xvEPA United States Environmental Protection Agency Industrial Environmental Research Laboratory Research Triangle Park NC 2771 1 EPA-600,'7-79-019 January 1979 Alternatives for High-temperature/ High-pressure Participate Control Interagency Energy/Environment R&D Program Report ------- RESEARCH REPORTING SERIES Research reports of the Office of Research and Development, U.S. Environmental Protection Agency, have been grouped into nine series. These nine broad cate- gories were established to facilitate further development and application of en- vironmental technology. Elimination of traditional grouping was consciously planned to foster technology transfer and a maximum interface in related fields. The nine series are: 1. Environmental Health Effects Research 2. Environmental Protection Technology 3. Ecological Research 4. Environmental Monitoring 5. Socioeconomic Environmental Studies 6. Scientific and Technical Assessment Reports (STAR) 7 Interagency Energy-Environment Research and Development 8. "Special" Reports 9. Miscellaneous Reports This report has been assigned to the INTERAGENCY ENERGY-ENVIRONMENT RESEARCH AND DEVELOPMENT series. Reports in this series result from the effort funded under the 17-agency Federal Energy/Environment Research and Development Program. These studies relate to EPA's mission to protect the public health and welfare from adverse effects of pollutants associated with energy sys- tems. The goal of the Program is to assure the rapid development of domestic energy supplies in an environmentally-compatible manner by providing the nec- essary environmental data and control technology. Investigations include analy- ses of the transport of energy-related pollutants and their health and ecological effects; assessments of, and development of, control technologies for energy systems; and integrated assessments of a wide range of energy-related environ- mental issues. EPA REVIEW NOTICE This report has been reviewed by the participating Federal Agencies, and approved for publication Approval does not signify that the contents necessarily reflect the views and policies of the Government, nor does mention of trade names or commercial products constitute endorsement or recommendation for use. This document is available to the public through the National Technical Informa- tion Service, Springfield, Virginia 22161. ------- EPA-600/7-79-019 January 1979 Alternatives for High-temperature/ High-pressure Participate Control by Richard Parker and Seymour Calvert Air Pollution Technology, Inc. 4901 Morena Boulevard, Suite 402 San Diego, California 92117 Contract No. 68-02-2190 Program Element No. 1NE624 EPA Project Officer: Dennis C. Drehmel Industrial Environmental Research Laboratory Office of Energy, Minerals, and Industry Research Triangle Park, NC 27711 Prepared for U.S. ENVIRONMENTAL PROTECTION AGENCY Office of Research and Development Washington, DC 20460 ------- ABSTRACT High temperature and pressure (HTP) particulate control offers efficiency and potential economic advantages over cold gas cleanup in pressurized fluidized bed combustion (PFBC) and low-BTU coal gasification (LBCG) combined-cycle power generation systems. However, considerably more development will be neces- sary in order to demonstrate the technical and economic feasi- bility of HTP gas cleanup on a commercial scale. This report presents the status of the most promising HTP particulate control devices currently being developed. Avail- able data are presented and anticipated performance and develop- ment problems are discussed. The alternative of recuperative heat exchange coupled with low temperature, high pressure particulate control is reviewed with regard to power system efficiencies for PFBC and LBCG com- bined-cycle processes. Successful hot gas cleanup has clear thermal efficiency advantages (1% to 7%) over cold gas cleanup. The economics of hot gas cleanup, however, are very speculative at the current state of development. The relative cost of HTP, pre-turbine particulate control using cyclones, multiclones, and granular bed filters is compared with low temperature and pressure (LTP) post-turbine control using conventional electrostatic precipitators. HTP control equipment costs are estimated to be significantly higher than LTP equipment costs. However, LTP costs are significant and should not be neglected when considering the feasibility of hot gas cleanup for turbine protection followed by post-turbine fine particulate control to meet emissions regulations. 111 ------- TABLE OF CONTENTS Page ABSTRACT iii FIGURES v TABLES Viii ACKNOWLEDGEMENT x SUMMARY AND CONCLUSIONS 1 INTRODUCTION 8 Particulate Removal Requirements 9 Background 11 Pressurized Fluidized Bed Coal Combustion 11 Low-BTU Coal Gasification 16 PARTICULATE CONTROL DEVICES 24 Primary and Secondary Collection 24 Tertiary Collection 29 Cyclones 32 Granular Bed Filters 41 Scrubbers 62 Electrostatic Precipitation 73 Fiber Filtration 78 Membrane Filtration 88 HOT VERSUS COLD GAS CLEANUP 94 Introduction 94 Pressurized Fluidized Bed Coal Combustion 95 PFB Boiler Process 95 Air-Cooled PFBC Process 99 Adiabatic PFBC Process 104 Post-Turbine Particulate Control 107 Low-BTU Coal Gasification Processes 108 REFERENCES • . 120 IV ------- FIGURES Number Page 1 Water-cooled combustor 12 2 Air-cooled combustor 12 3 Adiabatic combustor 12 4 LBCG combined-cycle system 18 5 Three stage hot gas cleanup -25 6 Fractional efficiency for secondary cyclone (from Hoke, et al. 1978) 27 7 HTP particulate control system for Westinghouse PFBC design (from Beecher, et al. 1976) 28 8a Efficiency vs. temperature for high temperature cyclone (from Parent, 1946) 33 8b Efficiency vs. pressure drop for high temperature cyclone (from Parent, 1946) 33 9 Rotary flow cyclone 36 10 Performance of rotary flow cyclone (from Ciliberti and Lancaster, 1976) 36 11 Cyclocentrifuge (from McCabe, 1977) 38 12 Comparison between estimated performance of cyclo- centrifuge and conventional cyclone (from McCabe, 1977) 40 13 Cold flow granular bed filter parameters 42 14a Fractional collection efficiency, nominal configura- tion, 45 14b Influence of operational parameter combinations on frac- tional efficiency (16" filter, 2 mm collector gran- ules 45 v ------- FIGURES, continued Number Page 14c Fractional efficiency performance, small media configuration. . 46 15a Influence of pressure drop function on overall collection efficiency, nominal configuration .... 46 15b Influence of pressure drop function on overall collection efficiency, thick bed configuration ... 47 15c Influence of pressure drop function on overall collection efficiency, small media 47 16 Rexnord gravel bed filter 50 17 Experimental grade efficiency curve of a Rexnord gravel bed filter (McCain, 1976) 52 18 Ducon granular bed filter 53 19 Fractional penetration curve for Ducon granular bed (from Kalen and Zenz, 1973) 54 20a Schematic of a single Exxon filter bed 55 20b Modified filter bed 55 21 Fractional efficiency data for Ducon GBF (from Bertrand, et al. , 1977) 59 22 Predicted GBF performance 61 23 Schematic diagram of A.P.T. dry scrubber system. . . 63 24 Predicted performance for A.P.T. dry scrubber. ... 65 25 Comparison of experimental with theoretical particle collection characteristics of the A.P.T. dry scrubber 67 26 Comparison of particle collection characteristics of the A.P.T. dry scrubber with the A.P.T. cut/power relationship 68 27 Viscosity/temperature relationship determined by NBS on synthetic slags formulated to represent the average compositions of fly ash from Montana Rosebud and Illinois no. 6 coal types 72 VI ------- FIGURES, continued Number Page 28 Predicted performance for ceramic fiber filter. . . 82 29 3M crossflow ceramic monolith 89 30 Pore size distribution for Thermacomb ceramic fiber material (from Poe, et al., 1977) 90 31a Pressurized fluidized bed/combined cycle system water cooled combustor with hot gas cleanup .... 97 31b Pressurized fluidized bed/combined cycle system water cooled combustor with cold gas cleanup. ... 98 32a Curtiss-Wright pressurized fluidized bed/combined cycle system hot gas cleanup with aerodyne cyclones 102 32b Curtiss-Wright pressurized fluidized bed/combined cycle system cold gas cleanup system with heat recovery 103 33a Pressurized fluidized bed combustion system with dual admission steam turbine 105 33b Pressurized fluidized bed combustion system with dual admission steam turbine, cold gas cleanup - low pressure evaporator added for heat recovery . . 106 34a Lurgi air blow gasifier - cold purification case. . 112 34b Lurgi air blown gasifier study - hot purification case 113 35a Air blown entrained bed gasifier study - cold purification case 114 35b Air blown entrained bed gasifier study - hot purification case 115 36a Slagging gasification study - cold purification case 116 36b Slagging gasification study - hot purification case 117 VII ------- TABLES Number Page 1 Summary of FBC Particulate Emissions Characteristics 15 2 Gas Analysis from Exxon Miniplant PFBC Unit 17 3 Summary of Particulate Emissions Data for Coal Gasification Processes 20 4 Estimated Gas Cleaning Equipment Performance (Beecher, et al. , 1976) 30 5 Estimated Temperature and Pressure Losses for Gas Cleanup System (Beecher, et al. 1976) 30 6 Estimated Gas Cleanup Equipment Costs Per Gas Turbine (from Beecher, et al., 1976) 31 7 Fractional Efficiencies for Multiclone at 538°C (from Yellott and Broadley, 1955) 34 8 Estimated Performance of Aerodyne Cyclone (from Klett, et al., 1977) 37 9 Test Parameters for CPC Moving Bed Filter (from Wade, et al. , 1978) 43 10 Granular Bed Filter Performance (from Bertrand, et al., 1977) 58 11 Salt Composition Used in PDU Demonstration Runs. . . 70 12 Particle Behavior: Molten Salt Pilot Plant Run Number 3 70 13 Particle Behavior: Molten Salt Pilot Plant Run Number 6 71 14 Test Data Summmary for ESP at 900°C, 4.4 atm (from Brown and Walker, 1971) 74 15 Recommended Design Parameters for HTP ESP (from Feldman, et al. , 1977) 76 Vlll ------- TABLES, continued Number Page 16 Effect of Temperature on Filtration Efficiency (from First, et al., 1955) 80 17 Fractional Efficiency for Composite Filter Tests. . 80 18 Ceramic Fiber Test Data 84 19 Summary of Hot Tests with 3M Thermacomb 92 20 System Parameters for PFBC Analysis (from Klett, et al., 1977) 96 21 Effectiveness Ranges for Recuperative Heat Exchangers 100 22 Performance of PFBC Processes with Hot and Cold Gas Cleanup (from Klett, et al., 1977) 101 23 Comparison Between Pre-turbine and Post-turbine Equipment Costs 109 24 Summary of Estimated Thermal Efficiencies for Hot Versus Cold Gas Cleanup in Coal Gasification Pro- cesses (from Jones and Donohue, 1977) HI IX ------- ACKNOWLEDGEMENT A.P.T., Inc. wishes to express its appreciation to Dr. Dennis Drehmel, EPA Project Officer, for excellent technical coordination and assistance in support of all our efforts under this contract. ------- SUMMARY AND CONCLUSIONS INTRODUCTION High temperature and pressure (HTP) particulate control offers system efficiency and potential economic advantages over cold gas cleanup in pressurized fluidized bed combustion (PFBC) and low-BTU coal gasification (LBCG) combined-cycle power genera- tion systems. However, considerably more development will be necessary in order to demonstrate the technical and economic feasibility of HTP gas cleanup on a commercial scale. Although HTP particulate control has been a recognized technical problem for over thirty years, no satisfactory solu- tions have been demonstrated. Renewed efforts have been directed at this problem during the past few years with the hope of develop- ing new concepts and equipment for HTP particulate control. This report presents the status of the most promising devices currently being developed. Available data are reported and anti- cipated performance and problems are discussed. Alternative approaches using recuperative heat exchangers coupled with cold gas cleanup are reviewed with regard to their effect on power system efficiencies for PFBC and LBCG combined- cycle processes. The relative costs of HTP gas cleanup for tur- bine protection are compared with the cost of post-turbine clean- up for emissions control. PRIMARY AND SECONDARY COLLECTION Most proposed HTP particulate control systems use one or two stages of cyclones for primary and secondary particulate removal. The primary cyclone recycles unreacted carbon to the combustor or gasifier. The secondary cyclone reduces the mass loading and size of particulates which pass through to the final collection stage- ------- Secondary cyclones may be multiclones, rotary flow cyclones, or other high efficiency cyclone designs. Cyclones may be subject to plugging if condensed tars are present. Primary and secondary cyclones are designed to collect particles with diameters larger than 10 to 20 ym. They generally are not effective for particles smaller than about 5 ym. Primary and secondary particle collection equipment are commercially available although HTP applications are scarce and there is room for improved materials, designs, and engineering models. TERTIARY COLLECTION The third stage (tertiary) collection device must be capa- ble of reducing the particle size and mass loading to a level which is compatible with gas turbine specifications and environ- mental emissions regulations. This most likely will require 90 to 99% collection efficiency on a particle size distribution with a mass median diameter of about 4 ym and a geometric stan- dard deviation of 3 (based on data from the Exxon PFBC miniplant). Cyclones Conventional cyclones have been tested at high temperature and pressure and generally have been found to be inadequate for tertiary cleanup requirements. High efficiency rotary flow cyclones have been proposed for the tertiary collection stage. To date, experimental data have not demonstrated that adequate collection efficiencies can be maintained with rotary flow cyclones. More high temperature and pressure tests are being planned. The "cyclocentrifuge" is a device under preliminary develop- ment which uses a high reaction turbine to drive a centrifuge which serves as the exit tube in a cyclone. High collection effi- ciencies for fine particles have been predicted but experimental data are not available yet to validate the predictions. Opera- tion of the centrifuge bearings at high temperature and pressure in a dirty environment is likely to present the most difficult development problem with this device. 