Matching Gasification Technologies To Coal Properties

International Journal of Coal Geology 65 (2006) 191 212 www.elsevier.
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Matching gasification technologies to coal properties

Anne-Gae lle Collot *
International Energy Agency-Clean Coal Centre, Gemini House, 10-18 Putney Hill, London SW15 6AA, United Kingdom Received 23 January 2004; received in revised form 18 May 2005; accepted 22 May 2005 Available online 9 August 2005
Abstract The gasification of coal to produce hydrogen for use either in power generation or/and for synthesis applications and transport is attracting considerable interest worldwide. Three types of generic gasifiers (entrained flow, fluidised bed and fixed bed gasifiers) presently in use in commercial gasification plants or under development worldwide are described. Their suitability for processing all types of coals is discussed. This includes an assessment of the impact of some of the major properties of coal on the design, performance and maintenance of gasification processes. D 2005 Elsevier B.V. All rights reserved.
Keywords: Hydrogen; Coal gasification; Gasifiers; Coal properties
1. Introduction Global electricity demand is increasing at about three times the rate of total energy while the industry is expected to reduce CO2 emissions because of global warming. As a consequence, there is pressure to improve the efficiency of energy use through changes in technology and to produce energy vectors such as H2 with near zero emissions of greenhouse gases. Oxygen-blown gasification may be the most attractive route for the production of H2 from coal with CO2 capture and sequestration as CO2 can be removed from the pressurised syngas (pre-combustion) rather
* Fax: +44 20 8780 17 46. E-mail address: collota@cia.org.uk. 0166-5162/$ - see front matter D 2005 Elsevier B.V. All rights reserved. doi:10.1016/j.coal.2005.05.003
than the exhaust gas (post-combustion). Removing CO2 from the exhaust gas in conventional combustion processes is feasible, but extremely expensive as this is carried out at atmospheric pressure and implies the treatment of a much larger volume of gas (10 times the volume of syngas). Another attraction of gasification technologies and, in particular, of Integrated Coal Gasification Combined Cycle (IGCC) is the possibility of cogeneration of electricity, H2 and chemicals. This contributes to the improvement of power generation efficiency compared with conventional pulverised coal fired plants as well as the reduction of emissions of greenhouse gases and particulates to the atmosphere (Clayton et al., 2002; Collot, 2003, 2004). H2 is currently produced from coal for use as an intermediate for the synthesis of chemicals such as methanol, ammonia/urea, FischerTropsch products
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and substitute natural gas (SNG) all over the world. However IGCC technology for commercial-scale plants is relatively recent. A summary of the main existing gasification processes is given in the following. There are presently sixty five Chevron Texaco owned or licensed gasification facilities worldwide that produce power, chemicals and H2 from coal (6 plants), oil derivatives and natural gas. Three of the coal gasification facilities produce ammonia, one produces town gas and electricity, one is an IGCC plant and one is producing methanol and chemicals. There are also other gasification projects in development or engineering for the production of diesel, H2/steam, syngas or electricity from either coal, natural gas or oil derivatives (Preston, 2003). Sasol, which was established in 1950 with the prime objective to convert low grade coal into petroleum products and chemical feedstocks currently operates three major coal to liquid (CTL) complexes based on the former Lurgi gasification process (now known as SasolLurgi dry bottom gasifier) in South Africa for the gasification of coal into Fischer Tropsch (FT) products (Van Dyk et al., 2001). The Great Plains Synfuels plant (Dakota Gasification) located in North Dakota (USA) has been producing substitute natural gas (SNG) from lignite using the same technology since 1984 (Lukes and Wallach, 2003). There are presently five gasification plants using the Shell gasification technology. Only one of them, the Nuon Power Buggenum IGCC plant in the Netherlands (formerly named Demkolec) which was started up in 1994, is fed with coal for the production of electricity. All the other gasification plants are fed with petroleum wastes to produce chemicals and/or H2 (Postuma et al., 2002). Eight other coal gasification plants using the Shell Coal Gasification Process (SCGP) for the production of chemicals are planned to be built in China and one in the USA (the Waste Management and Processors Inc project). The plants will all produce syngas for ammonia/urea, FischerTropsch liquids production or H2 for other chemical plants (methanol, oxo), replacing naphtha reformers, oil gasifiers or outdated coal gasifiers (Ploeg, 2001; Zuideveld, 2003). It is expected that the same technologies as the ones developed at the Nuon Power Bug-
genum IGGC facility, based in the Netherlands, will be used for the construction of future SCGP plants with power/H2. New projects based on demonstrated or commercial technologies for the production of hydrogen from coal for power generation are presently under development all over the world. The EAGLE project (coal Energy Application for Gas, Liquid and Electricity) is one of two Clean Coal Technologies (CCT) projects sponsored by the Japanese New Energy and Industrial Technology Development Organisation (NEDO) and the Ministry of Economy, Trade and Industry (METI) as part of a new strategy called the dDeployment of Coal Utilization Technology Development Strategy for the 21st centuryT. The objective of the EAGLE project is the development of an Integrated coal Gasification Fuel Cell combined cycle (IGFC) (Wasaka and Kubota, 2003). In Italy, a partnership of Sotacarbo, Ansaldo Ricerche, Enea and the University of Cagliari is presently developing a pilot scale gasifier for the production of H2 and power from coal/biomass and waste mixtures. The process, based on a 5 MW (thermal) gasifier combined with an internal combustion engine, will generate 0.2 MW power (Pratola et al., 2002). The New Zealand government through its science funding agency, the Foundation for Research, Science and Technology, has approved funding to develop a dtechnology platformT for hydrogen energy. CRL Energy Ltd is presently constructing a small scale atmospheric air blown fluidised bed gasifier pilot plant fed with local lignites for the production of an equivalent of 50 kW hydrogen energy (Pearce, 2003; S. Pearce, pers. comm., 2003). The FutureGen project in the USA is a 10 year, US$ 1 billion, demonstration project which was launched by the US government in February 2003 for the production of H2 from coal. The 275 MW prototype plant known as FutureGen will serve as a large-scale engineering laboratory for testing new clean power, carbon capture and coal to hydrogen technologies. Every aspect of the prototype plant will be based on cutting edge technologies (US DOE, 2003). Two new IGCC projects, the Kentucky Pioneer Energy project (Kentucky) and the Lima Energy pro-
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ject (Ohio) and one existing IGCC power plant, the Wabash River IGCC (Indiana), are being developed by Global Energy Inc in the USA. The objective of the Kentucky Pioneer Energy project co-sponsored by the US DOE, is to demonstrate the reliability, availability and maintainability of a utility-scale IGCC system using a high sulphur bituminous coal, coal fines and pelletized refuse-derived fuel (RDF) blend in a BGL (British Gas/Lurgi) gasifier (Bailey, 2001). The Lima Energy 580 MW gasification plant project is based on the use of the E-GASk technology, for the co-generation of H2 and electricity from petcoke. The Wabash River IGCC power plant also designed with an E-GASk entrained flow gasifier has been operating with a range of local coals since 1995. A molten carbonate fuel cell is currently being installed at the Wabash River IGCC plant instead of as originally planned, at the Kentucky Pioneer Energy plant. It is expected that operation of the integrated IGCC-fuel cell will start in spring 2004 first with natural gas followed soon after with coal syngas. The Wabash River IGCC power plant and the Lima Energy projects are owned by Global Energy although ConoPhillips recently acquired the patents and intellectual property associated with the E-GASk Technology for Gasification (P. Amick, pers. comm., 2004). There are also three projects of cogeneration plants (power and chemicals) projects sponsored by the US DOE as Early Entrance Coproduction Plants (EECP) (Amick et al., 2003; Rich et al., 2003; Shah and Schrader, 2003; Strickland and Tsang, 2003) and one project for the production of 100 t/d of dimethyl ether (DME) from coal in Japan (Ohno and Omiya, 2003). More details on these projects can be found in Collot (2004). New concepts based on the gasification of coal for the production of hydrogen are presently under development. Some of the concepts are based on the combination of three steps which include the gasification of coal (either steam gasification or hydrogasification), the shift reaction and carbon dioxide removal. Examples of this type of concept are the Absorption Enhanced Reforming (AER) process developed in Germany (Weimer et al., 2002), the Advanced Gasification-Combustion (AGC) project (Rizeq et al., 2002) and the Zero Emission Coal Alliance (ZECA) process (Ziock et al., 2002, 2003) developed in the USA, and the Hydrogen Production Reaction Inte-
