper are not the only properties affecting gasifier performance and stability, but are those properties that are measurable on laboratory scale and are easily related to gasifier performance. Interpretation of these results gives an indication of expected gasifier performance, and also the suitability of a specific coal source for Sasol-Lurgi fixed bed gasification. Interpretation of standard coal analyses and uniquely developed laboratory tests, together with previous experience gained by Sasol over the past 50 years, has put Sasol in a position to identify suitable coal sources for a Sasol-Lurgi fixed bed dry bottom gasification process. Sasol is furthermore in the unique position not only to have the ability to characterize and test coal from various sources on laboratory scale, but also to test new and current coal sources on an isolated commercial scale Sasol-Lurgi MK IV test gasifier at the Secunda site. These full scale tests require approximately 4000 tons of test coal, which allows a 6 day test run on a MK IV Sasol-Lurgi fixed bed dry bottom gasifier at a coal feed rate of ± 50 tons/h. Full scale test results are supportive to laboratory scale coal characterization data, since past experience showed that gasifier performance is usually not determined by one or two coal characteristics, but is dependent on the combined effect of all properties due to the large degree of interaction between them. This facility is used and will assist in future to further optimize product yields and to increase throughput by means of a thorough understanding of those coal characteristics that influence gasifier performance [7]. It is strongly recommended that full scale test work be conducted to confirm the design basis for new plants with unfamiliar coal sources. Sasol has experience and a proven track record on commercial scale test runs in Sasol Two and Sasol Three with South-African coal sources as well as with American coal sources, (e.g. DGC, EL Paso, CarteOil, Tristate, Phillips-Petroleum). 10 REFERENCES 1. 2. 3. 4. 5. 6. 7. 8. 9. 10. 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Keyser, M.J., Findings on the statistical evaluation of tests 14 to 23 on the test gasifier with a standard grate and standard grate/uniflo grate comparison, 28 January 2000. Sasol Annual Report 2000. Van Dyk, J.C., Development of an alternative laboratory method to determine thermal fragmentation of coal sources during pyrolysis in the gasification process, Fuel 80 (2001), pp. 245-249. Hirschfelder, H., Buttker, B., Steiner, G., Concept and realisation of the Schwarze Pumpe, FRG ‘Waste to Energy and chemicals centre’, IChemE Conference ‘Gasification in Practice’, Assolombarda, Milan, Italy, 26-27 February 1997. ACKNOWLEDGEMENTS The author gratefully acknowledges support and inputs received from the co-authors MJ Keyser, JW van Zyl as well as P van Nierop and also wishes to thank B Ashton and S du Plessis for their work contribution to the successful completion of this paper. 11