2 ------- Granular Bed Filters Granular bed filters (GBFs) are often proposed as tertiary cleanup devices. A granular bed filter is defined as any filtra- tion system comprised of a stationary or slowly moving bed of discrete, relatively closely packed granules as the filtration medium. Some laboratory data are available which show that very high collection efficiencies (99+%) can be achieved if a filter cake is allowed to form on the surface of the granular bed. Large scale pilot plant and industrial GBF' s have not been able to establish or maintain a filter cake and much lower efficiencies have resulted. Extensive HTP tests on a fixed bed, pilot plant GBF were conducted at the Exxon PFBC miniplant. Efficiencies as high as 97% were achieved but could not be maintained for more than a couple of hours operation. In all runs in which more than one outlet concentration was measured, the efficiency was found to decrease with time. Further HTP tests are planned on a smaller scale GBF. If this GBF can be modified to meet emissions requirements over a prolonged run additional full scale tests will be conducted. High temperature tests on a moving bed GBF (Combustion Power Company) are being conducted. Cold tests demonstrated that fine, submicron particles could be collected with greater than 90% efficiency using the proper velocities, dust loadings, and granule flow rates. No high temperature data are available. The intermittently moving panel bed filter being developed at CCNY (Squires design) has obtained high collection efficiency (99+%) by establishing a filter cake. The major problem with this design is the requirement for low gas capacity and thus relatively large capital costs for a HTP installation. There are not many HTP data available for this device. Establishment of a good cake and high collection efficiency may be more difficult at high temperatures. At this time, GBF's must be considered to be in a highly developmental stage. Design improvements and more data ------- at HTP operating conditions are required before their feasibility as tertiary collectors can be adequately evaluated. Scrubbers Conventional wet scrubbers are not generally suitable for high temperature gas cleaning because they necessarily cool the gas. However, dry scrubbers and molten salt scrubbers are being developed as alternatives for HTP particulate control. The A.P.T. dry scrubber (PxP) system uses large collector parti- cles as collection centers for the fine dust particles. In the configuration presently being developed, the solid collectors are fed into a high velocity throat and contacted with the dust par- ticles. The collectors are removed from the gas in an inertial separation device. Low temperature and pressure data have been obtained which show that the primary collection efficiency (>90% at 1.0 ymA) is as would be expected from theoretical predictions for SL venturi scrubber. A high temperature pilot demonstration of the PxP system is currently underway. The feasibility of electrostatic augmen- tation for improving the collection efficiency, lowering the pres- sure drop, and increasing particle-collector adhesion is being investigated. Molten salt scrubbing is being investigated for simultaneous particulate and H2 S control. Pilot plant data indicate that the mass loading of particles leaving the molten salt venturi scrub- ber may be close to the anticipated environmental emissions standards. Tests will be conducted on a full-scale demonstration plant. No data are available yet. Electrostatic Precipitation The operation of an electrostatic precipitator at high pressures and temperatures has been demonstrated. Stable corona can be maintained at higher electric field strengths than in con- ventional precipitators. There are few studies providing data on fine particle collection at high temperature and pressure. Future development problems will involve electrode rapping and alignment, reentrainment, and materials problems associated with HTP designs. 4 ------- Practical HTP electrostatic precipitation will be limited by thermal ionization at temperatures above 1,100 to 1,300°C. Also a positive barrier-type backup device may be required to prevent catastrophic turbine damage during possible electri cal outages. Fiber Filtration High temperature filtration using metal or ceramic fiber filters is being investigated. In practice it is expected that the effect of temperature and pressure on filtration mechanisms will not be a limiting factor in the overall collection efficiency, The main problems will be the physical and chemical effects of a high temperature environment on the filter materials. These effects may appear as reduced mechanical strength and resilience or loss of adhesion, leading to mechanical leakage and decrease in efficiency. Recent studies with ceramic fabric bags have shown that some have good properties for high temperature and pressure applica- tions. More data are required to adequately establish the useful bag life and other important design parameters. Blanket or felted ceramic materials look most promising because they combine good filtration properties with relatively high strength. How- ever, superficial gas velocities (air-to-cloth ratios) are low in comparison with granular bed filters and the large volume required for fabric filtration may present some economic limitations. Membrane Filtration Laboratory tests on ceramic membrane and honeycomb filtra- tion materials have been conducted. The honeycomb materials were able to obtain high collection efficiencies (averaging 96+%) on fine limestone particles at temperatures up to 815°C. More work is needed to determine optimum configurations for filtration and for cleaning. Also the durability and erosivity limitations need to be determined. The major advantage of these filtration media is that they have very high surface to volume ratios. Superfical velocities are similar to those for fabric filters. ------- HOT VERSUS COLD GAS CLEANUP Pressurized Fluidized Bed Combustion The relative advantages of hot versus cold gas cleanup are different for the three PFBC processes currently under development. These are: the water-cooled PFBC boiler, the air-cooled PFBC process, and the adiabatic PFBC process. The efficiency loss between hot and cold gas cleanup is greatest for the adiabatic combustor configuration because all the working fluid passes through the bed and must be cleaned. The air-cooled and water-cooled combustors appear to be capable of using cold gas cleanup techniques with fairly small (about 1 to 2% system efficiency) performance penalties. The Phase II EGAS studies showed the PFBC boiler process with hot gas cleanup to have a 1% advantage over conventional coal-fired boilers using flue gas scrubbing for SO control. 3C In order to fully assess the cold cleanup alternatives, re- cuperative heat exchangers must be studied more closely, especi- ally regarding their effectiveness, availability, and cost for high temperature and pressure applications. Post-Turbine Particulate Control If gas turbines which have relatively high tolerance for fine particles can be developed, then it may be feasible to use currently available hot gas cleanup devices (cyclones, multiclones) to protect the gas turbine. In such cases the emissions regula- tions would have to be met by applying conventional particulate control equipment downstream from the gas turbine. The cost of post-turbine particulate control equipment is noticeably less (about 10 to 30?0 than the cost of hot gas cleanup as estimated in the EGAS Phase II design studies. How- ever the post-turbine equipment costs are significant and must be considered in the overall capital cost for gas cleaning equipment when considering the feasibility of pre-turbine/post- turbine control systems. ------- Low-BTU Coal Gasification Gas cleanup in LBCG processes must consider acid gas removal (principally H2S and COS), tar removal, removal of alkali metal vapors and compounds, and fine particle removal. There is little incentive for hot particulate removal if the gas must be cooled and scrubbed to remove H2S. The presence of tars in LBCG processes presents serious problems.' They will contaminate or plug subsequent H2S and particulate removal systems unless they can be kept in the vapor phase. They may be removed in a quench scrubber before H2S and particulate removal, however, this wastes approximately 20% of the available energy through sensible heat loss, and as much as 20% of the available chemical energy in the fuel gas. Hot H2S and particulate control would save these energy losses and enable the tars to be burnt in the gas turbine combustor. For all LBCG gasifiers where tar removal is not a problem, thermal efficiency advantages associated with hot gas cleanup (H2S and fine particulate matter) appear to be marginal (1 to 2%). The Phase II EGAS studies showed LBCG combined-cycle processes with cold gas cleanup to have a 7% advantage over a conventional coal-fired boiler using flue gas scrubbing for SOX control. ------- INTRODUCTION The economic attraction of many advanced energy processes depends on the development of technology for cleaning gases at high temperatures and pressures. Two processes requiring high temperature and pressure gas cleanup are: 1) pressurized fluidized bed coal combustion, and 2) the combined open-cycle gas turbine- steam turbine system integrated with a low-BTU coal gasifier. These processes are among those recommended for further develop- ment by the Energy Conversion Alternatives Study (Lewis Research Center, 1976 and 1977). Both of these processes require expension of the gas through a gas turbine at high temperature and pressure. The gas must be cleaned to remove corrosive gases, condensible vapors and particu- late matter which could potentially damage the gas turbine. Any temperature and pressure losses during gas cleanup will reduce the overall thermodynamic efficiency of the process. Therefore it is desirable to clean the gas at system temperature and pressure. Equipment for removing particulate matter from high tempera- ture (HTP) gas streams has been under development to various de- grees for over thirty years. Recently there has been renewed interest in this problem and a number of new concepts and improved materials are now being investigated. In this report we review the present state-of-the art for HTP particulate collection and discuss the process requirements and possible alternative approaches to hot gas cleanup. In many situations, the requirement for hot particulate removal is coupled with a need for removing acid gas, and/or alkali metal vapor at high temperature and pressure. Therefore, systems which poten- tially can remove particulates, gases, tars and condensible vapors will be especially attractive. It has been assumed that readers are basically familiar with conventional particulate control technology. Details on conventional control equipment are presented by Calvert, et al. (1972), Billings and Wilder (1970) and Stern (1977). 8 ------- PARTICULATE REMOVAL REQUIREMENTS The degree to which particles must be removed from low-BTU coal gasification (LBCG) and pressurized fluidized bed combustion (PFBC) processes depends on the gas turbine tolerances for particu- late matter, the size distribution and mass loading of particulate matter, the gas composition, turbine blade material, gas tempera- ture, other process parameters and environmental regulations. There are no current New Source Performance Standards (NSPS) for advanced fossil-fuel conversion processes. In order to allow for industry growth while maintaining regional air quality stan- dards, it would be necessary to control particulate emissions from new sources more stringently than current standards. The NSPS for particulate emissions from advanced fossil fuel conver- sion processes will most likely be as stringent as the anti- cipated new standards for boilers. That is, <0.05 lb/106 BTU (21.5 mg/MJ), or at least be based on BACT (best available con- trol technology). The gas turbine specifications also impose a gas cleanup requirement. The useful life of a gas turbine depends on the extent of erosion and corrosion damage to the internal components of the turbine. The extent of damage depends upon the concentra- tion and size of particulate matter entrained in the gas, upon the chemical composition of the gas and particles, and upon' the gas temperature, turbine design and other operating para- meters . Erosion damage results from the inertial bombardment of particles onto the stator and rotor blades of the gas turbine. The erosion damage is proportional to the kinetic energy of the particulate matter striking the turbine blades. Therefore the damage is more severe when larger more massive particles are pre- sent in the gas stream. Large concentrations of very small particles may be even less harmful than their total mass would imply because their trajectories would tend to follow the gas streamlines and thus would be less likely to strike the turbine blades. ------- Corrosion damage depends on the amount of particulate matter that adheres to the turbine surfaces as well as the chemical com- position of the gas and particles. In general, the most corrosive compounds are those containing sodium and potassium. Liquid deposits of such compounds can form inside the turbine at tem- peratures between about 500°C and 1,000°C. These molten films attack the protective oxide scale on the blade material, and thus initiate accelerated oxidation of the turbine components. The buildup of particulate deposits on the turbine blades also can significantly impair the aerodynamic performance of the blades. Furthermore, large agglomerates can break off from such deposits and cause additional erosion damage. There is much debate regarding the definition of acceptable particle concentrations for gas turbines. There is general agreement that large particles must be removed from the gas. Robson (1976) recommends a maximum allowable concentration of 2.7 mg/Nm3 (0.0012 gr/SCF) for particles larger than 2 ym in diameter. There is less agreement on the allowable turbine tolerance for fine particles. A Westinghouse study (Westinghouse, 1974) proposed that a concentration of 340 mg/Nm3 (0.15 gr/SCF) of particles smaller than 2 ym could be tolerated. Sverdrup and Archer (1977) recommended that the concentration be maintained below 4.6 mg/Nm3 (0.002 gr/SCF) for all particle sizes with no particles larger than 6 ym. The variation in turbine tolerance estimates is not sur- prising considering the scarcity of direct experience with large coal-fired industrial gas turbines, the difficulty of extrapola- ting data from small turbines, the variations in existing and proposed turbine materials and blade temperatures, and variations and uncertainties in the chemical and physical properties of the particles and gases. These uncertainties pose a major problem to engineers throughout this report we have used the convention of "ym" for physical diameter and "ymA" for aerodynamic diameter. Particle densities are given whenever they are known. 10 ------- involved in the development and evaluation of advanced energy processes. Developers of hot gas cleanup devices do not know how efficient their equipment must be at removing fine particles, At the same time, estimates of the cost of electricity and capi- tal investment for advanced energy processes are strongly depen- dent on assumptions concerning the cost (and indirectly the effi- ciency) of gas cleanup equipment. This predicament results in part from the necessity for parallel development of advanced industrial scale gas turbines and high temperature and pressure gas cleanup technology. The cost of HTP gas cleanup will vary inversely with the allowable particle concentration entering the gas turbine. However, the process emissions must satisfy all environmental regulations. Gas turbines which can tolerate relatively large concen- trations of fine particles may necessitate particulate control equipment downstream from the gas turbine. The cost of this control equipment must be considered in the overall economic evaluation of the process. If expensive control equipment is required to protect the turbine, economics may require that this equipment satisfy the emissions regulations as well. BACKGROUND Pressurized Fluidized Bed Coal Combustion The combustion of coal in a fluidized bed of limestone or dolomite offers many advantages over conventional coal-fired boilers. The primary advantage is the ability to burn high sul- fur coals without requiring flue gas desulfurization equipment. Also PFBC processes have the potential for lower introgen oxide emissions, higher thermodynamic efficiencies, more efficient fuel utilization, lower cost of electricity and lower capital costs compared with conventional coal-fired power plants using stack gas scrubbers for SO control. J\. There are three approaches currently being considered for PFBC processes. The first is the PFBC boiler illustrated in Figure 1. Combustion takes place at a pressure of 10 atm and a temperature around 900°C. The combustion temperature is 11 ------- AIR COMPRESSOR STACK ADDITIVE COAL ASH DISPOSAL Figure 1. Water-cooled combustor. STACK STEAM TURBINE | CONDENSER FEED WATER AIR STACK STEAM TURBINE t BOILER FEED WATER AIR WASTE HEAT BOILER GAS TURBINE PARTICULATE REMOVAL ADDITIVE COAL ASH DISPOSAL Figure 2. Air-cooled combustor. ADDITIVE COAL U^ COMPRESSOR ~i I w Si 0 u t=J \ 1 GAS TURBINE PARTICULATE REMOVAL ASH DISPOSAL Figure 3. Adiabatic combustor. 