grated Novel Gasification (HyPr-RING) process developed in Japan (Lin et al., 2002, 2003). Other concepts under development include membrane reactors (Sammells and Barton, 2003) and molten bath processes (HydroMaxR, HyMeltR) adapted from metal smelting processes existing in the iron making industry (Alchemix Corporation, 2003; Trowbridge et al., 2002). More details on these new concepts can be found in Collot (2003).
2. Coal gasification and its applications Gasification is defined as the reaction of solid fuels with air, oxygen, steam, carbon dioxide, or a mixture of these gases at a temperature exceeding 700 8C, to yield a gaseous product suitable for use either as a source of energy or as a raw material for the synthesis of chemicals, liquid fuels or other gaseous fuels. More details concerning the mechanisms of these reactions and their kinetics can be found in Kristiansen (1996). Common gasifying agents used in industrial gasifiers include a mixture of steam and air or oxygen with the amount of oxygen being generally one-fifth to one-third the amount theoretically required for complete combustion. The chemical composition and future use of the gas produced (syngas) varies depending on the following parameters: coal composition and rank coal preparation (particle size) gasification agents employed (oxygen or air) gasification conditions: temperature, pressure, heating rate and residence time in the gasifier ! plant configuration which includes: the coal feeding system (fed as a dry powder or as a slurry with water); the way by which contact between the fuel and the gasification agents is established (flow geometry); as to whether the minerals are removed as dry ash or molten ash (slag); the way heat is produced and transferred and finally, the way syngas is cleaned (sulphur removal, nitrogen removal, other pollutants removal). ! ! ! ! A large number of gasification technologies exist (see Section 1) and are detailed by Collot (2002). They can however be classified into three
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categories of gasifier configurations according to their flow geometry: ! entrained flow gasifiers, in which pulverised coal particles and gases flow concurrently at high speed. They are the most commonly used gasifiers for coal gasification. ! fluidised bed gasifiers, in which coal particles are suspended in the gas flow; coal feed particles are mixed with the particles undergoing gasification, ! moving bed (also called fixed bed) gasifiers, in which gases flow relatively slowly upward through the bed of coal feed. Both concurrent and counter concurrent technologies are available but the latter is more common. Other gasifier types have been developed based on rotary kilns or molten baths, but no gasifiers of these types are near to commercialisation. Gasification may also be carried out in situ in coal deposits (also known as underground gasification). The choice of a gasification technology is difficult as it depends on diverse factors such as (Vamvuka, 1999): ! ! ! ! ! ! ! coal availability, type and cost; gasifier end use locations and interactions; size constraints; production rate of energy; turndown requirements; heating value of the gas; allowed gas purity (S, CO2, etc) and cleanliness (tars, soot, ash) for meeting international regulations, plant requirements and further use of the gas products.
load capacity but also require coal to be pulverised. Coal can either be fed dry (commonly using nitrogen as a transport gas) or wet (carried in a slurry water) into the gasifier. They usually operate at high temperatures of 12001600 8C and pressures in the range of 28 MPa. Entrained flow gasifiers are all slagging gasifiers which are either lined with a refractory or a slag self-coating system. Raw gas exiting the gasifier usually requires significant cooling before being cleaned. There are two main methods of cleaning the gas by: using a high temperature syngas cooler, this can also include recycling of cooled gas to the gasifier, or quenching the gas with water. In entrained flow gasifiers flexible load operation is more difficult to handle than with the other types of gasifiers (fluidised and moving bed gasifiers). As entrained flow gasifiers have a small heat capacity and no inventory of process feedstocks, it is critical to control the coal:oxidant ratio within narrow limits through the entire operation in order to maintain a stable flame close to the injector tip. Entrained flow gasifiers are the most widely used gasifiers with seven different gasification technologies based on entrained flow gasifiers presently used at industrial scale or under development worldwide. Tables 1 and 2 give a summary of the main characteristics of seven entrained flow gasification technologies. More detail on each gasification process can be found in Collot (2002). 3.1. Slurryability and grindability In entrained flow gasifiers, coal is pulverised to ensure high carbon conversion during gasification. The grindability of a coal is measured by the Hardgrove Grindability Index (HGI). The HGI is used as a comparison basis against experience with other coals that have had satisfactory size distribution from grinding operations. Slurryability is another important coal property to take into account for slurry-fed gasifiers. These two properties are very much interrelated as the grind size distribution from a grinding mill affects the slurry properties of a coal and then the conversion in the gasifier. If a coarse grind size is used, a high solid concentration of slurry can be produced but the larger coal particles will not gasify as well as smaller particles that will tend to form a slurry with a lower concentration. A coal with a high HGI favours the
Coal choice maybe the least flexible factor for economic, geographical and political reasons and it is thus necessary to adapt the gasification technology to the base coal to be processed.
3. Entrained flow gasifiers In entrained flow gasifiers, coal particles concurrently react at high speed with steam and oxygen or air in a suspension mode called entrained fluid flow. Short gas residence times (seconds) give them a high
A.-G. Collot / International Journal of Coal Geology 65 (2006) 191212 Table 1 Main characteristics of existing dry-fed entrained flow gasification processes Technology Hitachi Operating conditions Operate under slagging temperatures at pressure of 2.5 MPa Gasifier Water cooled tube. Two sets of burners are installed tangentially to the gasifier sidewall allowing a spiral flow of coal and oxygen from the upper stage to the lower stage and making particle residence time much longer than those of a gas stream. Two-stages: combustion zone where O coal is injected. Gas produced diffuses to a reducing section where the remaining coal is added. A welded water tube vessel is contained in a pressure shell. Gasifier lined with a refractory. Syngas cooler is incorporated into the gasifier shell.
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Cooling and cleaning modes and ash removal system Gas is cooled in a syngas cooler (4508C) followed by a cyclone and a filter. Char and fly ash are recycled to the gasifier. Slag is water quenched and removed through a lock hopper. Char particles are collected in a syngas cooler and cyclones and recycled to the gasifier. Slag is water quenched and removed through a lock hopper. Syngas is quenched with recycled cleaned cooled syngas. Raw gas is dedusted in ceramic candle filters. Slag is water quenched and removed through a lock hopper. Syngas is quenched with cooled recycled product gas and further cooled in a syngas cooler. Raw gas is cleaned in ceramic filters. 50% gas is recycled to act as a quenching medium. Molten slag is removed through a slag tap and water quenched.
Mitsubishi heavy industries
Air blown
Prenflo
Four burners at the bottom
Shell coal gasification process
Operation at 24 MPa, at 1500 8C and above
A carbon steel vessel, which contains a gasification chamber, is enclosed by a non-refractory membrane wall. Coal is fed into the gasifier through horizontally opposed burners.
production of slurry with a high concentration for use in slurry-fed gasifiers. Important points to consider for the slurry concentration are whether or not it is pumpable, stable with particle settling and its rheology. A considerable amount of research has been dedicated to the development of techniques for the production of coal/water mixtures in the last 2030 years with a view to replacing oil by coal slurries (Thambimuthu, 1994). Results are also relevant to the preparation of coal slurry for gasification. Dooher et al. (1990) studied the slurryability of six bituminous coals and one subbituminous coal to develop a methodology for assessing the suitability of coals for slurry fed gasifiers. They reported that the most important coal properties affecting coal slurryability were: equilibrium moisture, fixed carbon, surface carbon/oxygen bonding as determined by electron microscopy and free swelling index. The equilibrium moisture (ASTM test D1412) of the coal is a measure of the inherent moisture rather than the coal surface moisture. According to Curran