12 ------- maintained using water-cooled heat exchanger tubes. The steam generated is used to drive a steam turbine. The products of combustion leave the combustor at high temperature and pressure, and pass through the HTP gas cleanup system before being expan- ded through the gas turbine. Beecher, et al. (1976) reported the conceptual design of an advanced steam plant using a PFBC boiler. The plant gener- ates a net electric power of 679 MW. Four PFBC boiler modules are used to fire two gas turbine generators. The turbine inlet temperature is 959°C. Each turbine handles a gas flow of 345 kg/s (760 Ib/s). Each boiler has two stages of cyclones for dust re- moval. The first stage removes large particles and conveys them to the carbon burnup cell. The second stage is a multiclone de- vice which removes coarse and fine particles and thereby reduces the loading to the tertiary (third stage) cleanup devices. Four granular bed filters (43 kg/s or 95 Ib/s each) are proposed for tertiary cleanup for each boiler. The overall cost of electricity will be affected by the capital cost and operating cost of the particulate control equip- ment. The capital cost is a function of the size and number of units required, which depend primarily on the total volumetric gas flow to be treated at high temperature and pressure. The operating cost depends on the power requirement of the control equipment and the temperature and pressure losses which occur. In the PFBC boiler system, approximately 80% of the total elec- tricity is generated in the steam turbine cycle. Only 20% is generated downstream of the hot gas cleanup system in the gas turbine cycle. An air-cooled PFBC process is being developed by Curtiss- Wright Corporation under D.O.E. sponsorship. A schematic dia- gram of this process is shown in Figure 2. The FBC unit is cooled by passing approximately two-thirds of the compressed air through heat exchanger tubing in the combustor. The other third of the compressed air is used for combustion. 13 ------- The effluent gas from the combustor is cleaned before it is mixed with the hot gas from the heat exchanger tubes. The mixed gas is then expanded through the gas turbine and passed through a waste heat boiler. The principal advantage of this process is that it dilutes the gases leaving the cleanup equipment thereby reducing the mass loading entering the gas turbine. The total flow to the gas turbine is increased threefold. For equivalent size plants, the combustion gas flow will be approximately the same as that re- quired with the PFBC boiler. Depending on the heat loss during cleanup and the efficiency of heat transfer, the mixed gas may attain a higher or lower temperature than the effluent gas temperature from the PFBC boiler. All electricity is generated downstream from the control equipment. The third type of PFBC process currently being developed uses the adiabatic fluidized bed combustor. This process has been developed by the Combustion Power Company for refuse combustion and also is being investigated for its potential in burning coal. The adiabatic system is illustrated in Figure 3. The bed temperature is maintained suitably low by using large volumes of excess air (300%J. Thus the gas flow rate is approximately the same as the total flow used in the air-cooled PFBC process. In the adiabatic combustor system, all the gas passes directly through the combustor and must be cleaned. Therefore the size (and capital cost) of the cleanup equipment will be significantly more than in the other designs. Furthermore, all the power generation occurs downstream from the cleanup equip- ment and therefore the cost of electricity will be especially sensitive to temperature and pressure losses during cleanup. The particulate emissions and high temperature and pressure cleanup requirements for fluidized bed combustion processes has been reviewed by Parker and Calvert (1977). Particulate emis- sions data from their survey are presented in Table 1. 14 ------- TABLE 1. SUMMARY OF FBC PARTICULATE EMISSION CHARACTERISTICS Temperature, °C Pressure, atm Mass loading, g/Nm3 Mass loading, gr/SCF Mass median diameter, ym Geometric standard deviation Exxon Miniplant* 820-950 5-10 1.8-2.8 0.8-1.8 4-8 2.7 Argonne Natl. Labs 790-900 to 8 0.5-4.8 0.2-2.1 Combustion Power Cot* 760-980 3-7 0.09 0.04 1.2 1.9 National Coal Board (G.B.) 750-950 1-5 3.0 1.4 Pope, Evans § Robbins** 300-400 1 0.2-1.7 0.5-4 4.6 2 * Particle density estimated to be 1.5 g/cm3 *** Waste-fired combustor ------- The particulate removal requirements for pressurized fluidized bed combustion processes will depend on the turbine tolerances for fine particles and the emissions regulations for coal-fired boilers. An emission of 0.05 lb/106 BTU corresponds to a particu- late loading of approximately 57 mg/DNm3 (0.025 gr/SCF) based on the heat input of the coal and emissions data from the Exxon PFBC miniplant (Hoke, et al., 1978). The emissions regulations will be approximately the same for all three PFBC designs. Particulate control to protect the gas turbine is coupled with the problem of alkali metal vapor removal. HTP control equipment for PFBC processes may need to remove alkali metal vapors as well as fine particles. Recent data taken at the Exxon miniplant (Bertrand, et al. 1978) indicated that 2 ppm sodium vapor, 0.05 ppm potassium vapor were present in the effluent gas. Gas analyses for the same run showed very low H2S and hydrocarbon concentrations and 285 ppm S02. These data are listed in Table 2. Low-BTU Coal Gasification Low-BTU coal gasification processes are under development as a possible means of obtaining electrical energy from coal while satisfying all environmental regulations. Preliminary economic analyses (Lewis Research Center, 1976 and 1977) in- dicate that a combined cycle gas turbine-steam power generation cycle fired by gas from an integrated low-BTU coal gasifier offers significant economic advantages over conventional coal- fired boilers in terms of more efficient coal usage and lower cost of electricity. A typical process flow diagram is shown in Figure 4. The basic gasification process converts solid coal into a combustible gaseous fuel by reacting it with air and steam. The product gas contains hydrogen, carbon monoxide, carbon dioxide, nitrogen, methane and hydrogen sulfide. The product gas leaves the gasifier at high temperature (500 to 1,500°C) 16 ------- TABLE 2. GAS ANALYSIS FROM EXXON MINIPLANT PFBC UNIT COMPONENT CO 2 02 S02 (std.dev.) N0x CO H2S COS CS2 CHi, C2H6 C3 to C6 Na K CONCENTRATION 13.5 I 4.5 % 285 ppm (110 ppm) 50 ppm 600-750 ppm 1 ppm not detectable not detectable 18 ppm 14 ppm not detectable 2 ppm 0 . 5 ppm 17 ------- 00 RECYCLE GAS TO GASIFIER CLEAN LOW GAS PRETREATED LIMESTONE r COMPRESSED AIR CHAR STRIP *_STEAM COMBUSTOR AIR GAS TURBINE -*- ELECTRICITY SULFUR (^BOILER )—>• TO STACK WATER -^AMMONIA DUST STEAM GASIFIER ELECTRICITY ,. STEAM TURBINE SLAG Figure 4. LBCG combined-cycle system. ------- and often at high pressure (10 to 20 atm). The gas usually will contain large concentrations of entrained particulate matter (ash, carbon, and possibly tars). Alkali metal vapors and other contaminants also may be present. There are many different processes for gasifying coal, and the gaseous and particulate emissions can vary widely from one process to another. The most popular classification of gasification processes is classification according to the flow of the gas relative to the coal. The four basic gasifier types classified in this manner are: 1. Fixed or slowly moving beds of solids 2. Entrained solids 3. Fluidized beds 4. Molten baths Gasifiers also may be classified with regard to the ash removal method. At temperatures below approximately 1,000°C the mineral matter in the ash remains dry. At temperatures somewhat higher the ash becomes tacky and tends to agglomerate. At even higher temperatures the ash melts. Molten ash usually becomes free-flowing at temperatures of about 1,500°C to 1,600°C. Therefore coal gasifiers can be classified as dry bottom, ash agglomerating, or slagging gasifiers with regard to ash removal. Gasifiers also can be classified as to pressure level, number of reaction stages, and the source of oxygen (either air blown or oxygen blown). In general, particulate emissions are expected to be greater for entrained bed and fluidized bed dry bottom gasifiers. Par- ticulate emissions should be less for ash agglomerating and molten bath gasifiers. Parker and Calvert (1977) reviewed the available data on particulate emissions from coal gasification processes and their results are summarized in Table 3. Particulate control for coal gasification processes is closely coupled with acid gas removal (principally H2S, COS, and Ca), tar removal, and alkali vapor removal. In some processes there may be a need for NH3 removal also. There is little 19 ------- TABLE 3. SUMMARY OF PARTICULATE EMISSION DATA FOR COAL GASIFICATION PROCESSES Process I Fixed Beds Lurgi USBM Stirred Bed Gasifier Exit Temperature 400-600 500-650 II Dry Fluidized Beds Winkler USMB Synthane COa Acceptor - Gasifier C02 Acceptor - Regenerator 800-1,000 400-750 800-850 1,000 BCR Fluidized Bed 1,000-1,150 III Ash Agglomerating Fluidized Bed Battelle - Union Carbide IGT U-Gas Westinghouse • 1,100 1,000 750-900 Gas Cleanup Temperature °C 200 150-200 250 200 1,000 650 -- 400 Pressure atm 20-30 7 1 10 10 10 20 7 20 10-15 Mass Loading g/Nm3 24 24 -- -- 20 18 -- -- -- gr/SCF 10 10 -- -- 8.8 7.8 -- -- -- Control Devices Used or Anticipated scrubbers scrubbers cyclones, scrubbers, electrostatic precipitators scrubber venturi scrubber cyclones, sand bed filters -- cyclones proprietary process > rotary flow cyclones, granu lar bed filters Remarks tars present tars present tars § heavy hydrocarbons present IX) O ------- TABLE 3. Continued Process IV S lagging-Entrained Flow Koppers-Totzek Combustion Engineering Foster Wheeler BYU Texaco V Molten Bath ATC Molten Iron Atomics Internal ' 1 VI In-Situ LERC Gasifier Exit Temperature °C 1,200-1,300 900 1,000 650-1,300 1,400 1,100 950 — Gas Cleanup Temperature °C 200 150 100 -- 300 -- — 250-350 Pressure atm 1 10 30 1 15 1 5 2-7 Mass Loading g/Nm3 40 _ _ — -- -- — — -- gr/SCF 17.5 -- — — — — — Control Devices Used or Anticipated two disintegra- tor or venturi scrubber in series scrubber scrubber -- -- -- — scrubbers Remarks MMD l,000ym a ~ 15 g bench scale development alkali meta: fumes presei tars presem ------- advantage to hot particulate control unless acid gases and metal vapors also can be controlled at high temperature. Gas cleanup at low temperature (system pressure) is being proposed for most coal gasification processes. There are three basic reasons for this: 1. The energy content of the gas is predominantly chemical energy rather than sensible heat. Sensible heat accounts for approximately 10 to 20% of the total energy content of the gas. 2. High pressure/low temperature gas cleanup equipment is available commercially although it has not necessarily been optimized for coal gasification applications. No hot gas cleanup systems have been demonstrated to be satisfactory and they must be considered as not commercially available. 3. Coal gases which contain tars must be cooled in the tar removal quencher to prevent tars from depositing in downstream system components. If the gas can be kept hot enough it is conceivable that tar condensation can be prevented and tars can be built in the gas turbine combustor. In this case hot gas cleanup would save the sensible heat in the gas and the chemical energy in the tars. Tars can contain as high as 201 of the chemical energy in the gas leaving the gasifier (MERC, 1978). However, most LBCG pro- cesses which emit tars propose a quench to remove the tars. Al- though relying on existing technology, this severely limits the thermal efficiency of the process. Tar removal is a problem with fixed bed and slowly moving bed gasifier designs where the gasifier temperature is too low to crack tars. If the process temperature is high enough to prevent the formation of tars (as in many entrained bed and fluidized bed gasifier designs), it usually is proposed that the gas be cooled in a heat exchanger to provide process steam for the gasifier or superheat steam for the steam turbine cycle of the process. 22 ------- Hot gas cleanup has some advantages over cold gas cleanup for coal gasification processes in terms of the overall thermo- dynamic efficiency. However, the availability and cost of hot gas cleanup systems (particulate removal and acid gas removal) may hinder realization of the higher thermodynamic efficiency in practice. In the next section of this report we review the current developmental status and anticipated problems or limitations of high temperature and pressure particulate control devices. In the final section we review the advantages and disadvantages of hot versus cold gas cleanup for pressurized fluidized bed combustion and low-BTU coal gasification combined-cycle processes 23 ------- PARTICULATE CONTROL DEVICES PRIMARY AND SECONDARY COLLECTION Most proposed high temperature and pressure particulate control systems use three particle collection stages as illus- trated in Figure 5. The first stage usually is a large cyclone which removes coarse particles and recycles them to the combustor or gasifier. The particles removed in the primary cyclone are predominantly unreacted carbon. In the PFBC system these large particles can ignite and cause fires in the primary cyclone. Fires may cause excessive temperatures and corrosion in the cyclone. Very sticky particles may also be present and can eventually cause the cyclone to become plugged. This problem has been encountered in the fluidized bed combustion of refuse although it has not been a serious problem with coal combustion. The PFBC systems use limestone or dolo- mite as bed sorbent material to react with sulfur from the coal. The primary cyclone also will collect and recycle large sorbent particles. In gasification processes where tar removal is required, plugging of the primary cyclone may be a problem. In such situ- ations the primary collection stage is usually a quench tower which cools the gas, and condenses and removes tars and other coarse particles. In processes where tars are not a problem or where hot gas cleanup is viable, primary cyclones may be used. Because of the reducing atmosphere and the presence of hydrogen sulfide, materials requirements will be different than for combustion processes. The purpose of the secondary collection stage is to remove particles larger than approximately 20 ym in diameter. This 24 ------- PRIMARY COLLECTION! COAL FEED. TERTIARY COLLECTION TO GAS TURBINE i Y ASH T ASH SECONDARY COLLECTION GAS Figure 5. Three stage hot gas cleanup 25 ------- reduces the particle size and mass loading to the third stage or tertiary collector. Proposed designs for secondary collectors use various high efficiency cyclones or multiclones. In some cases it may be desirable to eliminate the secondary collector in order to increase the size and loading of particles to the tertiary collector. An example of this might be a ceramic fiber baghouse in which large particles and high dust loadings are required in the formation of a dust cake which is necessary to maintain high collection efficiency. Experimental measurements of the fractional collection effi ciency for the conventional secondary cyclone at the Exxon PFBC miniplant have been reported by Hoke, et al., (1978). Their data are plotted in Figure 6. Beecher, et al. (1976) described the design of a 680 MWe power plant. Four pressurized fluidized bed boilers supplied gas to two gas turbines. Each turbine handled 345 kg/s (760 Ib/s) of gas. Each boiler had four primary cyclones, one secon- dary collector, and four tertiary collectors associated with it. Each cylone handled about 43 kg/s of gas or approximately 850 m3/min (30,000 ft /min) at 966°C (1,770°F) and 10 atm. A flow diagram of the cleanup system is shown in Figure 7. The first stage of particulate removal is a group of four cyclone collectors housed in a pressure vessel. The solids collected by these cyclones consist of dolomite fines, coal ash, and unburnt char. To maximize the combustion efficiency of the system, these solids are fed to a carbon burn-up cell operating at approximately 1,000°C. The combustion products from the burn-up cell mixed with the gases leaving the primary cyclone and pass on to the secondary collector. The primary cyclones are made from Haynes Alloy 188 which is a cobalt-based high temperature, corrosion-resistant super- alloy. The inner surfaces are lined with a hard refractory. Main- tenance of these surfaces is anticipated at approximately 2 year intervals. 26 ------- fO U 2 100 90 80 70 60 tu IX, u 50 u 8 40 30 20 10 0 \ 20 30 40 50 Figure 6. 2 3 4 5678 10 PARTICLE SIZE, ym Fractional efficiency for secondary cyclone (from Hoke, et al., 1978). ------- MULTICLONE CARBON BURNUP CELL RECUPERATOR WATER BOOSTER COMPRESSOR TO WASTE TREATMENT Figure 7. HTP particulate control system for Westinghouse PFBC design. 28 ------- The second stage collector is a multiclone (multiple cy- clone) . Approximately 1% of the gas flow is bled off and used to transport the collected solids. The solids are removed from the bleed stream by a separate cyclone, then are depressurized, and deposited in an ash lock-hopper. The bleed gas is cooled in a recuperator, scrubbed, compressed, reheated and used as the re- verse cleaning gas for the tertiary collectors (granular bed filters) The particulate mass loadings and overall efficiencies for each cleanup stage are listed in Table 4. The estimated temperature and pressure losses are shown in Table 5. The estimated gas cleanup costs per gas turbine are listed in Table 6. Primary and secondary collection equipment are commercially available although high temperature and pressure applications are scarce and there is room for substantial improvements in materials, designs, and engineering models. Also, high tempera- ture and pressure conditions necessitate the use of expensive materials and fabrication techniques. In the design reported by Beecher, et al. (1976), eight primary cyclones served each gas turbine at an average major component cost of $117,250 per cyclone (1975 dollars). Each cyclone handled 850 m'/min (30,000 ACFM) of gas. For comparison we have used the curves presented by Neveril, et al. (1978) to estimate the cost of a conventional cyclone of similar capacity. A 10 gage stainless steel cyclone handling 850 m3/min would cost approximately $23,000 (1975 dollars). If the materials were 10 gage carbon steel the cost would be approximately $11,000. It should be noted that the HTP cyclone handles approximately 2.2 times the mass flow of gas handled by the conventional cyclone in this comparison. TERTIARY COLLECTION The final collection stage must reduce the mass loading of particles to a level compatible with gas-turbine operating specifications and environmental standards. This most likely will require 90 to 99% collection efficiency on a particle 29 ------- TABLE 4. ESTIMATED GAS CLEANING EQUIPMENT PERFORMANCE (BEECHER ET AL., 1976) Stage Primary Cyclone Inlet Loading, Outlet Loading, Efficiency g/g gas g/g gas % 0.0245 0.0005 97.9 Multiclone Granular Bed Filter 0.01521 0.00075 0.00075 0.000014* 95.1 98.1 * Equivalent to 16.9 mg/Nm3 (0.0074 gr/SCF) entering the gas turbine TABLE 5. ESTIMATED TEMPERATURE AND PRESSURE LOSSES FOR GAS CLEANUP SYSTEM (BEECHER, ET AL. 1976) Description Primary Cyclone Multiclone Granular Bed Filters Temperature Drop, °C 2.2 3.1 11.8 Pressure Drop*, % 0.6 2.0 0.6 * % of gas turbine discharge pressure 30 ------- TABLE 6. ESTIMATED GAS CLEANUP EQUIPMENT COSTS PER GAS TURBINE BEECHER ET AL., 1976)* Major Comp. Material Installation Total ' CycLfleparators $ 938>°°° 1,594,064 _. ccn 34'550 27,900 24,900 21'600 2. Multiclones 3. Multiclone Bleed Cyclone 4. Multiclone Bleed Cooler 5. Multiclone Bleed Scrubbers 6. Multiclone Bleed Cooler^ 462>000 $1,400,000 785,136 2,379,200 0 8'650 43>200 4,500 7,500 32,400 32,400 22>600 7. Multiclone Bleed Recuperator 8. Multiclone Bleed Compressor ' ' ' 205,500 10. Granular Bed r 1 -L L- Ci 5 11. Balance of Plant Materials and Installation SUBTOTAL 36,800 2,452,200 3,680 1,207,800 1,066,800 40,480 3,660,000 1,066,800 $ 5,334,214 $ 3,571,566 $ 8,905,780 *Costs are based on mid-1975 dollars. 31 ------- size distribution which is approximately log-normal with a mass median diameter of about 4 ym and a geometric standard deviation of 3. In recent years cyclones and granular bed filters have received the most attention as potential tertiary collection devices. To date, neither device has been demonstrated to be efficient enough to satisfy the emissions regulations or the turbine specifications. It is apparent that the current state of the technology is not sufficient and more reliable and effi- cient cleanup devices are required. Economic studies of the pressurized fluidized bed combus- tion process have generally assumed that granular bed filters in their current state of development will be sufficient, or at least representative of the tertiary collector costs. Recent experience at the Exxon miniplant has indicated that granular bed filters need further development before they can be con- sidered commercially viable for PFBC applications. The economic feasibility of pressurized fluidized bed combustion processes must remain highly speculative until a satisfactory solution to the hot gas cleanup problem has been demonstrated. Cyclones Background The application of cyclone separators for particulate re- moval at high temperature and pressure has been considered for over thirty years. Parent (1946) tested small sampling cyclones (2 and 3 inch diameter) at temperatures up to 1,400°F and pressures to 6.8 atm (100 lb/in2). Dust loadings from 0.34 to 6.86 g/Nm3 (0.15 to 3.0 gr/SCF) were also considered. His results are shown in Figure 8. Figure 8a shows the decrease in overall efficiency as tem- perature increases for a constant pressure drop. Figure 8b in- dicates that an increase in pressure drop from about 10 cm W.C0 to 25 cm W.C. is required to maintain the overall collection efficiency at 951 when the temperature increases from 24°C to 540°C. Parent 's data also indicate that there was no significant effect of mass loading on the efficiency for the parameters studied 32 ------- 100 0\° tu p- o w o u OH 0- PJ z o I— I H u 8 90 • 80 i i i AP = 7.6 cm W.C. 100 200 300 400 TEMPERATURE, °C 500 600 Figure 8a. Efficiency vs. temperature for high temperature cyclone (from Parent, 1946). 100 90 80 i l l l l i i I i i l I I 540°C l I I l I l i i 24 8 10 12 14 16 18 20 22 24 26 PRESSURE DROP, cm W.C. Figure 8b. Efficiency vs. pressure drop for high temperature cyclone (from Parent, 1946) . 33 ------- Yellott and Broadley (1955) studied the efficiency and pressure drop of cyclones operating at high temperatures. They also found that efficiency decreased with increasing temperature, Their study included a 10-inch multiclone for which the frac- tional efficiency is presented in Table 7. These data are for fly ash particles at 1 atm and 538°C (1,000°F). TABLE 7. FRACTIONAL EFFICIENCIES FOR MULTICLONE AT 538°C (FROM YELLOTT AND BROADLEY, 1955) Pressure Drop , kPa 0.75 1.00 1.34 Air Flow, m3/min 21.4 24.1 28.0 Size analysis of dust Particle Size, ym 0-10 50.3% 55.2 60.6 46.3 10-20 91.51 92.0 92.6 17.8 20-44 97.5% 97.5 97.5 15.8 + 44 99.0% 99.0 99.0 20.1 Advanced Cyclone Designs Experience with cyclones and multiclones generally confirms that these devices are not sufficient either for protecting the turbine or for satisfying environmental regulations. Recent data obtained at the Exxon miniplant (Bertrand, et al., 1978) show unusually high collection efficiency for a ter- tiary cyclone of conventional design. Efficiencies in excess of 80% for 1 ym diameter particles were reported. The size dis- tribution of particles entering the cyclone was not measured directly and it may be that particles were agglomerating some- where upstream. These results need to be looked at more care- fully in order to identify the cause of the high efficiencies measured. 34 ------- Rotary flow cyclone - A rotary flow cyclone design by Aerodyne Corporation has the potential for higher collection efficiency than conventional cyclones or multiclones and has been proposed as a possible tertiary cleanup device. This cyclone is illustrated in Figure 9. In the rotary flow cyclone, the primary flow (to be cleaned) enters through a set of vanes located at the base of the unit. A secondary flow is introduced around the circum- ference of the unit at the top through tangential inlet nozzles. The secondary flow is approximately 601 of the primary flow. As particles in the primary flow are forced towards the wall they are swept downward to the collection hopper by the secondary flow. The secondary flow may be either clean or dirty gas. A commercially available Aerodyne rotary flow cyclone, rated at 2.3 m3/min (80 CFM))was tested at Westinghouse Research Laboratories (Ciliberti and Lancaster, 1976). They used a portion (30 CFM) of the dirty gas stream as the secondary flow. Their results are presented in Figure 10. Also shown are their theoretical predictions. Both their theoretical and experimental performance curves showed lower efficiency than the manufacturers performance curves which claim 50% efficiency for approximately 0.5 ym particles. From the Westinghouse data, it seems unlikely that the rotary flow cyclone will be able to collect any particles smaller than about 1 to 2 ym. From particle size data obtained at the Exxon miniplant, approximately 30% of the mass leaving the secondary cyclone is smaller than 2 ym. This corresponds to a mass loading of roughly 0.69 g/Nm3 (0.3 gr/SCF). Westinghouse plans further tests on the Aerodyne cyclone at high temperature and pressure. Although it may not be sufficient as a tertiary collector, it may be a useful alter- native to multiclones as the secondary collection device. 35 ------- CLEAN GAS TANGENTIAL NOZZLES TURNING VANES tu »-H u tL. U. o I-H U U] o u PRIMARY I GAS FLOW I —•" PRIMARY GAS FLOW UPWARD SPIRAL (ROTATIONAL FLOW) SECONDARY GAS FLOW SECONDARY GAS FLOW DOWNWARD SPIRAL (POTENTIAL FLOW) DUST COLLECTED DUST Figure 9. Rotary flow cyclone. 100 90 80 70 60 50 40 30 20 10 0 I i I PRESENT MODEL PREVIOUS MODEL _°~° EXPERIMENTAL Ib/ft-s- ft lb/ft; CFM 50 CFM i 1 PARTICLE DIAMETER, ym Figure 10. Performance of rotary flow cyclone (from Ciliberti and Lancaster, 1976). 36 ------- Klett, et al. (1977) reported on a high temperature and pressure design for the Aerodyne cyclone in which the inlet gas is split to provide both primary and secondary flows. They predicted outlet loadings from this cyclone based on the manu- facturers performance curves and available data on emissions from PFBC processes. Their predictions are presented in Table 8. Even if this level of performance is attained the emissions will exceed the anticipated emissions regulations (approximately 57.2 mg/Nm3 or 0.025 gr/SCF for a PFBC process). TABLE 8. ESTIMATED PERFORMANCE OF AERODYNE CYCLONE (from Klett, et al. 1977) Particle Diameter ym 0-2 2-3 3-4 4-5 5-6 6-10 10-20 + 20 TOTAL Inlet mg/Nm 460.0 153.3 153.3 153.3 153.3 460.0 766.6 13,032 15,332 Loading, 3 (gr/SCF) (0.201) (0.067) (0.067) (0.067) (0.067) (0.201) (0.335) (5.695). (6.700) Outlet mg/Nm3 96.1 22.9 13.7 9.2 6.9 4.6 0.0 0.0 153.4 Loading, (gr/SCF) (0.042) (0.010) (0.006) (0.004) (0.003) (0.002) (0.000) (0.000) (0.067) Efficiency, % 79 85 91 94 96 99 99.9 100 99.0 Cyclocentrifuge - Mechanical Technology, Inc. is developing a gas cleanup device which they call a "cyclocentrifuge" (McCabe, 1977). The basic design of this device is illustrated in Figure 11. It is a hybrid device using a rotating assembly 37 ------- SHAFT CLEAN GAS OUTLET BEARING ASSEMBLY DIRTY GAS INLET CENTRIFUGE SHELL SWIRL AUGMENTATION BLADES CYCLONE SHELL DRIVE TURBINE ASSEMBLY JOURNAL BEARING TO HOPPER Figure 11. Cyclocentrifuge (from McCabe, 1977) 38 ------- called the "centrifuge" and a stationary assembly called the "cyclone". The centrifuge is driven by a high reaction axial turbine driven by energy extracted from the process gas. The predicted fractional efficiency for this device was presented by McCabe and is shown as Figure 12. The design parameters are listed below. • Volume flow 3,457 Nm3/min (125,260 SCFM) • Inlet pressure 17 atm (250 lb/in2) • Inlet temperature 538°C (1,000°F) • Pressure drop 1 atm (14.6 lb/in2) The explanation given for the improved efficiency as com- pared to a conventional cyclone is as follows: • The length from the inlet duct to the centrifuge is longer than in a conventional cyclone. • The centrifuge collects particles that are reentrained from the cyclone section. • The centrifugal force in the centrifuge is larger than in a cyclone. • Agglomeration will be increased by the increased cen- trifugal force field. If the cyclocentrifuge works as predictedsthe outlet load- ing still may exceed the environmental regulations, depending on the mass loading of particles smaller than 2 ym. One of the most attractive aspects of cyclones for dust removal is that they have no moving parts. This is not true for the cyclocentrifuge. Operation of the centrifuge bearings at high temperature and pressure in a dirty environment is likely to present the most difficult development problem with this device. Assuming the predicted performance can be achieved and mechanical problems are not severe, the economic analysis pre- sented by McCabe indicates that the cyclocentrifuge is economi- cally viable for low-BTU coal gasification processes. 39 ------- CONVENTIONAL CYCLONE 4 56789 PARTICLE DIAMETER, ym 10 11 12 Figure 12. Comparison between estimated performance of cyclocentrifuge and conventional cyclone (from McCabe, 1977). 