(1989), experience showed that the equilibrium moisture correlates with pumpable slurry concentrations. Kanamori et al. (1990) performed tests on twenty coals and found that it was possible to predict the slurryability and stability of coal slurries with the oxygen to carbon ratio in coal, the oxygen-containing groups and the clay minerals. All coals that can be pulverised (high HGI) can be processed in dry-fed entrained flow gasifier systems. Bituminous coals with their low inherent moisture content and hydrophobic nature are the coals of choice for the commercial preparation of high solid content coal/water fuels. However higher and lower rank coals can also be processed in slurry fed gasifiers provided the coal is pre-treated or an additive is used (Thambimuthu, 1994). 3.2. Coal reactivity Highly reactive coals provide high carbon conversion at moderate gasifier temperatures improving
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Table 2 Main characteristics of existing slurry fed entrained flow gasifiers Technology Babcok borsig power (Noell) Operating conditions Dry-fed or slurry-fed gasifier. Operate in the range 13501600 8C at pressure of 2.6 MPa Gasifier Either covered by a cooling screen (refractory on which are mounted cooling tubes supported by pins) for coals with a ash content N 1%wt or a cooling wall (other feedstocks than coal). Two-stage pressure shell lined with refractory. Cooling and cleaning modes and ash removal system Raw gas is cooled with water spray and further cooled before being recycled to the gasifier. The molten slag is water quenched. The granular slag is removed from the gasifier through a lock hopper. Crude gas is cooled in a firetube syngas cooler, which is a boiler system with the hot gas circulating on the boiler side as opposed to a water gas cooler. Syngas is cleaned in metal filters and ash and char particles are re-injected into the gasifier. Molten slag is removed through a tap hole into a water quench. Raw gas can either be cooled and cleaned from slag by water quenching or radiant cooler. The raw gas and slag flow out towards the bottom of the gasifier. The molten slag is water quenched and removed through a lock hopper.
E-GASk
Slurry is preheated prior to injection. 80% of the coal is injected through 2 burners and is partially combusted at temperatures of 13501400 8C and 3 MPa pressure. The remaining coal slurry is injected in the upper stage and reacts with the fuel gas produced in the lower stage.
Texaco
Slurry-fed through burners at the top of the gasifier. Operate at temperatures in the range 12501450 8C and 38 MPa pressures.
Pressure vessel with refractory lining.
overall system efficiency. The reactivity of coal chars under gasification conditions is a major determinant of the gasifier size and design. Char reactivity has a significant influence on the degree of char recycle and on the volume of oxidant required for the gasifier. Boyd and Benyon (1999) studied the reactivity of six Australian coals in a laboratory-scale pressurised Drop Tube Furnace (DTF) and a Pressurised Thermogravimetric Apparatus (PTGA). Chars were produced in the DTF and their reactivities were measured with the PTGA. Their results were then extrapolated to full-scale entrained flow gasifiers (Shell, Texaco and Mitsubishi Heavy Industries) using a dsensitivity method of analysisT. They reported that the effects of change in char reactivity (coal) were the largest in the air blown MHI process and the lowest in the Shell process. They concluded that even though the rank of the six coals studied was very similar, they had significant differences in reactivity. These differences were due to physical characteristics as well as the chemical characteristics defining ASTM rank. A correlation with fixed carbon, volatile matter or specific
energy was not found. They also pointed out that inorganic constituents may have a small effect on coal reactivity by acting as catalysts. More fundamental studies (Kelly et al., 2001; Roberts et al., 2000) to better understand the process of coal conversion focused on the effect of operating pressure, temperatures and heating rate on coal reaction behaviour under conditions relevant to entrained flow gasification systems. The work reported by Kelly et al. (2001) provided comparative data on 13 Australian coals usually processed in entrained flow gasifiers worldwide. Volatile yields of the coals were determined in a wire mesh reactor and results showed that coal volatile yield decreases with increasing reaction pressure despite the enhancing effect of heating rates. The greatest reduction in volatile yield with pressure was observed for the higher coal ranks. Char gasification of the same coals was studied in a PTGA. Results indicated that char gasification in CO2 atmospheres was strongly influenced by coal rank, whereas steam and O2 gasification did not show much of a coal rank effect on apparent reaction
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rates. These results suggest that other coal characteristics, such as crystallinity and coal mineral matter are playing a greater role under these conditions. The conversion profiles of each char were also different with the different gases tested (CO2, H2O, O2). This fundamental study claims to be useful for predicting coal performance in practical high-pressure reaction systems as well as contributing to the resolution of problems associated with Australian coals in international demonstration and pilot-scale facilities. The same authors are now expanding their study to international coals (Harris et al., 2003; Roberts and Harris, 2003). In practice, reactive coals can be gasified at lower temperatures and hence at higher cold gas efficiency, whereas less reactive coals may need higher gasification temperatures in order to achieve adequate conversion efficiencies. At the same time, the temperature must be high enough to yield a tappable slag. Thus the preferred operating strategy for a coal is always a balance between reactivity and slag tapping considerations. 3.3. Ash/slag properties Entrained flow gasifiers are usually recommended for coals with a low ash content for both economical and technical reasons. Considering that gasifier operating conditions are kept constant, an increase in coal ash content will lead to a decrease in gasification efficiency and an increase in slag production and disposal. These three factors contribute to an increase in the overall cost of the process. The decrease in gasification efficiency is mainly due to an increase in oxygen consumption which is necessary to melt the minerals as well as a thermodynamic penaltythe heat in the slag exiting the gasifier cannot be fully recovered. An increase of the slag quantity can also cause blockage of the slag removal and cleaning devices. It is nevertheless difficult to draw an optimum ash content value for coals processed in entrained flow gasifiers. This is because some of the technologies require a minimum ash content. These technologies (BBP, Hitachi and SCGP, see Tables 1 and 2) use a slag self coating system that has to be covered by slag to function and minimise heat loss through the wall of the gasifiers.
3.3.1. Ash chemical composition In entrained flow gasifiers, the high temperature of gasification (usually up to 1600 8C) combined with pressures of up to 3 MPa can accelerate the deterioration of refractory lining existing on the walls of some gasifiers. Current refractory materials, which are expensive pieces of gasifier equipment, have typically a service life of no more than two years and the study of their service life is an important parameter for the selection of base coals for a gasifier. Texaco developed a method to predict gasifier refractory life based on coal ash ASTM fluid temperature which depends directly on the composition of the ash/slag (see also Section 3.3.2). Dogan et al. (2001) performed an extensive analysis of spent refractories from commercial gasifiers and concluded that some compounds present in coal slag (SiO2, CaO, iron oxides) can penetrate deeply into high chrome refractory materials and eventually give rise to cracks that lead to material loss. 3.3.2. Ash fusion temperature (AFT) or ash melting point In slagging gasifiers, the ash flows down the gasifier walls and drains from the gasifier as a molten slag. Coals selected for slagging gasifiers should thus have an ash fusion temperature (AFT) below the operating temperature of the gasifier (14001600 8C). In practice, AFT can be lowered by either the addition of flux, such as limestone, or by blending with low ash fusion coals. AFT is widely used as a guide to slag behaviour and can be simply and quickly determined by laboratory standard methods, which consist of coal ashing by slow heating in air. However this method does not reproduce real commercial gasification conditions and other tests have been developed. For example, engineers at the Polk power station (Texaco technology) in the USA use the difference between the ASTM ash fluid temperature, determined under reducing conditions and the gasifier operating temperature plotted versus refractory liner life, to estimate the optimum operating temperature of the gasifier for successful tapping (McDaniel and Shelnut, 1998; McDaniel et al., 1998). Shell uses the ash melting point as a preliminary indication for a new coal and to check if the addition of flux would be required (Ploeg, 1997). The temperature of 1400 8C is considered as a breaking point with higher values of ash fusion temperatures requiring flux. For an actual design/operation a complete analysis of the ash should
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be done to confirm the first approach and it is then necessary to either perform further measurements on slags produced in a gasifier or to rely on other methods which can predict ash fusion temperature based on the chemical composition of the ash. Ashizawa et al. (1993) developed a method to determine the ash fusion temperature of 26 coals as a function of the chemical composition of their ash (acidity). The acidity is defined as follows: Acidity = (SiO2+Al2O3)/ (Fe2O3 + CaO + MgO + Na2O+K2O). To validate the dacidityT method they produced slags under oxidising conditions in a 2 t/d pilot plant gasifier developed by CRIEPI (MHI technology). The slags produced were analysed and compared to results obtained by the dacidityT method. They found a correlation between the ash composition (acidity) and the ash fusion temperature and the equation giving the relationship between Tf (fusion temperature) and X (acidity) is as follows: Tf 27:7931TX 1236:89: This dacidityT method was then used to predict the ash fusion temperature of coals in the presence of flux and coal blends. Results obtained showed that the prediction was even more precise when flux was added to the coals. This could be explained by the lowering of the importance of the influence that minor oxides have on the ash fusion temperature when flux is used. 3.3.3. Slag viscosity and temperature of critical viscosity (Tcv) As the ash melts, its viscosity has to be low enough to enable it to flow down and drain from the gasifier. The viscosity of the slag, which depends on the slag composition, is one of the most critical factors in the operation of slagging gasifiers. There are two types of coal slag behaviours: ! Type I exhibits a glassy behaviour, which means that when the slag cools down the increase in the viscosity of the slag, is predictable and continuous. ! Type II exhibits a crystalline behaviour when cooling down and, as a consequence, the flow becomes non-Newtonian and the viscosity of the slag
increases sharply below a temperature called the temperature of critical viscosity (Tcv). This type of slag will behave the same as Type I (Newtonian flow) at temperatures well above the Tcv. However in the Tcv region crystallisation begins to have a significant effect on the viscosity of the slag and induces the possibility of blockage of the tapping system with crystalline deposits. Tcv is the minimum temperature required for safe operation with slags that exhibit crystalline behaviour rather than glassy behaviour. In practice the operating temperature of the gasifier must be high enough to maintain the slag in the Newtonian flow region (Scott and Carpenter, 1996). Tcv depends on slag composition and, in particular, on the ratio of SiO2/Al2O3 in the slag. It has been established that slag viscosity must be low enough (2515 Pa.s), with an optimum value of 15 Pa.s at temperatures of 14001500 8C, to achieve successful slag tapping (Browning et al., 1999). As a consequence, viscosity models have been developed to predict coal ash slag behaviour in coal slagging gasification processes; this is necessary for optimisation of the operating parameters (coal selection, blending and flux) in order to achieve stable process conditions and to reduce operating costs. Shell uses a model (bSLAGSQ program) developed by Mills and Broabent (1994) to predict ash behaviour for the range of coals in the SCGP (Ploeg, 1997, 2000). The model gives an estimation of the physical properties of the slags from their chemical compositions. This model was originally developed for metallurgical slags but was later successfully applied to coal slags, provided that all components present at concentrations above 5%wt were included for the calculations. The bSLAGSQ model contains routines for the estimation of ash fusion temperatures, viscosities, densities and surface tensions. Fluxing agents (mainly limestone) are then used to balance the slag viscosity of the different coals fed. Eastman Chemicals developed an in-house test in order to determine the quality of their feedstocks prior to gasification in a Texaco gasifier (Trapp, 2001, 2002). Considering that the typical standard viscosity or melt point tests usually used to estimate slag viscosity are inadequate to fully predict slag behaviour in the gasifier, they determined a continuous curve of
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viscosity as a function of temperature. Eastman Chemicals also reported, without giving more details, that they co-fed slag modifiers (probably limestone) to positively affect certain ash properties. As a result, dbetter qualityT coals were gasified leading to a reduction in operation difficulties and shutdowns. Oh et al. (1995) studied the slag characteristics of four US coals used in a Texaco gasifier. They stated that all the empirical models used to determine slag viscosity as a function of temperature and composition can only be applied with success for slags having a dglassyT behaviour and that the models often fail to predict correct slag viscosity behaviour when a crystalline phase appears during cooling. Patterson et al. (2001) studied the slag characteristics of 68 Australian coals for their utilisation in slagging gasifiers. They established an extensive slag viscosity database versus ash composition, temperature and flux addition (Patterson and Hurst, 2000). They concluded that the slag viscosities of Australian coals can be properly predicted from their models for tappings at 1500 8C, however these predictions were not validated for all the coals at 1400 8C due to slag crystallisation. The same authors (Patterson and Harris, 1998) also reported that after addition of limestone flux (up to 20% CaO) to some Australian coals having a very low iron content (b 2.5% Fe3O2 in ash) and a very high ash flow temperature (N 1600 8C), the slag viscosities of those coals were independent of SiO2/Al2O3 in the range 1.25 at the optimum viscosity of 15 Pa.s. They then concluded that variability in ash composition of those coals was not a problem and that the addition of a fixed amount of limestone flux by weight of coal should be effective at all times. The effects of slag composition on the Tcv still remain poorly understood and need more investigation. Nevertheless, three solutions can be implemented to tackle the problem arising in slagging processes when using coals having a high ash fusion temperature and slags with high critical viscosity temperature (Tcv). The most common solution implemented is flux addition (either CaO or FeO) in order to decrease ash melting points and slag viscosity. The viscosity models will give the optimum quantity of flux to add to the coal in order to have a continuous flow. The second solution is blending with a low ash fusion coal to provide the necessary CaO and FeO. Blending
presents two advantages: The first one is that it could help to overcome limitations arising from slag crystallisation at the slagging temperature by choosing the appropriate coal. The second one is economic as blending can minimise or even avoid the use of flux. The third solution would be to increase the gasifier operating temperature above 15001600 8C to achieve the necessary slag tap viscosity or to reduce the rate of flux addition. However this solution would necessitate an additional oxidant requirement that would lead to a reduced cold gas efficiency and a decrease in refractory life for gasifiers lined with a refractory layer. The optimum ash fusion temperature (AFT) and critical temperature viscosity (Tcv) recommended for smooth slag tapping in entrained flow gasification processes differ depending on the operating temperature of the gasifier. In principle, the AFT of a coal should be below the operating temperature of the gasifier (14001600 8C). Tcv is the minimum gasifier operating temperature required for safe operation with slags that exhibit crystalline behaviour. Tcv depends on slag composition (SiO2/Al2O3). A solution commonly applied to widen the range of coals that can be processed in entrained flow slagging systems is to either blend them with flux or with a coal having a low AFT. 3.3.4. Ash fouling Some of the minerals present in coals are entrained in the gas stream and can lead to fouling at different locations downstream of the gasifier. Fouling problems can often be characterised as the impaction of particles into a sticky layer of material in piping that could occur in the quench zone of the gasifier and/or in the cooling sections downstream of the gasifier. As an example, during the first commercial operating year of the Wabash River repowering plant (EGASk technology) the cleaning device of the plant experienced problems related to ash deposition at the inlet of the firetube boiler and particulate breakthrough in the particulate filter system. These problems necessitated a large-scale capital improvement programme. The Polk Power station (Texaco Technology) also experienced several convective syngas cooler pluggings that led to serious damage of the combustion turbine during the second and third years of commercial operation (US DOE, 2000). This was