40 ------- Granular Bed Filters Granular bed filter technology has recently been reviewed by Yung, et al. (1977a, 1977b, 1978) to assess the state-of-the- art and to evaluate the feasibility of granular bed filters for high temperature and pressure applications. Granular bed filters may be defined as any filtration system comprised of a stationary or slowly moving bed of discrete, relatively closely packed granules as the filtration medium. With respect to motion of the granules, granular bed filters may be classified as continuously moving, intermittently moving, and fixed bed filters. Moving Bed Filters The continuously moving bed filter is usually arranged in a cross-flow configuration. The bed is a vertical layer of granular material held in place by louvered walls. The gas passes horizontally through the granular layer while the granules and collected dust move continously downward and are removed from the bottom. The dust is separated from the granules by mechanical vibration. The cleaned granules are then returned to the overhead hopper and the panel by a granule recirculation system. The Combustion Power Company's dry scrubber is an example of a continuously moving bed filter. The system is shown in Figure 13. The granular bed material flows downward between two concentric cylinders. The gas passes through the bed and is filtered by the granules. The granules are recycled pneu- matically and the collected dust particles are disengaged from the granules and sent to a conventional baghouse. The performance of this device has been reported by Wade, et al. (1978). They conducted extensive cold flow tests to in- vestigate the effects of bed depth,granule diameter, amd other parameters on the collection efficiency. Test parameters for the nominal, thick bed, and small collector granule configurations are listed in Table 9. Particulate loadings ranged from 0.46 to 4.6 g/Nm3 41 ------- MEDIA CLEANING AIR FILTERED AIR GRANULAR BED MEDIA INJECTION AIR TO BAGHOUSE INLET OUTLET SCREEN TRANSPORT PIPE MEDIA TRANSPORT AIR Figure 13. Cold flow granular bed filter parameters. 42 ------- TABLE 9. TEST PARAMETERS FOR CPC MOVING BED FILTER (FROM WADE ET AL., 1978) Mass Median Particle Configuration Nominal Thick Bed Bed Depth, mm 203.2 406.4 Medium Diameter, mm 2.0 2.0 Diameter, Vim 3.2 2.6 Small Granules 203.2 0.8 7.0* * Correlation was not materially influenced by deletion of four data points resulting in an average median diameter of 2.5 ym 43 ------- (0.2 to 2.0 gr/SCF). The superficial gas velocity was varied from 20 to 80 cm/s (40 to 160 ft/min). The medium flow rate was varied from 0.4 to 1.6 kg granules/kg air. Pressure drop ranged from 1.2 to 5.7 kPa (5 to 23 in.W.C.). Fractional efficiency curves are shown in Figures 14a, b, c. The overall penetration (and efficiency) are correlated with the pressure drop function,0, in Figures 15a, b, c. The pressure drop function was defined in English units as: AP L. e - —^ (i) V M where AP = pressure drop, in.W.C. L. = mass loading of dust, gr/SCF V = superficial velocity, ft/min M = media rate, Ib granules/lb air In general the CPC moving bed filter was found to be capa- ble of particulate removal efficiencies in excess of 98% for particles in the 1 to lOymA diameter range. Submicron particles were collected at an efficiency in excess of 90% in cases with high velocities, high loadings, and low granule rates. Beds with larger thickness to granule diameter ratios were most effective in the capture and retention of particles in the 2 to 5 ymA dia- meter range. Also, intermittent granule movement was shown to improve efficiency by a few percent. However, the economics of this operational technique have not been analyzed. High temperature tests of the moving bed filter are planned. No high temperature data are available at this time. The major advantage of the moving bed filter design is that the bed granules are removed and cleaned out of the primary gas stream. This enables efficient cleaning and a relatively steady collection efficiency. Also it is not necessary to isolate filter units during cleaning so that the total filter area open to gas flow is available for filtration at any time. 44 ------- 0\° U 2 u. UH o u 100 a 90 80 u m 70 12 4 6 8 10 12 14 AERODYNAMIC PARTICLE DIAMETER, ym 16 Figure 14a. Fractional collection efficiency, nominal configuration. 100 0\° u I—I 0- U-, tu § I—I H u tu »J o u 90 80 U 12 4 6 8 10 12 14 16 AERODYNAMIC PARTICLE DIAMETER, ym Figure 14b. Influence of operational parameter combinations on fraction efficiency (16" filter, 2mm media). 45 ------- u u h- 1 UH B- U4 100 90 80 70 4 6 8 10 12 AERODYNAMIC DIAMETER, umA 14 16 Figure 14c. Fractional efficiency performance, small media configuration. 10 -1 g 10 o cfl £ io-2 10 _3 10 -2 cor 10 -1 0.5 0.9 0.95 § •H 4-> U rt u 0.99 0.995 10 Figure 15a. Influence of pressure drop function on overall collection efficiency, nominal configuration. 46 ------- 10 o o oj 10 -1 £ io-2 10" _ 3 o;s 0.9 u 0.95 g hH U. W 0.99 0.995 10 -2 10 - 1 10 0 Figure 15b. Influence of pressure drop function on overall collection efficiency, thick bed configuration. g 0.10 O cU (H 0.01 g I-H U tu W 0.01 0.1 1.0 e Figure 15c. Influence of pressure drop function on overall collection efficiency, small media. 47 ------- The moving bed design also has some limiting operating characteristics. The granule recirculation system adds signifi- cantly to the operating cost. Particle reentrainment caused by the relative motion of the granules limits the granule flow rate and affects the overall collection efficiency. Erosion of the retaining grids, louvers, and transport system components may be a problem, especially in high temperature and pressure systems. The collected dust particles cannot form a filter cake so that the operating efficiency will be essentially that of a clean bed. Temperature losses may be large and will be propor- tional to the energy required to keep the granules hot during recirculation. It may be possible to resolve most of these problems through further development and testing. Performance data at , high temperatures and pressures will be important in identifying the most serious operational problems. Intermittently Moving Bed In the late 1950s, Squires modified the continuously moving bed design to obtain a fixed bed device with an intermittent movement of granular solids. The bed is stationary during fil- tration. The accumulated filter cake and the surface layer of granules are ejected from the panel by a sharp backwash pulse and fall to the bottom of the filter vessel. The expelled granules are immediately replaced by downward movement of fresh granules from the overhead hoppers. Intermittent movement is normally limited to vertical panel filters. The granules are intermittently removed in a cross.-flow arrangement panel bed. The advantage of this type of bed struc- ture is the capability for external granule/dust separation with minimum disturbance to the rooting cake. A rooting cake is the foundation for the formation of a surface cake. After cleaning, the surface cake is formed readily without disturbing the rooting cake and filtration efficiencies can be much higher. The intermittently moving bed also has the advantage that granule cleaning is off-line and potentially more effective. 48 ------- The major disadvantage is that the gas capacity is lower than for other granular bed filter designs and this results in high capital costs for a given installation. During cleaning, about two to three layers of granules are removed from the bed. To prevent the dust from being carried deep into the bed by the gas, CCNY recommends the velocity be kept as low as possible to reduce the aerodynamic drag force- They usually operate the panel bed filter at about 15 cm/s (30 ft/min). This velocity is about one third the velocity used in the fixed bed and con- tinuously moving bed GBFs. Thus, more filtration area is required. Bed plugging also can be a problem if the surface cake is not formed properly. Erosion of the retaining grids, louvers, and other components may be a problem. Granule recirculation temperature losses, and the requirement for blow-back air pulses during cleaning add to the overall operating costs. Recent work on the CCNY panel bed was reported by Lee, et al. (1977). Fixed Bed Filters Fixed bed filters operate in two modes; the filtration mode and the cleaning mode. During filtration the bed is sta- tionary. The gas passes through the bed and collected particles are deposited within the bed and on the bed surface. During cleaning the bed is isolated from the main flow and agitated mechanically or pneumatically by a reverse flow of gas. There are two fixed bed devices currently being developed; the Rexnord gravel bed filter and the Ducon granular bed filter. The Rexnord filter (Figure 16) uses a rake-shaped stirring device to agitate the bed during cleaning. This loosens the filter cake which is then removed by a reverse flow of clean air. Rexnord granular bed filter - No Rexnord filters have been tested at high temperature and pressure, however, McCain (1976) reported the results of a performance test on a Rexnord filter used to control the emissions from a clinker cooler in a Portland cement plant. 49 ------- OPERATING PHASE BACKFLUSH PHASE 12 14 BACKFLUSH AIR 1. INLET CHAMBER 2. PRIMARY COLLECTOR (CYCLONE) 3. DOUBLE TIPPING GATE (DUST DISCHARGE) 4. VORTEX TUBE 5. FILTER CHAMBER 6. GRAVEL BED 7. SCREEN SUPPORT FOR BED 8. CLEAN GAS COLLECTION CHAMBER 9. EXHAUST PORT 10. BACKWASH CONTROL VALVE 11. BACKWASH AIR INLET 12. VALVE CYLINDER 13. STIRRING RAKE 14. STIRRING RAKE MOTOR/REDUCERS Figure 16. Rexnord gravel bed filter. 50 ------- Samples were taken simultaneously at the filter inlet and outlet with cascade impactors. The operating conditions of the gravel bed were: Gravel diameter = 4 mm Face velocity = 73 cm/s Gas temperature = 174°C Pressure drop = 25.4 cm W.C. The grade penetration curves for these tests are shown in Figure 17. The predicted curve was obtained using the model presented by Yung, et al. (1977b) which assumes the bed is clean and particulate collection results from the inertial impaction mechanism only. Ducon granular bed filters - The Ducon granular bed filter cleans the bed by a reverse flow of gas which fluidizes the bed and elutriates the fine collected particles. The filtration and cleaning modes of the Ducon filter are illustrated in Figure 18. The Ducon filter was tested on the effluent from a fluid bed catalytic cracking unit regenerator at an oil refinery (Kalen and Zenz, 1973). The gas was at 370°C to 480°C and 1 to 1.5 atm. The dust loading ranged from 0.34 to 1.94 g/m3 (0.15 to 0.85 gr/ ACF) . A collection efficiency of 85-98% was obtained on dust with a mass median diameter of 35 ym and a geometric standard deviation of about 4. Yung, et al. (1978) estimated fractional penetrations from their data and the results are shown in Figure 19. A high temperature and pressure design of the Ducon filter was tested at the Exxon miniplant (Hoke, et al., 1978). Ini- tially severe plugging of the bed retaining grids was encountered, This problem was resolved by eliminating the grids and redesign- ing the bed housing to provide sufficient freeboard above the bed to allow cleaning of the bed without loss of bed material. The modified filter module is illustrated in Figure 20. A number of operating problems were encountered during the 51 ------- 1.0 0.5 o I o DJ o.i tu _J y 0.05 (X 0.01 0.1 DATA J I I I THEORY 0.5 1.0 AERODYNAMIC PARTICLE DIAMETER, ymA 10 Figure 17. Experimental grade efficiency curve of a Rexnord gravel bed filter (McCain, 1976). 52 ------- FILTRATION CYCLE BLOWBACK CYCLE FILTER MEDIA CLEAN GAS EXIT DIRTY GAS RETAINING SCREEN ^ 7 *,v> ^^m m '"*. -"'••:• *2 ***/"' ^ 1 1 ^ f ':•'." *^ • •^1: .'-V ^»*.-. ^ '•%'• & m \ FLY ASH f- *~ DIRTY GAS FLUIDIZED FILTER MEDIA LOCK HOPPER LOCK HOPPER Figure 18. Ducon granular bed filter. 53 ------- 1.0 0.05 u P-. oi w z tu 0.1 0.05 0.01 I I I i i 0.5 5 10 PARTICLE DIAMETER, ym I I J I i 15 Figure 19. Fractional penetration for Ducon granular bed (from Kalen and Zenz, 1973). 54 ------- DIRTY GAS TOP RETAINING SCREEN BOTTOM RETAINING SCREEN FILTER MEDIUM CLEAN GAS Figure 20a. Schematic o£ a single Exxon filter bed. DIRTY GAS INLET -*- CLEAN GAS OUTLET FLUIDIZING GRID I i Figure 20b. Modified filter bed. 55 ------- Exxon tests of the modified Ducon filter. The lowest demon- strated particulate outlet concentration was 68.6 mg/Nm3 (0.03 gr/SCF) which was considered to be too large to protect a gas turbine and borderline for meeting current emissions regulations, The use of smaller filter media could be expected to improve efficiency. However, at times the filtration efficiency was very poor and the outlet particulate concentrations were as high as 700 to 1,200 mg/Nm3 (0.3 to 0.5 gr/SCF). It was also ob- served that the efficiency decreased with time in the longer runs, dropping from 90% initially to about 50% later in the run. Loss of filter medium during blow back was another recurring problem. Further attempts were made to use 50 mesh retaining screens but they failed because of plugging. Additional tests made with 10 mesh screens also resulted in significant screen plug- ging. A large buildup of particles in the filter beds also was observed amounting to about 30% of the weight of the filter medium. A possible steady long term increase in filter pressure drop may result because of this. However, no signifi- cant increase in filter pressure drop was noted during any of the shakedown runs. It was observed that the particles were not only building up in the beds, but were uniformly mixed with the fil- ter medium. It is possible that the buildup and mixing of parti- cles in the bed could be responsible for the increase in the particle concentration in the outlet gas with time. Another potential problem with the current design was its vulnerability to upsets. When upsets occurred, such as bed plugging or loss of filter medium, the operating problems caused by such upsets required shutdown of the system. Another problem which may be unique to the miniplant was the interaction of the granu- lar bed filter with the rest of the FBC system during the blow back cycle. An increase in system pressure was noted during blow back resulting in problems with the coal feed system 56 ------- which is controlled by the differential pressure between the coal feed vessel and combustor. This required modifications to the coal feed control system to minimize these effects. Granular bed filter performance data for all runs through November, 1977 are listed in Table 10. The efficiencies are based on an inlet concentration of 2.3 g/Nm3 (1.0 gr/SCF) which is the average for the emissions from the secondary cyclone. Fractional efficiency data are presented in Figure 21. The granular bed filter test program was suspended in November, 1977. In all runs in which more than one outlet con- centration was measured, it was observed that the outlet con- centration increased with time. They were not able to demon- strate that the current EPA emission standard (0.1 lb/106 BTU or 0.05 gr/SCF) could be met for more than a few hours of opera- tion. In no run was the anticipated new standard (0.05 lb/106 BTU or approximately 0.025 gr/SCF) satisfied. Further tests are planned on a 0.85 m3/min (30 ACFM) slip stream from the miniplant combustor. The slipstream will be at 870°C and 9 atm pressure. If the filter can be modified to satisfy the EPA regulations for a prolonged run, it will be tested on the full miniplant flow stream. Summary At this time granular bed filters have not been demonstra- ted to be efficient enough to perform as tertiary collectors in high temperature and pressure gas cleanup systems. High collection efficiencies may be obtained if a filter cake is formed on the surface of the bed. This has been accom- plished with the CCNY (Squires) design at low temperature and pressure operating conditions. Efficiencies in excess of 99.9% have been measured. However, when this filter was tested at the Morgantown Energy Research Center at 1,000°F, no filter cake was formed, although 99% efficiency was obtained. Operation of the Ducon granular bed filter at the Exxon miniplant also indicated that no filter cake was formed. 