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particularly due to the ash constituents of some of the fuels tested. Two major research and development programmes on Coal Ash Behaviour in Reducing Environments (CABRE I and II) were initiated by a consortium of industries in partnership with the US DOE, the Netherlands Energy Research Foundation (ECN) and the Netherlands Agency for Energy and the Environment (NOVEM) (Kiel and Bos, 1999). A series of tests was performed with seven coals and a coal mixture currently used in industrial IGCC power plants. The fuels were subjected to an initial particle temperature of more than 2000 8C followed by a gasification temperature of up to 1400 8C under 1.0 MPa pressure. These conditions were considered as a realistic gaseous environment for entrained flow gasification simulation. It was reported that in the presence of H2S in the gas phase there were small deposits of FeS on the surface of the ash (solidified Ca/Fe-containing aluminosilicate spheres) collected in the cyclone sample of the PEFG-simulator. The authors explained that FeS formed in the vapour-phase condensed on the ash sample during quenching in the collection probe. All the experiments and observations undertaken on the different ash samples led to the building of an ash deposition model that is claimed to predict ash partitioning, ash fouling and also ash slagging under gasification conditions in entrained flow gasifiers (Kiel et al., 2000). 3.4. Sulphur and chlorine contents During gasification sulphur originally present in coal is converted to H2S which is highly corrosive to syngas coolers and causes serious damage to heat exchange systems as well as having an impact on the cost of sulphur removal and recovery units. Sulphur content in coals is reported by Shell (Ploeg, 1997) and Texaco (McDaniel and Shelnut, 1998; McDaniel et al., 1998) to be one of the major coal properties to take into account for the design of a gasification plant. Most coals also contain minor quantities of chlorine with concentrations ranging from 0.05 wt.% to 0.5 wt.% with 0.10.2 wt.% being the most typical. As an example, 0.1% Cl in coal will result in 200400 ppm of HCl in the syngas. HCl can react with available metal compounds present on flyash, which has accumulated on syngas coolers. This results in local depos-
its containing up to 15% chlorides such as FeCl2, NaCl, CaCl and causes other problems downstream such as those at the Wabash River repowering plant (E-GASk technology) which experienced during its first commercial year of operation, the poisoning of the COS catalyst by chloride vapours present in the syngas (US DOE, 2002). Alloy composition is one of the main factors influencing corrosion behaviour and most of the research in this area has focused on the development of new materials with enhanced resistance to corrosion. Most of the high temperature alloys used for syngas coolers are made of Cr, Ni and Al with some minor elements influencing their properties. Bakker (1997, 1998, 1999, 2000) studied mixed oxidant corrosion in gas simulating conditions under a non-equilibrium state in syngas coolers of coal gasifiers and reported that corrosion losses were a function of the PS2/PO2 ratio and defined three types of corrosion depending on this ratio and the concentration of HCl in the syngas. 3.5. Comments All entrained flow gasifiers are slagging gasifiers and each technology has slightly different requirements for coal properties depending on the design. There is a minimum ash content required for gasifiers with slag self-coating walls which have to be covered by slag to function and minimise heat loss through the wall. A maximum ash content is also usually fixed for each type of entrained flow gasifier as the tolerance to ash content depends on economic and technical factors. Gasifiers lined with a refractory are susceptible to some of the compounds present in coal slag (SiO2, CaO, iron oxides) which can penetrate deep into the refractory and eventually give rise to cracks that lead to material loss. The optimum ash fusion temperature (AFT) and critical temperature viscosity (Tcv) recommended for smooth slag tapping in entrained flow gasification processes differ depending on the operating temperature of the gasifier. In principle, the AFT of a coal should be below the operating temperature of the gasifier (14001600 8C). Tcv is the minimum gasifier operating temperature required for safe operation with slags that exhibit crystalline behaviour. Tcv depends on slag composition (SiO2/Al2O3). A solution commonly applied to widen the range of coals
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that can be processed in entrained flow slagging systems is to either blend them with flux or with a coal having a low AFT. The tolerance of entrained flow gasifiers to sulphur and halogens depends on the composition and resistance of the material used in the cooling, cleaning and tapping systems but also on the operating conditions of the gasification process (gasifier temperature), as well as the processing capacity of the downstream equipment, such as the sulphur plant.
and burnt in a separate combustion unit (hybrid cycle) or recirculated into the gasifier. Fluidised bed gasifiers may differ in ash discharge conditions, being dry or agglomerated. One of the main advantages of this type of gasifier is that they can operate at variable loads which gives them a high turndown flexibility. There are six types of gasification processes using fluidised bed gasifiers. Only two of them have been operated at industrial scale. Their main characteristics are summarised in Tables 38. 4.1. Coal reactivity As fluidised bed gasification is a low temperature process (8001050 8C), the reactivity of the coalderived char must be sufficiently high. The reaction which plays the biggest role in the coal conversion rate is the endothermic carbon-steam reaction that results from coal devolatilisation. The rate of this reaction determines whether or not a coal is sufficiently reactive for fluidised bed gasification. Some examples of studies of coal reactivity impact on fluidised bed gasification processes are given in the following. Clemens et al. (2000) have studied the applicability of clean coal gasification technologies to New Zealand coals using a laboratory-scale fluidised bed gasifier and a pressurised thermogravimetric analyser (PTGA). They determined the reactivities of New Zealand coals, which include lignites and sub-bituminous coals, and compared them with those of overseas coals known to have sufficient reactivity to be gasified in fluidised bed gasifiers. A peculiarity of New Zealand coals is their high content in alkaline elements which can probably act as a catalyst and hence
4. Fluidised bed gasifiers Fluidised bed gasifiers, with the exception of the Transport Reactor Gasifier which is midway between a fluidised bed and an entrained flow gasifier, can only operate with solid crushed fuels (coal: 0.55 mm, less than 50 Am for the Transport Reactor Gasifier) that are introduced into an upward flow of gas (either air or oxygen/steam) that fluidises the bed of fuel while the reaction is taking place. The bed is either formed of sand/coke/char/sorbent or ash. Residence time of the feed in the gasifier is typically in the order of 10100 s but can also be much longer, with the feed experiencing a high heating rate from the entry in the gasifier. High levels of back-mixing ensure a uniform temperature distribution in the gasifier. Fluidised bed gasifiers usually operate at temperatures well below the ash fusion temperatures of the fuels (9001050 8C) to avoid ash melting, thereby avoiding clinker formation and loss of fluidity of the bed. A consequence of the low operating temperatures is the incomplete carbon conversion in a single stage and it is therefore common for the residual char to be either removed
Table 3 The BHEL fluidised bed gasifier Feeding system and operating conditions Crushed coal injected through lock hoppers. Operates at a temperature of 1000 8C and 1.3 MPa pressure. Gasifier Refractory lined reactor with 1.4 m inside diameter expanding to 2 m at the upper section of the gasifier.
Ash discharge mode Dry granular ash withdrawn from the bottom of the gasifier through a water-cooled screw extractor and discharged through a lock hopper.
Cooling and cleaning modes Fines collected in three cyclones can be recycled in the gasifier.
Comments 168 t/d air-blown gasifier designed for the gasification of Indian coals with high ash content.
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Table 4 The High Temperature Winkler (HTW) gasifier Feeding system and operating conditions Coal dropped from a bin via a gravity pipe into the gasifier. Gasifier is fluidised from the bottom. Additional gasification agent is introduced at the freeboard (900950 8C). Operating pressure is 13 MPa Gasifier Bed is formed of particles of ash, semi-coke and coal and is maintained at 800 8C. Ash discharge mode Dry ash is removed at the bottom of the gasifier via a discharge screw. Cooling and cleaning modes Raw gas is passed through a cyclone to remove particulates that are recycled to the gasifier. Either water cooled or fire tube syngas cooling system. Comments Successfully applied for the synthesis of methanol from lignites between 1986 and 1997. Wide range of coals tested. Plan to replace old Lurgi dry ash reactors by HTW technology at Vresova IGCC plant (Czech republic)
increase char gasification reactivity. Calcium, which is present in significant proportions in New Zealand coal ashes is one of the most efficient catalysts. Although the overseas coals they studied had very different characteristics (very high ash content in German brown coals and very high water content in Australian lignite), the authors concluded that New Zealand coals were readily able to meet the reactivity criterion for being processed successfully in future fluidised bed IGCC plants. A laboratory at Imperial College London (UK), studied the impact of several coal characteristics on the gasification reactivity of some internationally traded coals in bench scale reactors that could mimic the behaviour of single coal particles in the ABGC (Megaritis et al., 1998; Collot, 1999; Messenbo ck et al., 2000; Zhuo et al., 2000a; Lemaignen et al., 2002). The characteristics of coal studied included coal maceral composition and coal mineral matter composition. CO2-gasification experiments with coals and their macerals revealed that it was difficult