57 ------- TABLE 10. GRANULAR BED FILTER PERFORMANCE (FROM BERTRAND ET AL., 1977) Outlet Concentration Run Number 54 57 59 59 59 61 62. 62. 63 63 63 64 64 64 65 65 66 gr/SCF 0. 69 0.04-0.08 (Sample (Sample (Sample 1 3 (Sample (Sample (Sample (Sample (Sample (Sample (Sample (Sample 1) 2) 3) 1) 2) 3) 1) 2) 3) 1) 2) 0. 0. 0. 0. 0. 0. 0. 0. 0. 0. 0. 0. 0. 0. 0. 08 28 54 46 03 21 05 07 12 28 29 27 05 06 06 g/m3 1. Collection Efficii 57 0.09-0.18 0. 0. 1. 1. 0. 0. 0. 0. 0. 0. 0. 0. 0. 0. 0. 18 64 23 05 07 48 11 16 27 64 66 61 11 14 14 31. 0 92.0-96.0 92. 72. 46. 54. 97. 79. 95. 93. 88. 72. 71. 73. 95. 94. 94. 0 0 0 0 0 0 0 0 0 0 0 0 0 0 0 * Based on a 2.3 g/Nm3(1.0 gr/SCF) inlet concentration 58 ------- en 100 96 w 92 o 3 88 u Si 84 80 I I I 6 8 10 12 PARTICLE DIAMETER, ym 14 16 18 Figure 21. Fractional efficiency data for Ducon GBF (from Bertrand, et al.) 1977). ------- Therefore, the current state of development of granular bed filters for high temperature applications seems to be pre- dominantly limited to clean bed filtration. The model developed by Yung, et al. (1977b, 1978) can be used to predict performance for clean bed granular bed filters. This has been done using typical operating parameters from the Exxon tests, as listed below. Granule diameter = 400 ym Bed depth = 3.8 cm Superficial velocity = 45 cm/s Particle mass median diameter = 3.5 ym Particle density = 1.5 g/cm3 Bed porosity = 0.25 The results are presented as Figure 22. The collection efficiency decreases (penetration increases) radically as the gas conditions go from ambient to high temperature and pressure This effect should be remembered when interpreting low tempera- ture and pressure performance data for granular bed filters. There are many operational problems and uncertainties which need to be resolved before HTP granular bed filters can be considered sufficiently reliable for commercial application. These problems include the needs to: 1. Prevent particle seepage through the bed (during cleaning or filtration. 2. Reduce temperature losses (especially during cleaning). 3. Improve the efficiency and reduce the cost of granule regeneration and recirculation. 4. Prevent attrition of granules causing particle reentrainment. 5. Prevent sintering of granules. 6. Prevent plugging of retaining grids. 7. Reduce pressure drop across the bed. 60 ------- 1.0 0.5 o O 0.1 jg g 0.05 0.01 10 atm 20°C I I I i GRANULE DIAMETER: 400 ym BED DEPTH: 3.8 cm SUPERFICIAL VELOCITY = 45 cm/S~ PARTICLE DENSITY =1.5 g/cm3 _ POROSITY =0.25 10 atm 870°C 1 apn 870 C i i i i i i i i 0.1 0.5 1.0 PARTICLE DIAMETER, ym Figure 22. Predicted GBF performance. 10 61 ------- Resolving these problems may provide a solution to the HTP particle collection problem, and will improve granular bed filter technology for many other applications, especially where hot, corrosive gases are encountered. Scrubbers Wet scrubbers are not generally suitable for high tempera- ture and pressure gas cleaning because they necessarily cool down the gas. It is possible to cool the gas in a regenerative heat exchanger and then use a wet scrubber to clean the gas at high pressure before the gas is reheated. Wet scrubbers also are used for tar removal, H2S removal, and particulate removal in many coal gasification process designs. Dry scrubbers and molten glass or metal salt scrubbers are being developed for hot gas cleanup applications. These systems are described and available data are reported below. A.P.T. Dry Scrubber A.P.T., Inc. is developing a dry scrubber system, called the PxP (particle collection by particles) system which can be used for high temperature and pressure gas cleaning. This system has been reported by Calvert et al.(1977) and Patterson, et al.(1978). The PxP system is somewhat similar to a venturi scrubber sys- tem in that it uses relatively large particles as collection centers for the fine particles in the gas stream. The principal advantage with this system is that it maximizes the collection efficiency of individual collector particles and thereby reduces the number of collectors that need to be cleaned and recycled. The collector particles introduced to the gas stream collect fine particles by mechanisms such as diffusion, inertial impaction, interception and electrophoresis. The larger size of the collector particles allows easy separation from the gas stream by methods such as cyclones and gravitational settling. Figure 23 is a functional diagram of the process steps for a representative PxP system. The functions represented on this diagram could occur concurrently or separately in several 62 ------- CONTACTOR SEPARATOR DUSTY GAS COLLECTOR PARTICLES CLEAN GAS DISCARD +- DISCARD COLLECTOR CLEANER Figure 23. Schematic diagram of A.P.T. dry scrubber system. 63 ------- types of equipment. The first step involves introducing the collectors to the gas stream. This process can involve pneumatic or mechanical injection. The second stage involves contacting the collectors with the gas in such a way as to encourage the movement of the fine particles towards the collectors. A venturi device can be used for the contactor in which case the system would be analogous to a venturi scrubber with solid collectors used instead of liquid drops. The next process step is to remove the collector particles after they have captured the fine particles initially present in the gas. This is accomplished by using the large size and mass of the collector particles to separate them from the gas. A cyclone separator, gravity settler, or virtual impactor could be used for this step. Two streams are shown leaving the separator: the cleaned gas leaves the process at this point and the second stream represents the flow of collector particles to the next step. The final process involves either discarding the collector particles or cleaning them for recycle and disposing of the particulate matter collected from the gas stream. The particle collection efficiency and pressure drop for an A.P.T. dry scrubber with cocurrent flow can be predicted with the same relationships that define cocurrent wet scrubber performance. The theoretical performance of the PxP scrubber has been determined based on the venturi scrubber performance model of Yung, et al. (1977). Figure 24 shows the predicted efficiency at 20°C and 820°C. Efficiencies will be somewhat lower at high pressure for the same pressure drop. Experimental work has been done by A.P.T. to determine fine particle collection efficiency in a PxP scrubber in order to confirm the predictions obtained from available mathematical models. A dibutylphthalate (DBP) aerosol was used in collection efficiency experiments with 100 ym mean diameter sand as collec- tor particles. The DBP aerosol had a mass median aerodynamic diameter of 1.3ymA and a geometric standard deviation of 2.0. 64 ------- 1.0 0.05 Z O O cu w Cu 0.1 0.005 0.001 0.0005 0.001 820°C 0.1 0.2 0.5 1.0 2 5 PARTICLE AERODYNAMIC DIAMETER, ymA 10 Figure 24. Predicted performance for A.P.T. dry scrubber. 65 ------- The resulting penetration data are shown in Figure 25. The prediction is also shown in Figure 25 and compares well with the experimental curve. Higher collection efficiencies can be achieved using denser collector particles. For this reason experiments were also conducted with 125 ym nickel beads. Particle penetration data for all runs with nickel and sand collectors are represented in Figure 26 in terms of the 50% cut diameter as a function of gas pressure drop. The line represents the best available relationship for industrial scale wet venturi scrubbers. Therefore the A.P.T. dry scrubber follows the same primary collection efficiency/power relation- ship as venturi-type wet scrubbers. The overall efficiency of the PxP system will depend on the reentrainment characteristics of the specific system confi- guration in addition to the primary collection efficiency. Particle and collector properties, system geometry, flow rates, and other parameters will influence reentrainment. A.P.T. has built an atmospheric fluidized bed coal combus- tor which will be used for testing a pilot plant PxP system at high tem- perature. Electrostatic augmentation is also being investigated as a means of increasing the collection efficiency independently of pressure drop, and possibly improving the adhesion of fine particles to collector particles. The economics of the PxP system for high temperature and pressure particulate control will be analyzed in connection with the pilot plant test program. Molten Salt Scrubber Battelle-Northwest has constructed a process demonstration unit for the molten salt scrubber. The scrubber is designed to remove H2S as well as particulates from the high temperature and pressure gases produced in low-BTU coal gasification pro- cesses. Minor impurities such as halogens, volatile metals and non-metals, and ammonia also potentially could be removed from the gas with this system. Details of the system design and pilot plant data were presented by Moore, et al. (1977). The system consists of a 66 ------- 1.0 o t-H E~ U I-H H W O- 0.1 0.01 \ \ I THEORETICAL EXPERIMENTAL 0.1 0.5 1.0 2.0 AERODYNAMIC DIAMETER, ymA 5.0 Figure 25. Comparison of experimental with theoretical particle collection characteritics of the A.P.T dry scrubber. 67 ------- oi tu H Q U Q § UJ 3.0 2.0 1.0 0.7 0.5 0.3 0.2 0.1 I r I I HORIZONTAL Q VERTICAL FLOW Q THEORETICAL I I I I I 0.1 0.2 0.3 0.5 0.7 1 23 GAS PHASE PRESSURE DROP, kPa I I 7 10 Figure 26. Comparison of particle characteristics of the A.P.T. dry scrubber with the A.P.T. cut/power relationship. 68 ------- venturi scrubber followed by a packed tower entrainment separator. The venturi is operated vertically to avoid the need for a mechan- ical pump to feed the molten salt. The salt composition used is shown in Table 11. The parti- culate removal efficiency was measured using an Andersen impactor. The particle size distribution and mass loadings leaving the scrubber are shown in Tables 12 and 13. Poe, et al. (1977) evaluated the molten scrubber process for particulate control. They pointed out numerous potential problems including material corrosion, alkali metal vapor emis- sions, line clogging due to precipitation of metal oxides, par- ticulate buildup in the molten salt and particulate solubility in the molten salt. Their analysis indicated that, from an economic standpoint, molten scrubbing appears to be a promising approach for high temperature fine particle collection. They did not consider the effect of gas density on the scrubber performance at high pres- sure. Theoretical considerations based on the venturi scrubber model of Yung, et al. (1977) indicate that high temperature and high pressure operation may be less favorable in terms of the pressure drop required to achieve a desired efficiency. Hot Gas Cleanup by Molten Glass The General Electric Company is investigating the use of coal slag based glasses for hot gas cleanup. Preliminary work has been presented by McCreight, et al. (1977) and Fedarko, et al. (1978). Figure 27 shows viscosity curves for typical coal slags as a function of temperature. Particulate collection studies are being carried out by inertial impingement onto plates coated with glycerine. In the temperature range -20 to 30°C glycerine has a similar viscosity to that of coal slag in the range 1,200 to 1,600°C. The work is in a very early stage and there are no data available to indicate the potential particle collection efficiencies and operational problems that can be expected for large scale molten glass scrubbing equipment. 69 ------- TABLE 11. SALT COMPOSITION USED IN PDU DEMONSTRATION RUNS (FROM MOORE, ET AL., 1977) Component Li2C03 Na2C03 K2C03 CaC03 Mole % 18.0 37.3 29.6 15.1 Weight % 13.0 36.0 37.3 13.8 TABLE 12. PARTICLE SIZE DATA; MOLTEN SALT PILOT PLANT RUN NUMBER 3 (FROM MOORE, ET AL., 1977) Inlet Gas; Total Particle Burden = 0.109 gr/SCF, % H20 =9.1 Outlet Gas; Total Particle Burden = 0.077 gr/SCF, % H20 = 4.5 Anderson Head Particle Size Distribution Plate No. 1 2 3 4 5 6 7 8 Filter Total Wt. 0. 0. 0. 0. 0. 0. 0. 0. 0. 0. Calculated Gain Effective g Cut-off Dia, ym % 0048 0042 0327 0498 0405 0381 0289 0314 0948 3253 17. 11. 7. 5. 3. 1. 1. 0. — 6 2 5 3 5 7 0 7 1. 1. 10. 15. 12. 11. 8. 9. 29. 5 3 1 3 5 7 9 7 2 Concentration in Gas gr/SCF 0. 0. 0. 0. 0. 0. 0. 0. 0. 00114 00099 00774 0118 0096 0091 0069 0075 0224 0. 0. 00 0. 0. 0. 0. 0. 0. g/Nnr' 0026 0023 0176 0270 0220 0208 0158 0172 0513 70 ------- TABLE 13. PARTICLE SIZE DATA; MOLTEN SALE PILOT PLANT RUN NUMBER 6 (FROM MOORE, ET AL., 1977) Inlet Gas; Total Particle Burden = 0.074gr/SCF, % H20 = 11.2 Outlet Gas; Total Particle Burden = 0.024 gr/SCF, % H20 =3.3 Anderson Head Particle Size Distribution Plate No. 1 2 3 4 5 6 7 8 Filter Total Wt. Gain g 0.0015 0.0013 0.0016 0.0019 0.0026 0.0029 0.0030 0.0047 0.0106 0.0301 Calculated Effective Cut-off Dia, ym 20.1 10.5 7.0 5.0 3.1 1.6 1.0 0.6 -- % 5.0 4.3 5.3 6.3 8.6 9.6 10.0 15.6 35.2 Concentration gr/SCF 0.0012 0.0011 0.0013 0.0015 0.0021 0.0021 0.0024 0.0038 0.0086 in Gas g/Nm3 0.0027 0,0025 0.0030 0.0034 0.0048 0.0048 0.0055 0.0087 0.0197 71 ------- pq en i—i O o. 8 AVERAGE MONTANA ROSEBUD SLAG (K-875) TYPICAL AVG. SLAG (K-884) AVERAGE ILLINOIS NO. 6 SLAG (K-878) 1200 1300 1400 1500 1600 1700 TEMPERATURE, °C Figure 27. Viscosity/temperature relationship determined by NBS on synthetic slags formulated to represent the average compositions of fly ash from Montana Rosebud and Illinois No. 6 coal types. ------- Electrostatic Precipitation The normal operating temperature range for industrial electrostatic precipitators is 20 to 300°C. In a few special applications they are used at temperatures up to about 550°C. The application of electrostatic precipitation at higher tem- peratures and pressures has been considered in many studies over the past 30 years. Roller and Fremont (1950) studied the corona characteristics of precipitators at temperatures to 500°C and pressures to 5 atm. Thomas and Wong (1958) conducted a similar study to 800°C and 8 atm. Both studies showed that the current-voltage charac- teristics were predominantly a function of gas density rather than temperature and pressure independently. Thomas and Wong exper- ienced regions of instability at temperatures above approximately 800°C at atmospheric pressure. At 815°C and pressures above 4.6 atm (relative density >_ 1.25) adequate electric field can be maintained for effective electrostatic precipitation. Shale and Faaching (1969) reported on the operation of a high temperature (800°C) and pressure (6.4 atm) electrostatic precipitator. Dust removal efficiency ranged from 91 to 96% for negative corona with a voltage of 36.5 kV and power input averaging 6.4 kW. For positive corona the efficiency was only 75 to 77% even though a higher operating voltage was possible (54 kV) at a lower power input (2.0kW). The particulate matter had a mass median diameter of approximately 30 to 40 ym. There was no significant mass below 5 ym. The input power-removal efficiency relationships at high temperature (800°C) compared favorably with those found in con- ventional industrial precipitation. No apparent insurmountable electronic problems were encountered, however, thermal misalignj ment of the tube and mechanical difficulties with the tube rapper presented problems. Brown and Walker (1971) operated an electrostatic precipi- tator at about 900°C and 4.4 atm. Particle removal efficiencies ranged from 25% for positive polarity to 87% for negative polarity, Test data are summarized in Table 14. 73 ------- TABLE 14. TEST DATA SUMMARY FOR ESP AT 900°C, 4.4 ATM (FROM BROWN S WALKER, 1971) Run No. 1 2 3 4 5 6 Polarity Negative Positive Negative Positive Negative Negative Applied Voltage, kV 29 47.5 34 25.5 42 44.5 Current , mA 1.9 4.6 3.7 2.4 3.5 11.0 Field Strength, kV/cm 2.9 4.6 3.3 2.5 4.1 4.4 Power, W 55 230 126 61 147 490 Efficiency, % 37.7 25.0 59.5 16.0 73.5 78.1 Effective Migration Velocity, cm/s 1.8 0.9 3.4 0.6 5.2 5.8 74 ------- The effective migration velocity for negative polarity averaged about 4.0 cm/s. This is about half that ex- pected for a conventional precipitator operating at a similar field strength and low temperature. The lower migration velocity can be accounted for adequately by considering the effect of high temperature on the gas viscosity. More recent work on high temperature and pressure electro- static precipitation has been reported by Feldman, et al. (1977, 1978) and by Robinson (1978). They reported work conducted at Research-Cottrell which demonstrated that stable operating condi- tions can be maintained at temperatures and pressures up to 1,100°C and 35 atm. Their major conclusions are summarized below: 1. There are no temperature or pressure limitations to electrostatic precipitation over the range studied. Practical high temperature precipitation may be limited by thermal ioniza- tion at temperatures exceeding 1,100 to 1,300°C. 2. High temperature and pressure enables operation at higher voltages than is possible at standard conditions. This is in part due to the supression of back-corona by operation at high pressure. The higher operating voltage should more than compen- sate for the adverse effect of high temperature gas viscosity on the migration velocity and collection efficiency. 3. The critical pressure (above which sparkover results) increases with temperature. Negative polarity gives higher critical pressure than positive polarity. 4. In most cases negative currents are larger than positive currents. They prepared a preliminary design for a high temperature and pressure electrostatic precipitator to be used in a pressurized fluidized bed combustion unit. The operating temperature and pressure are 815°C, 10 atm. Their recommended design parameters are presented in Table 15. 75 ------- TABLE 15. RECOMMENDED DESIGN PARAMETERS FOR HTP ESP (FROM FELDMAN ET AL., 1977) Number of Precipitators per Boiler Module Pipes per Precipitator Pipe Size Vessel Diameter Vessel Height Steel Thickness Vessel Weight Capacity MW of Plant capacity Collecting Surface Area Discharge Electrode Length Specific Collection Area Expected Efficiency Power Supply Voltage Current Discharge Electrode 320 0.229 x 3.05 m 7.0 m 10.7 m 0.038 m 52.8 x 103 kg 19.82 m3/s 42,000 ACFM 106,000 SCFM 75 MW 700.5 m2 975.4 m 35.3 m2/m3/s 180 ft2/103 ACFM 98-99% 150 kV 3,0:00 mA 3.08 mA/m 76 ------- TABLE 15. Continued Current Density/Collecting 4.31 mA/m2 Surface Specific Power 1.462 x 10"W/m3/s 6.9 W/ACFM Capital Costs Per Precipitator - Less Engineering Stainless steel internals $1,945,000 Inconel internals $2,185,000 Per 300 MW Plant - Including Engineering Stainless steel internals $7,980,000 Inconel internals $8,940,000 Per kW of Plant Capacity Stainless steel internals $26.60/kW Inconel internals $29.80/kW 77 ------- The recent Research-Cottrell work did not include the effects of dust particles on the electrical performance. In general, the presence of dust particles suppresses current flow and creates a space charge between the electrodes. This enables higher operating voltages than are possible in a clean gas. However, as dust accumulates on the collection surface the sparkover voltage decreases and may to some extent nullify the effect of space charge. Many practical problems are likely to be encountered in the further development and demonstration of HTP electrostatic precipitation. The very low electrical resistivity of ash par- ticles at temperatures above 400-500°C may result in excessive reentrainment during electrode rapping operations. Also mechani- cal problems such as electrode alignment and strength after many rapping cycles will need to be resolved. Also it will probably be necessary to follow the precipita- tor with a barrier collection device such as a granular bed filter because even brief outages of the precipitator can cause catastrophic damage to the gas turbine. Plans are being considered for testing the Research-Cottrell high temperature and pressure electrostatic precipitator on a slip' stream from the Exxon PFBC miniplant. It would operate at 870°C 9 atm, and would handle 0.85 m3/min (30 ACFM) of gas containing 2.3 g/Nm3 (1.0 gr/SCF) of fly ash particles with a mass median diameter of about 4 urn and a geometric standard deviation of approximately 3. Fiber Filtration Conventional fabric filters are limited to operating tempera- ture below 250°C. The maximum temperature varies with the spe- cific fabric and is determined as the temperature at which accel- erated fabric deterioration or abrasion occurs. Glass fiber bags are the most common type used for higher temperature applications and are limited to about 300°C. The glass fibers are coated with a silicone, silicone-graphite, or equivalent finish in order to provide lubrication between the 78 ------- fibers. Unfinished glass fibers experience extreme abrasion and unsatisfactory bag life. The temperature limit of glass fiber fabrics is directly related to the temperature limit of the finish. Lundgren and Gunderson (1976) reviewed the filtration characteristics of glass fiber filters at elevated temperatures (to approximately 500°C). Their review indicated that in practice the effect of temperature and pressure on filtration mechanisms was not a determining factor in the application of high effi- ciency filters. The main problems are the physical and chemical effects of a high temperature environment on the filter materials. These effects may appear as reduced mechanical strength and re- silience or loss of adhesion, leading to mechanical leakage, decrease in efficiency and eventually mechanical failure. High Temperature Filtration Studies Filtration media for extreme temperatures and pressures has been investigated by many authors. Silverman and Davidson (1956) suggested the use of ceramic fibers sandwiched between layers of woven metallic or ceramic fabrics for filtration at temperatures to 1,100°C and higher. Billings, et al. (1955) and Silverman (1962) discussed the use of metallic fiber "slag/wool" filters for high temperature filtration of open-hearth furnace fume. They tested the slag-wool filter at temperatures from 300 to 650°C and dust loadings from 0.1 to 1.1 g/Nm3 (0.1 to 0.5 gr/SCF). Efficiencies ranged from 75 to 98%. A continuous slag-wood fil- ter was designed and tested at 300-400°C. The efficiency ranged from 10 to 80% for Fe20a particles with a mass median diameter of 0.65 ym. First, et al. (1956) and Kane, et al. (1960) reported on the use of ceramic fiber filters capable of withstanding tem- peratures up to 1,100°C. First, et al. (1955) measured collec- tion efficiencies at 21°C and 760°C. The mass median particle diameter was 8.5 ym with a particle density of 6.4 g/cm3. The effect of temperature on efficiency for individual fiber dia- meters is shown in Table 16. 79 ------- TABLE 16. EFFECT OF TEMPERATURE ON FILTRATION EFFICIENCY (FROM FIRST, ET AL. 1955) Filter Diameter, ym 20 8 4 Filter Depth, cm 10.16 3.81 2.54 Superficial Velocity cm/s 203.2 203.2 203.2 Efficiency, Wt. % 21°C 85 99 98 760°C 82 94 91 TABLE 17. FRACTIONAL EFFICIENCY FOR COMPOSITE FILTER TESTS (FROM FIRST, ET AL., 1955) Particle Diameter Range Collection Efficiency 0-1 urn 28.4% 1-2 ym 95.4% 2-5 ym 99.4% >5 ym 99.4% 80 ------- A composite filter comprised of fibers from 4 ym to 20 ym in diameter gave over 99% collection for all temperatures. The fractional efficiency for the composite tests is shown in Table 17. Theoretical Predictions Filtration theory has been reviewed by many authors including Davies (1973) and Pich (1966). We have used the theory presented by Davies to predict the collection efficiency of a clean fiber filter at high temperature and high pressure. The following parameters were assumed: Filter weight = 0.026 g/cm2 Fiber density = 2.53 g/cm3 Fiber diameter = 5.0 ym Superficial velocity = 12 cm/s Particle density = 2.5 g/cm3 Air properties at: Temperature = 20°C and 1,100°C Pressure = 1 atm and 15 atm These parameters simulate a typical aluminum-silicate ceramic paper. The results are presented in Figure 28. At high temperature and low pressure the Brownian diffusion regime becomes very significant and the collection efficiency of particles smaller than approximately 0.5 ym increases drama- tically. At high temperature and high pressure this effect is less apparent. In the inertial impaction regime, high temperature and high pressure reduce the collection efficiency from that obtained at standard conditions. Even at high temperature and pressure, however, the predicted collection efficiency is effectively 100% for particles larger than 2 ym. This is consistent with the data reported earlier from the work by First, et al. (1955). Current Development Work Recent development work on high temperature and pressure ceramic fiber filters is being carried out by Acurex Corporation 81 ------- oo 100 90 80 70 w 60 U, UH UJ g 50 w 40 30 20 10 7 / INERTIAL IMPACTION / / REGIME 1 atm 15 atm I I I I I 0.1 0.2 1.0 0.5 PARTICLE DIAMETER, ym Figure 28. Predicted performance for ceramic fiber filter. 2.0 ------- and has been reported by Shackelton (1977, 1978). They have conducted a detailed survey and evaluation of ceramic fiber media with potential for high temperature filtration, Available ceramic fiber configurations can be classified into the following three groups of materials: 1. Woven structures - Cloth woven from long-filament yarns of ceramic fibers. 2. Papers - Ceramic structures produced from short lengths of fibers, generally held together with binders. 3. Felts - Structures produced to form mats of relatively long fibers. These materials are known as blankets in the insulation industry. They tend to be less tightly packed than conventional felt materials. A summary of room temperature data is presented in Table 18. The last three materials are conventional fabric filter media which are only included for purposes of comparison. A number of the media show high collection efficiencies for 0.3 ym dia- meter DOP aerosol particles. It should be noted that this is the efficiency of a clean filter media and higher efficiencies can be anticipated for a dirty filter operating with some residual dust deposited between the fibers. Permeability is measured as the flow per unit area at a constant pressure drop. Thus, a material with low permeability offers a high restriction to gas flow and one with high perme- ability allows more gas to penetrate for a given pressure drop. Table 18 shows that some ceramic materials are available which have low permeability, while others have high permeability. Most of the paper and felt materials have permeability similar to that of commonly used filter materials. Ceramic fiber filters have two major drawbacks regarding application at high temperature and pressure. First of all they must be very durable. Conventional filter bags are expected to last at least one year (see Billings and Wilder, 1970). Bag life at the Nucla Power Plant was estimated to be 5+ 1.3 years 83 ------- TABLE 18. CERAMIC FIBER TEST DATA (FROM SHACKLETON AND DREHMEL, 1978) (W) Woven (P) Paper (F) Felt 1. Carborundum Fiberfrax cloth (W) with nichrome wire insert 2. Zircar Zirconia felt ZFY-100 (F) 3. ICI Saffil alumina paper (P) with binder 4. ICI Saffil mat (F) 5. Babcock S Wilcox Kaowoll (F) 6. Carborundum Fiberfrax (F) durablanket 7. John-Mansville Fiberchrome (F) 8. Stevens Astroquartz (W) style 581 9. Hitco Refrasil C-100-96 (W) heat cleaned 10. Hitco Refrasil C-100-48 (W) not heat cleaned 11 . Stevens Astroquartz cloth Basis Weight g/m2 1366 615 165 355 746 1363 1297 283 1284 667 667 Permeability Percent Efficiency on cm3/s/cm 2 ft3/min/ft2 0.3 ym OOP at cm/s 1.27 cm H20 at 0.5 in. W.C. 2.68 5.35 14.22 8.7 10.9 9.3 12.4 8.1 5.6 11.9 37.2 1.2 3.1 22.8 17.1 45 21.4 75 18.3 82 24.4 79 15.9 96.5 11.0 97.1 23.4 78 73.3 0 2.4 0 6.1 0 44.8 0 47 78 65 80 93.5 94.6 73 9 19 11 13 50 72 62 73 86 90.5 74 12 34 10 32 (W) style 570 continued ------- TABLE 18. Continued 00 in (W) Woven (P) Paper (F) Felt 12. 3M AB-312 basket weave (W) cloth 13. 3M AB-312 twill weave (W) cloth 14. HITCO Refrasil cloth (W) UC-100-48 15. Zircar Zironia cloth (W) ZFY-30A 16. FMI -Stevens Astroquartz (W) cloth crowfoot satin 17. 3M AB-312 twill weave (W) cloth coated with 3M coating 18. 3M AB-312 basket weave (W) cloth coated with 3M coating 19. 3M AB-312 twill weave (W) cloth Menarde coating 20. HITCO Refrasil cloth (W) UC-100-96 not heat cleaned 21 . Carborundum Fiberfrax (W) no insert wire L-126TT 22. HITCO Refrasil batt B100-1 Basis Weight g/m2 311 231 643 608 352 227 281 254 1249 1544 807 Permeability Percent Efficiency on cm3/s/cm 2 ft3/rain/ft2 0.3 urn OOP at cm/s 1.27 cm H20 at 0.5 in. W.C. 2.68 5.35 14.22 13.6 28.4 8.7 5.8 16.6 65.2 47.6 51.2 3.4 7.4 8.9 26.7 058 56.0 032 17.1 043 11.4 29 37 34 32.6 056 128.3 0 3 10 93.7 070 100.8 0 6 10 6.7 0 11 16 14.7 55 55 57 17.5 84 79 72 (F) ------- TABLE 18. Continued oo (W) Woven (P) Paper (F) Felt 23. HITCO Refrasil standard (W) not heat cleaned very thin UC-100-28 24. HITCO Irish Refrasil (W) chromized C-1554-48 25 . Carborundum Fiberf rax (P) paper (with binder) 970J 26. ICI Saffil Zirconia paper (P) (with binder) 27. Carborundum Fiberf rax (P) paper (no binder) 970-AH 28. 3M AB-312 double thick (W) plain weave 29. FMI crowfoot satin cloth (W) astroquartz 30. 3M AB-312 12 harness satin (W) weave 31. 630 Tuflex fiberglass* (W) 32. 15-011-020 woven filment* (W) polyester 33. 25-200-070 polyester felt* (F) Basis Permeability Percent Efficiency on Weight cm3/s/cm2 ft3/min/ft2 0.3 ym OOP at cm/s g/m 1.27 cm H20 at 0.5 in. H.C. 2.68 5.35 14.22 335 11.9 23.4 010 683 5.2 10.1 2 8 10 604 26.9 53.0 99.5 99.0 97.6 212 8.8 17.1 83 78 74 152 12.4 24.4 88 -- 73 1035 84.8 167.0 0 10 41 905 62.1 122.2 0 10 32 675 75.5 148.7 0 8 24 564 16.0 31.6 10 9 19 175 6.8 13.4 604 524 11.9 23.4 34 24 29 *These materials are conventional (not ceramic) media. ------- (Ensor, et al. 1976). For typical cleaning pulse frequencies, a bag may have to withstand a few million pulses in its lifetime. For this reason, blanket or felted ceramic fiber materials are expected to be the most promising. They combine good filtration properties with relatively high strength. The second drawback is the size of typical fabric filter installations. Most conventional fabric filters operate at super- ficial velocities in the range of 1 to 3 cm/s. Somewhat higher velocities up to 10 or 20 cm/s are possible with some felted fabrics although bag life will be shortened. In comparison, granular bed filters operate at superficial velocities from 40 to 80 cm/s. For a given gas flow rate, fabric filters will require from 4 to 20 times the surface area required by granular bed filters. This is especially important at high pressure where the cost of the pressure vessel can be a signifi- cant fraction of the capital cost. Both baghouses and GBFs will have to be designed so as to maximize the surface to volume ratio, These problems are being considered in the EPA-sponsored development program. Preliminary experience at high tempera- ture and pressure indicate that at least three configurations show promise, having survived 50,000 cleaning pulses at 815°C and 9 atm. Test conditions were as follows: Temperature - 815°C Pressure - 930 kPa (9 atm) Air-to-cloth-ratio - 5 to 1 (2.54 cm/s) Cleaning pulse pressure - 1,100 kPa Cleaning pulse interval - 10 s Cleaning pulse duration - 100 m/s Dust - redispersed fly ash The three filter media configurations tested were: 1. Saffil alumina mat contained between an inside and an outside layer of 304 stainless steel knit wire screen. 