Table 5 The Integrated Drying Gasification Combined Cycle (IDGC) Feeding system and operating conditions Feed coal is pressurised in a lock hopper and fed into a dryer where it is mixed with the hot gas leaving the gasifier. The gasifier operates at 900 8C and 2.5 MPa pressure. Ash discharge mode Char and ash are collected at the bottom of the gasifier and burnt in a separate boiler.
to predict coal gasification reactivity in the ABGC only from coal maceral composition, although prediction of coal pyrolysis reactivity matched quite well results obtained in the bench scale reactors. However the authors (Zhuo et al., 2000b) concluded that the nature and reactivity of the chars depend on a number of factors which include not only the maceral content of the coals but also the conditions of char formation, such as temperature, pressure, residence time and parent coal. These affect the two main processes that seem to govern the reactivity, which are the deposition of secondary carbon (by the intraparticle decomposition of volatiles) and change in the base char structure (caused by the development of fluidity and escape of volatiles from the melt and its re-solidification). Their results showed that under conditions relevant to the ABGC, vitrinite is a maceral that melts and swells, liptinite also melts but does not swell or agglomerate and loses a large proportion of its mass by pyrolysis and the third maceral, inertite, does not melt, but only loses a small proportion of its mass under pyrolysis
Cooling and cleaning modes The heat of the gas produced is used to dry the coal whilst the evaporation of water from the coal cools down the gas: there is no need for a syngas cooler.
Comments Air-blown gasification system specially developed for the gasification of high moisture (up to 62%) low rank coals.
A.-G. Collot / International Journal of Coal Geology 65 (2006) 191212 Table 6 The Kellog Rust Westinghouse (KRW) gasifier Feeding system and operating conditions Crushed coal is fed at the bottom through lock hoppers. Operates at pressure up to 2 MPa. Gasifier Combustion of a portion of the coal and agglomeration of the ash occurring at temperatures of 11501260 8C around the tip of the feed nozzle. Large agglomerated particles formed are removed at the bottom of the gasifier while finer particles flow upwards to the upper section where gasification and sulphur capture occur. Ash discharge mode The separation of the large agglomerated particles formed of char, ash and sorbent is done through a char-ash separator at a minimum fluidisation velocity between that of the char and ash so that the char is kept in the bed while ash and sorbent are removed from the gasifier via an ash feed hopper. Cooling and cleaning modes Raw gas (900 8C) passes through a cyclone and particles collected are recycled to the gasifier. The gas is cooled to 600 8C and enters a hot gas cleaning system. A portion of the gas is re-circulated to the gasifier to control the temperature of the agglomeration zone. Comments
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Air-blown system. The Pinon Pine IGCC plant was designed for bituminous coal but other coals were tested.
and is unreactive towards the gasification agent, CO2. The suite of coals tested were rich in vitrinite and the authors claim that this maceral seemed to dominate the morphological changes that occurred during char formation. The second part of their study was on the influence of mineral matter composition in coals. Experiments consisted of the pyrolysis and CO2-gasification of two coals, which were first demineralised and then impregnated with different salts, in a wiremesh reactor in which gasification conditions were relevant to the ABGC. Results from their work showed that although mineral matter contents clearly affect coal conversion under pyrolysis and gasification conditions, it was difficult to find systematic patterns for the effect of specific inorganic components on different coals. The authors also concluded that it
Table 7 The transport reactor gasifier Feeding system and operating conditions Coal is ground close to 50 Am. Coal and sorbent are fed separately through lock hoppers into the mixing zone. Operates at temperatures between 8701000 8C and pressures of up to 1.5 Mpa Gasifier Operates with a much higher circulation rate and higher velocities than conventional fluidised bed gasifiers. Gas and entrained particles move up from the mixing zone into the riser and enter a disengager.
was almost impossible to develop a predictive tool linking catalytic activity to amounts and composition of particular inorganic components (Lemaignen et al., 2002). 4.2. Bed agglomeration and in bed desulphurisation In fluidised bed gasifiers, mineral matter is a major constituent of the bed and, as a consequence, the characteristics of coal ash can have a major impact on the operation of the gasifier. Ash fusion temperature is, in particular, a parameter to study as some components of the mineral matter can soften at the bed temperature usually leading to agglomeration and uneven fluidisation. Disturbances will thereby result in problems of blockage in the bottom product dis-
Ash discharge mode Both the char and ash extracted from the gasifiers, and collected in the barrier filter, are cooled, depressurised in lock hoppers and combined prior to combustion in an atmospheric fluidised bed combustor.
Cooling and cleaning modes The disengager removes the larger particles by gravity separation and the remaining particles are removed in a cyclone. Solids collected are recycled to the mixing zone.
Comments Designed to operate as a gasifier or a combustor. The reactor is under commission and is being tested with several fluxes. The multiple passes of the coal/char through the gasification zone leads to a high carbon conversion of 95%.
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Table 8 The Air Blown Gasification Cycle (ABGC) Feeding system and operating conditions Coal is injected with sorbent to retain sulphur in bed. Operates at temperatures up to 1000 8C and pressures up to 2.5 MPa Gasifier Gasifier based on a spouted bed. Only 7080% of the coal is gasified. Ash discharge mode Partially gasified char and other residues are transferred to an atmospheric pressure circulating fluidised bed combustor operating at 1000 8C. Cooling and cleaning modes Syngas is first cleaned in a cyclone then cooled to 400 8C and cleaned by a ceramic filter. Comments The preferred fuels are high-volatile bituminous coals or possibly lower rank coals (subbituminous, lignites/brown coals)
charge and also in the re-circulating system if there is one. West et al. (1994) studied the agglomeration properties of eight UK coals in a pressurised spouted fluidised bed and an atmospheric fluidised bed pilot plant. The authors observed the formation of a FeSO coating on large clay-derived particles present in coal and claimed that these particles could be the precursors to agglomerate formation. They concluded that iron present in coal as Fe2O3 (pyrite) plays a crucial role in the formation of agglomerates in fluidised bed gasifiers. Uemiya et al. (1997), who studied the agglomeration formation of coals with an Fe2O3 content of 16% and 6.2% in a jetting fluidised bed gasifier, reported that iron compounds were concentrated near the surface of the agglomerated particles. Holden and Hodges (1997) studied ash clinker formation during the gasification of Australian brown coals in a fluidised bed gasifier (0.3 t/d) prior to the development of the IDGCC. Their results showed that the rate of clinker formation in the bed and near the air nozzles was related to the bed temperature as well as the amount of sodium and silica (quartz and clay) in the feed coal. They claimed that the reaction of gaseous sodium species with silica particles could result in the formation of sodium silicate phases, which melt at low temperature (b 1000 8C). When the operating temperature exceeds the melting point of sodium silicate, particles become sticky and can agglomerate on impact, resulting in the formation of porous clinkers. More drastic gasification conditions, such as higher gasification temperature or longer particle residence time, will produce a molten or fused material, which can capture and flow around ash particles, forming a consolidated clinker.
4.2.1. In bed-desulphurisation In most of the fluidised bed gasification processes sulphur released during gasification (essentially H2S and COS) is retained in the bed in the form of sulphides of calcium and/or iron when using limestone or dolomite. Retention efficiency is usually around 90%. Although gasifiers are usually insensitive to sulphur coals with a higher sulphur content will require a higher addition of sorbents which will consequently increase the quantities of solids discharged by the process and hence its overall cost. Alternatively in bed-sulphur capture can also be adversely affected by coal ash chemistry and particularly by the presence of alkalis in coal that promote bed agglomeration. Sulphur capture on limestone requires a bed temperature of 870 8C or higher for sorbent activation by calcination. At this temperature alkalis are likely to cause agglomeration in the fluidised bed. Thus the gasification of high alkali coals requires careful control of the temperature in a range at which carbon conversion can be maximised (Sondreal et al., 1997; Rousaki and Couch, 2000). 4.2.2. High free swelling index The caking and swelling characteristics of a coal can be described by the high free swelling index which is related to ash composition. During the heating phase (360450 8C), coal particles pass through a plastic state and swollen particles can then combine to form agglomerates. Agglomerate formation can be reduced by passing the temperature range of the plastic state rapidly and by mixing the swollen particles with non swelling particles, such as demonstrated at the HTW Wesseling gasification plant (Germany) in which Pittsburgh No 8, a high swelling index coal, could be processed successfully in the plant only if it
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was mixed with a coked (non-swelling) fluidised bed material prior to injection into the gasifier. However test operations (air-blown and oxygen-blown) performed at Wesseling showed that, even with a pneumatic feeding system, Pittsburgh No 8 input could not be more than 1.5 t/h. Up to this coal feed rate, the formation of agglomerates was controlled by strong base fluidisation and stepped-bottom product discharge. Changing the injection pipe into the flow direction of the gas would have improved rapid mixing of the feed coal with the fluidised bed material (Adlhoch et al., 1993). The spouted bed designed for the ABGC plant in the UK nearly eliminated the agglomeration problem by introducing the coal through the spout in a dilute phase hence limiting coal particles interactions during the plastic phase. However the rapid heating rate of the coal in the spout reduces its swelling propensity implying a preference for the processing of low swelling coals in the ABGC (Welford et al., 2000). 4.3. Gas cleaning system and corrosion Most of the studies on corrosion have been performed by simulation of syngas from dry fed entrained flow gasifiers (see Section 3.4). However Norton et al. (2000) recently studied the effect of a CO-based gas mixture containing 0.1% H2S under non-equilibrium conditions at 550 8C on a series of five alloys used in syngas coolers. The low percentage of H2S present in the syngas represented the average concentration of H2S that can be found in syngas produced in fluidised bed gasifiers, where coal is gasified in the presence of limestone, which can capture up to 90% of the sulphur as solid CaS. The alloys tested, although cheaper than the ones used in syngas coolers of dry fed entrained flow gasifiers, resisted corrosion well. According to Norton et al. (2000), their corrosion resistance was improved by having an ash deposit on their surface. The same authors (Bakker, 1999, 2000) did some corrosion tests of syngas with an even lower concentration of H2S (0.05% instead of 0.8% for entrained flow gasifiers) and HCl (0.01% instead of 0.04%) to simulate syngas produced in hybrid coal gasification systems, such as the ABGC which also uses dolomite and limestone for in-bed desulphurisation. Their preliminary results indicated that in-bed desulphurisation could signifi-
cantly reduce corrosion and may permit the use of less expensive alloy (ferritic 12 Cr steels) for the building of cleaning devices and heat exchangers. Corrosion at low H2S levels is being further investigated by EPRI and the EEC Institute for Advanced Material in the Netherlands. 4.4. Comments In fluidised bed processes it is necessary to process coals with a higher ash fusion temperature (AFT) than the operating temperature (N 1000 8C) of the gasifier to avoid ash agglomeration (which causes uneven fluidisation in dry ash, fluidised bed gasifiers). The presence of pyrite (Fe2O3) in coal as well as sodium silicates formed during gasification are believed to be among the factors that can cause agglomeration in fluidised bed systems. Very careful control of the gasifier operating temperature is therefore required when processing coals with high alkali content. The use of coals with a low swelling index (low caking coals) are preferred to avoid bed agglomeration. Fluidised bed gasifiers are more tolerant to coals with high sulphur content as sulphur can be partly retained in the bed (up to 90%) by the use of sorbents.
5. Moving bed gasifiers Moving bed gasifiers are only suitable for solid fuels with a particle size in the range of 580 mm. A mixture of steam and oxygen is introduced at the bottom of the reactor and runs counter-flow to the coal. Coal residence times in moving bed gasifiers are of the order of 15 to 60 min for high pressure steam/oxygen gasifiers and can be several hours for atmospheric steam/air gasifiers. The pressure in the bed is typically of the order of 3 MPa for commercial gasifiers with tests realised at up to 10 MPa. Coal enters the top of the gasifier and it is sequentially preheated, dried, devolatilised/pyrolysed, gasified and combusted while moving towards the bottom of the gasifier. Moisture is first driven off in the drying zone then the coal is further heated and devolatilised by the hotter product gas while moving down to the gasification zone where it is gasified by reacting with steam and carbon dioxide. The remaining char is finally completely burnt in the combus-
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tion zone where the bed reaches its highest temperature. Maximum temperatures in the combustion zone are typically in the range of 15001800 8C for slagging gasifiers and 1300 8C for dry ash gasifiers. As the flow is counter-current, the gas leaving the gasifier is cooled against the incoming feed and typical gas exit temperatures are of the order of 400500 8C. Ash is removed either as a dry ash or as a slag, depending on the gasifier type. Although moving bed gasifiers are presently less used than entrained flow gasifiers for the construction of new power plants, these moving bed gasifiers present the advantage of being a mature technology. Three gasification processes based on moving bed gasifiers are detailed in Tables 9 and 10. 5.1. Bed permeability The main requirements for moving bed gasifiers are efficient heat and mass transfer between solids and gases within the bed. This involves good bed permeability and consequently the control of coal particle size. 5.1.1. Coal particle size Modern mining methods and mechanical cutting of coal as well as wet coal, plugged coal screens and aged/brittle coal, tend to reduce coal particle size to the extent that run of mine coal can contain up to 40 50% fines by weight. Dittus and Johnson (2001) pointed out that a high concentration of fines entering the Lurgi dry ash gasifier with the coal feed will lead to a disruption of the entire plant operation as the operator will have to reduce the gas production by decreasing coal loading at the top of the gasifier. The authors fixed a design limit at a maximum of 5% coal
Table 9 The BHEL moving bed gasifier Feeding mode and operating conditions Crushed coal (540 mm). Operates at 1 MPa Gasifier High jacketed gasifier. Air and steam are fed through a grate, which also enables ash removal.
fines with less than 6 mm in size for the Lurgi dry ash gasifier. A high concentration of fines in coal will lead to unstable operation of the gasifier as it will cause pressure drops in the bed. Pressure drop problems induce the possibility of grate traction loss (due to bed fluidisation), channel burning (leading to unacceptable gas outlet temperatures) and solid elutriation. At Sasol (Van Dyk et al., 2001), pressure drop is estimated by the Ergun equation as a function of bed voidage (e ), viscosity (l ), density (q ), superficial velocity U s and particle size diameter (d p).
2 1:751 eqUs2 =e3 dp P=L 1501 e2 lUs =e3 dp
As it is a particle size distribution rather than a p, where U is uniform particle, d p is replaced by Ud 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 mean diameter of a coal sample with a specific particle size distribution is calculated as follows: dp 1=Ui xi =dp;i where i is the screen number x i the fraction (mass %) on screen id p,i is the diameter (mm) of screen i . According to Van Dyk et al. (2001), experience on p the Lurgi dry ash gasifiers at Sasol has shown that d is a useful parameter to predict which particle size distributions are more likely to result in gasifier instability. They also reported that an inefficient screening due to screen overload causes misplacement of coal fines that can easily reduce the Sauter diameter to unacceptably low values resulting in highly unstable gasifier operation. Lacey et al. (1992) reported a study on coal fines in BGL gasifiers. Their results showed that the BGL
Ash removal system Ash removal through a grate.
Cooling and cleaning modes A gas cooler is used to produce steam for the gasifier. Further gas cooling and tar condensation are done by water quenching. Particulates are removed by Venturi scrubber
Comments The development was stopped due to poor performance of the gas cooler and the gasifier was replaced by a fluidised bed (see Table 3)
A.-G. Collot / International Journal of Coal Geology 65 (2006) 191212 Table 10 Lurgi moving bed gasification processes Technology Feeding mode and operating conditions British Gas Lurgi (BGL) Lumped coal together with a flux is discharged at the top of the gasifier as a sequence of batches. A distributor plate slowly rotates to ensure even distribution of the coal at the top of the bed. For caking coals, the distributor is connected to a stirrer to prevent the bed from agglomerating. Double-walled cylindrical reactor surrounded by a steam jacket. O2 and steam are added towards the bottom of the bed through tuyeres. This results in high internal temperature within the gasifier (2000 8C). SasolLurgi dry bottom gasifier Similar to BGL.
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Gasifier
Ash removal system Cooling and cleaning modes
Comments
Slagging gasifier. Molten ash is tapped off and quenched with water. Tars, high boiling points hydrocarbons and particulates released during the devolatilisation step are removed in a quench vessel and re-injected in the bed near the tuyeres. The gas (450500 8C) is cooled and cleaned by a water quench and scrubbed to remove H2S. It is a slagging gasifier modified from the Lurgi dry ash gasifier.
Gasifier is surrounded by a water jacket that raises steam for use in the gasifier. A high ratio of steam to O2 (55 : 1) is blown up through a grate at the bottom of the gasifier. The combustion zone is at a temperature (1000 8C) just below the AFT. Ash removed by a revolving grate and depressurised in a lock hopper. The gas (300500 C) is water quenched.
More suitable than BGL for use with the more highly reactive coals.
gasifier can accommodate a reasonable quantity of fines (b 6 mm) in the lump feed. The authors performed tests in the BGL gasifier from the Westfield facility (500 t coal/d, 2.3 m diameter) with coal fines at a pressure of 2.5 MPa. Two UK power plant coals, one weakly caking (Kellingley) and the other medium caking (Coventry) and two American coals (Pittsburgh No 8 and Illinois No 6) were tested. When an excess of fines was injected at the top of the gasifier, the free flow of coal and gas within the bed was disturbed leading to unstable gasifier operation. This was characterised by the fluctuation of the outlet temperatures and a product gas with varying compositions. It was however possible to process at standard load, Pittsburgh No 8 coal, a caking coal, with fine contents of up to 30 to 40%, without adversely affecting the stability of the gasifier. Gasification of Illinois No 6 was also found to be satisfactory but the amount of fines that could be tolerated in the coal feed was lower than with Pittsburgh No 8. Other tests with the two coals included the injection of their slurries (30% coal/70% water) through the tuyeres while simultaneously feeding the top of the gasifier with 30% to 40% of their fines. This enabled the processing of
coals with up to 50% fines in the gasifier. Briquetting is also an alternative to be considered for processing coal fines but it is not a cheap process and can introduce a cost penalty to the process. A joint programme, supported by amongst others the UK Department of Energy (now UK DTI) and the EC, tested the performance of the BGL gasifier with oversize coals collected from a screening plant and briquettes made from the fines of British power plant coals (Coventry and Kellingley). Stable operation of the gasifier was achieved at standard load with the two coals (British Gas/Lurgi slagging gasifier, 1993). 5.1.2. Thermal fragmentation High concentrations of fines in the coal feed can also cause carry over of fines to downstream equipment. To estimate the quantity of fines carried over downstream of the gasifier Van Dyk et al. (2001) defined the term dthermal fragmentationT, as the difference between average particle size before and after pyrolysis at a temperature of 700 8C. Thermal fragmentation is largely affected by the moisture in coal but also by a complex interaction with other factors, such as oxidation and weathering (Van Dyk, 1999).
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5.1.3. Caking properties Caking of coal within the gasifier can also cause pressure drop fluctuations and channel burning, resulting again in unstable gasifier operations. In severe cases oxygen break-through can occur, which can cause a safety hazard because of the probability of downstream explosions. Caking of coal particles can be defined as the softening or plasticity property of coal, which causes particles to melt together to form larger particles when heated. In order to process caking coals, a stirrer connected to the coal plate distributor has been added to the BGL gasifier. It ensures that strongly caking coals are completely carbonised and converted to free-flowing solids that pass to the lower gasification bed (Lacey et al., 1992). Sasol has developed an in-house technique to characterise caking propensity of coal processed under gasification conditions existing in their plants. Details of the technique are given by Van Dyk et al. (2001). A solution used at Sasol to avoid caking (Van Dyk et al., 2001), is the blending of high caking coals with low caking ones. Normal blends used for gasification at Secunda have a caking property that can vary within +/ 20% and coal blends used in the Sasolburg plant have no or little caking. 5.1.4. Ash fusion temperature Low ash fusion temperature (AFT) can result in the formation of a large amount of fused ash or clinkers in the ash bed of the dry ash Lurgi gasifiers. Ash clinkering can also cause channel burning, pressure drop problems and unstable gasifier operation in both the slagging and non slagging gasifiers. Ash composition, especially calcium and iron content give an indication of the expected ash fusion temperature (see Section 3.3). A coal rich in Fe or Ca has usually a low ash fusion temperature due to the fluxing properties of the Ca and Fe minerals. The ash fusion temperature gives an indication of the extent of ash agglomeration and clinkering within the gasifier and is used by Sasol to estimate the risk of ash clinkering. The Dakota Gasification Co has experienced the formation of clinkers that filled 20% of the gasifier. The gasifier had to be shutdown and jack hammers used to break up the clinker so it could be removed. Dakota Gasification believe that sodium in the coals they process in their gasifiers, is mainly responsible for ash clinkering and they fixed the limit of sodium content at which clin-
kering can be avoided. Coal blending is also a solution to keep the sodium content constant. 5.2. Slag mobility in the BGL gasifier The most recent published work on slagging properties in gasifiers concerned entrained flow gasifiers. However it has been reported by Patterson and Hurst (1996) that an optimum slag viscosity at tapping temperature should be less than 5 Pa.s in the BGL gasifier in comparison to less than 15 Pa.s in entrained flow gasifiers. The same author also suggested a tapping temperature of 1400 8C which is lower than in most of the major entrained flow gasifiers. That means that more flux may need to be used in order to comply with those limits and as a consequence the total cost of the system might be increased. 5.3. Comments The main requirement of moving bed gasifiers is good bed permeability to avoid pressure drops and channel burning that can lead to unstable gas outlet temperatures and composition as well as risk of a downstream explosion. Depending on the gasifier design and other characteristics of coal, such as caking propensity, the tolerance of the different gasifiers to coal fines varies from 5% in the Lurgi dry ash gasifier to up to 50% fines in the BGL gasifier. As caking causes particles to melt and sinter together to form larger particles when heated, caking coals can be processed in Lurgi dry ash gasifiers only if they are blended with non-caking coals. However, BGL gasifiers are equipped with a stirrer connected to the coal plate distributor to allow the processing of strongly caking coals.
6. Conclusions Hydrogen is currently and mainly used as an intermediate for the synthesis of chemicals and clean fuels. However with the move towards the dhydrogen economyT there is an incentive to use Hydrogen itself as an energy carrier itself. New programmes and research projects, which are particularly dedicated to the production of Hydrogen from coal, are presently underway worldwide. In this paper some coal properties
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that have an influence on gasifier design, operation and performance have been reviewed. All types of coal can be gasified and gasification appears to have a promising future for the production of hydrogen from coal. Gasification plants are also in the best position, compared to other coal-based alternatives, to capture CO2. The main technical challenge presently faced in the production of hydrogen from coal is the separation of hydrogen from the syngas and the capture and sequestration of CO2.
Acknowledgements The author would like to thank Dr Geoffrey Morrison, head of publication at the IEA Clean Coal Centre for his help in preparing the manuscript.
References
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Matching gasification technologies to coal properties

A.-G. Collot / International Journal of Coal Geology 65 (2006) 191212

A.-G. Collot / International Journal of Coal Geology 65 (2006) 191212

A.-G. Collot / International Journal of Coal Geology 65 (2006) 191212

Mitsubishi heavy industries

Four burners at the bottom

Shell coal gasification process

Operation at 24 MPa, at 1500 8C and above

A.-G. Collot / International Journal of Coal Geology 65 (2006) 191212

Pressure vessel with refractory lining.

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A.-G. Collot / International Journal of Coal Geology 65 (2006) 191212

A.-G. Collot / International Journal of Coal Geology 65 (2006) 191212

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A.-G. Collot / International Journal of Coal Geology 65 (2006) 191212

A.-G. Collot / International Journal of Coal Geology 65 (2006) 191212

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A.-G. Collot / International Journal of Coal Geology 65 (2006) 191212

Ash removal system Ash removal through a grate.

Ash removal system Cooling and cleaning modes

A.-G. Collot / International Journal of Coal Geology 65 (2006) 191212

A.-G. Collot / International Journal of Coal Geology 65 (2006) 191212

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