2. Woven Fiberfrax cloth with nichrome wire scrim insert. 3. Fiberfrax blanket contained between an inside and an 87 ------- outside cylinder of 304 SS square mesh screen similar to common window screen. The ceramic fiber blanket was held in position between the screens with 302 SS wire sewn between the screens. Pressure drop during the tests was controlled by rapid cleaning pulses and in general remained less than about 5 kPa (20 in.W.C.). Formation and removal of the filter cake for these configurations and test conditions presented no problems. The average outlet loading during the Fiberfrax blanket test was 0.0055 g/Nm3 (0.0024 gr/SCF). The fly ash dust dis- persion apparatus used was suitable for filter loading tests but may not be representative of the dust characteristics and size distribution to be encountered in a real application. In order to obtain test data in a real PFBC application, the Acurex ceramic baghouse is to be tested on a slipstream at the Exxon miniplant. Installation has begun and the test pro- gram is scheduled to start in late November, 1978. Membrane Filtration Several available ceramic materials in many configurations have been evaluated as possible high-temperature filters by Ciliberti (1977) and Poe, et al. (1977). One of the most promising materials tested was a ceramic cross flow monolith produced by 3M Company under the trade name of Thermacomb. This material is composed of alternate layers of corrugations separated by thin filtering barriers. This type of configuration affords a large amount of filter surface in a very small volume. Figure 29 shows a piece of this material and indicates the cross flow con- figuration. The material has an average pore size of 10 ym with a range as shown in Figure 30. The Thermacomb cross flow structure is made up of several layers in the following pattern: a thin (0.25 - 1.5 mm) porous cordierite sheet, a layer of cordierite corrugations similar in 88 ------- CLEAN GAS GAS FLOW Figure 29. 3M crossflow ceramic monolith. 89 ------- 100 80 UJ IS! in o o ex UH o 60 40 20 0 0.001 I I I 0.01 0.1 1.0 PORE DIAMETER (MICRONS) 10 100 Figure 30. Pore size distribution for Thermacomb ceramic fiber material (from Poe, et al., 1977). 90 ------- appearance to those used in cardboard, another flat sheet of cordierite followed by another layer of corrugations oriented 90° from the corrugations below. The presently available forms of the material have 1.97, 3.15 or 4.72 corrugations per cm. A similar material is manufactured by W.R. Grace § Company. This material has perpendicular dividers which given rectangular holes rather than the triangular holes seen in the Thermacomb. The Grace material tested had approximately 8.5 holes per cm and an equal number of layers per cm. These materials have many properties that make them attrac- tive as filters. Among these are (1) working temperature to 1,200°C, (2) very good mechanical strength despite thin separators, (3) excellent resistance to thermal shock, (4) excellent resis- tance to corrosive atmospheres and, (5) very high surface area to volume ratios. Ciliberti (1977) estimated that the Therma- comb material tested had 3.27 cm2 filter area per cm3 of element while the W.R. Grace § Company material had approximately 6.52 cm2 of usable area per cm3 of element. Cascade impactors were used to measure the size of the limestone test dust. The mass median diameter was typically 1.4 ym and the geometric standard deviation was 3.0. Results of the high temperature Thermacomb tests are pre- sented in Table 19. The overall collection efficiency averaged 96.4% with some tests showing 100% collection. No problems were encountered in cleaning the filter media by reverse pulses of compressed air. It was possible to clean the filter and return to a stable pressure drop even the relatively heavy dust loadings. Similar results were obtained in a limited number of tests on the W.R. Grace material. Although ceramic honeycomb filters operated successfully on limestone particulate in bench scale tests, there are a number of uncertainties regarding their application as tertiary cleanup devices. Further development work is needed to resolve the fol- lowing major questions. 91 ------- TABLE 19. SUMMARY OF HOT TESTS WITH 3M THERMACOMB (FROM CILIBERTI, 1977) Temperature, °C 815 750 720 360 520 710 700 680 690 680 695 680 660 650 700 630 620 615 Superficial Velocity cm/s 11.6 7.3 7.0 4.5 5.7 7.3 6.9 6.8 6.8 6.8 6.9 2.9 2.8 2.7 2.2 1.6 1.5 1.4 Inlet Concentration g/m3 1.2-2.2 1.8-2.1 8.4-12.0 3.6 5.2 4.5 2.7-7.9 2.6 3.8 3.2 5.4 0.05 0.11 0.11 1.1 0.06 0.12 0.08 Overall Efficiency, % 95.5 85.0 95.0 100.0 100.0 99.6 99.9 99.6 100.0 100.0 100.0 100.0 100.0 93.0 99.0 88.0 92.0 81.0 92 ------- 1. Are ceramic honeycombs susceptible to clogging with actual process particulate matter? 2. Can these filter media be redesigned or optimized with regard to particle collection, pressure drop, permeability? 3. What are the temperature and pressure losses associated with alternative cleaning methods? 4. How durable are these media over a prolonged high tem- perature and pressure run, and how serious are the pro- blems of erosion and degradation of the media ? 93 ------- HOT VERSUS COLD GAS CLEANUP INTRODUCTION Because of the technical and economic uncertainties associa- ted with high temperature and pressure particulate control, there is a possibility that the only practical approach to particulate removal which will allow for reasonable turbine life is low temperature, high pressure cleanup. In most cases, low temperature-high pressure gas cleaning equipment can be based on conventional technology. However, the specific design configurations for high pressure applications will generally be different than for low pressure applications. For example, tubular electrostatic precipitators are more suit- able than parallel plate designs for operation at high pressure. This is essentially a matter of packaging the precipitator in a pressure vessel. However, increased pressure increases pre- cipitation efficiency by reducing ion mobility and thereby enabling operation at higher electrical potential. Therefore particle collection should not present problems. Fabric filtration baghouses should operate adequately at high pressure. However the expense of high pressure housings may require special design to minimize the baghouse volume and maximize the superficial velocity (air-to-cloth ratio). Wet scrubbers can also be designed to work well at high pressure. However, large gas densities may require higher liquid-to-gas ratios, and in some configurations high pressure frictional losses may become more significant than in conven- tional applications. In general, low temperature-high pressure particulate control technology is feasible and to some extent commercially available. This is the major advantage to cold gas cleanup 94 ------- as 'Compared to hot gas cleanup. On the other hand, hot gas cleanup can achieve higher overall thermal efficiencies and therefore more efficient fuel usage. The relative process efficiencies for hot and cold gas cleanup depend on the specific process configuration. Hot ver- sus cold gas cleanup for pressurized fluidized bed combustion and low-BTU coal gasification processes are reviewed in this section. PRESSURIZED FLUIDIZED BED COAL COMBUSTION Klett, et al. (1977) carried out an analytical study to determine the performance penalties which accompany cold gas cleanup for representative pressurized fluidized bed combustion combined-cycle systems. They considered a cold gas cleanup cycle consisting of a recuperator followed by a baghouse or electrostatic precipitator. The PFBC boiler, air-cooled combus- tor, and adiabatic combustor designs were considered. The system parameters are listed in Table 20. PFB Boiler Process The G.E. 1,000 MW commercial scale combined-cycle design was used as a basis for the water cooled PFBC process. The system is illustrated in Figure 31. Water and steam pass through tubes in the bed to control bed temperature. Combustion is carried out with approximately 20% excess air and the combus- tion gas is cleanetd prior to entering the gas turbine. The proposed G.E. system cleans the combustion gas at high temperature ( 955°C ) using two stages of cyclone separation and a final gas cleanup stage. Klett, et al. (1977) also con- sidered cold gas cleanup with heat recovery. For all cases, the temperatures out of the bed were held constant at 955°C which are consistent with those chosen by G.E. for their pre- liminary base case. The tertiary cleanup device was a moving granular bed filter (GBF) . A pressure drop of 0.34 atm and a temperature drop of 14°C across the bed were assumed. A 1% mass flow loss due to medium recirculation and leakage was also assumed for the moving bed filter. 95 ------- TABLE 20. SYSTEM PARAMETERS FOR PFBC ANALYSIS (FROM KLETT, ET AL., 1977) vo PFBC Temperature (°C) PFBC Pressure (atm) Excess Air for Combustion (%) Gas Cleanup Temperature (°C) RHX Effectiveness Gas Turbine Inlet Temperature Steam Turbine Pressure/ Temperature (atm/°C) Steam Turbine Pressure/ Temperature (psia/°F) Stack Temperature (°C) Gas Turbine Electrical Output Steam Turbine Electrical Outpi Adiabatic (CPC-400 Hot Gas Cleanup 983 6.3 300 969 N/A (°C) 933 31.6/426- 7.14/204 465/800- 105/400 163 (MW) 12.5 it 7.4 Combustor System) Cold Gas Cleanup 983 6.3 300 316 0.80 802 31.6/426- 70 14/204 465/800- 105/450 133 9.7 7.8 Air Cooled Combustor (Curtiss -Wright System) Hot Gas Cleanup 899 6.9 33 899 N/A 916 54.4/440 800/825 149 304 190 Cold Gas Cleanup 899 6.9 33 316 0.80 864 54.4/440 800/825 149 280 194 Water Cooled (GE CFCC Hot Gas Cleanup 955 10 20 955 N/A 926 238/538/538 Combustor System) Cold Gas Cleanup 955 10 20 316 0.80 814 238/538/538 3500/1000/1000 3500/1000/1000 149 222 731 149 174 768 (MW) ------- T - TEMPERATURE, F P - PRESSURE, PSIA AIR IN 59T 14.7P COMP. 147P 667T 4358P FEED WATER FURB. 1700T PFBC J2 STAGE — CYCLONE 17OTT 1000T 574P 1003T 3575P 926T TO STACK 0.98P Figure 31a. Pressurized fluidized bed/combined cycle system, water cooled combustor with hot gas cleanup. ------- 00 T - TEMPERATURE, F P - PRESSURE, PSIA 810T AIR IN 59T 14.7P COMPR 147P FEED WATER TURB. TO STACK 1500T PFBC RECUP. HEAT EXCHANGER 1750T 1725T 837T 1003T 3575P Figure 31b. Pressurized fluidized bed/combined cycle steam, water cooled combustor with cold gas cleanup. ------- The cold gas cleanup system used a pressurized baghouse, in conjunction with a gas/gas recuperative heat exchanger. An effec- tiveness of 80% and a pressure drop of 76 cm W.C. per side were assumed for the heat exchanger. These values are consistent with those found on gas/air heat exchangers used on regenerative gas turbines in electric power generation service. Effectiveness ranges for various commerically available recuperative heat ex- changer designs are given in Table 21. The heat removed from the cleanup stream prior to reentering the recuperator was recovered in a bottoming cycle auxiliary econo- mizer. The baghouse filter inlet temperature was set at 316°C based on design limitations for available material. The results are presented in Table 22. Air-Cooled PFBC Process The air-cooled PFBC analysis was based on the Curtiss-Wright 500 MW combined cycle system. This system is illustrated in Figure 32. Approximately two-thirds of the total gas flow is passed as cooling air through tubes in the combustor bed to control the bed temperature. Combustion is carried out with approximately 33% excess air. The combustion gas is cleaned and mixed with the heated air prior to entering the combustion turbine. The proposed Curtiss-Wright system cleans the combustion gas at high temperature (899°C) using two stages of Aerodyne rotary flow cyclones. Klett, et al. considered alternative hot gas cleanup systems as well as cold gas cleanup with heat recovery. For all cases, the temperature out of the bypass air heat exchanger was held constant at 856°C. The alternative hot gas cleanup method studied was a gravel bed filter (GBF). Two types of GBF were considered: fixed bed and moving bed. For both filters, a pressure drop of 34.5 kPa (5 psij and a temperature drop of 14°C across the bed were assumed. A 1% flow loss due to media recirculation and leakage was assumed for the moving bed filter. A 0.25% flow leakage was assumed for the fixed bed filter. 99 ------- TABLE 21. EFFECTIVENESS RANGES FOR RECUPERATIVE HEAT EXCHANGERS Heat Exchanger Type Effectiveness* Shell $ Tube 48-57.5% Single Pass Shell § Tube 60-73% Double Pass Shell § Tube 81-83% Three Pass Rotary (Heat Wheel) 75-80% (3 or 4 units) *Effectiveness is the percentage of available temperature differential recovered. 100 ------- TABLE 22. PERFORMANCE OF PFBC PROCESSES WITH HOT AND COLD GAS CLEANUP (FROM KLETT, ET AL., 1977) Process Configuration I. PFB Boiler A. Hot Gas Cleaning 1. Moving GBF B. Cold Gas Cleanup 1 . Pressurized baghouse II. Air-Cooled PFBC A. Hot Gas Cleanup 1. Two stages Aerodyne cyclones 2. Moving GBF 3. Fixed GBF B. Cold Gas Cleanup 1. Baghouse/low pressure heat 2 . Baghouse/high pressure heat recove II. Adiabatic PFBC A. Hot Gas Cleanup 1. Moving GBF B. Cold Gas Cleanup 1. Baghouse high pressure steam with heat recovery Gas Turbine Inlet Temp.°C 926 814 871 866 867 828 ry 828 932 802 Thermodynamic Efficiency, % 40.6 39.6 38.8 37.1 37.3 35.5 36.0 37.1 32.6 Heat Rate, BTU/kW-hr 8,399 8,624 8,805 9,200 9,154 9,621 9,476 9,203 10,450 Net Power MW 953 942 458.1 435.4 440.7 419.3 425.7 19.9 17.5 101 ------- AIR IN o txj T - TEMPERATURE, F P - PRESSURE, PSIA Figure 32a. Curtiss-Wright pressurized fluidized bed/combined cycle system, hot gas cleanup with aerodyne cyclones. ------- AIR IN T - TEMPERATURE, F P - PRESSURE, PSIA Figure 32b. Curtiss-Wright pressurized fluidized bed/combined cycle system cold gas cleanup system with heat recovery. ------- A baghouse, in conjunction with a gas/gas recuperative heat exchanger, was considered for cold gas cleanup. As with the preceding study, an effectiveness of 80% and pressure drops of 76 cm W.C. per side were assumed for the heat exchanger. The heat removed from the cleanup stream prior to reentering the recupera- tor was used to generate additional steam. in one system, a second low pressure evaporator was added to recover the heat. In a second system, the heat was recovered by adding a high pressure econo- mizer . The results are presented in Table 22. Adiabatic PFBC Process The Combustion Power Company's adiabatic PFBC system was used as the basis for the adiabatic process. The system incor- porates a moving bed granular bed filter (GBF) for high tem- perature cleanup of the combustion gas prior to entering the gas turbine. The system is illustrated in Figure 33. The cold gas cleanup method was a baghouse with fiberglass filters. A pressure drop of 13 cmW»C. through the baghouse was assumed. The maximum operating temperature of the baghouse is about 315°C (600°F). The combustion gas was cooled by means of a gas/gas heat exchanger which was added to the system ahead of the baghouse. The heat exchanger effectiveness and pressure drop per side were assumed to be 80% and 76 cm W0C. The results are presented in Table 22. The efficiency loss between hot and cold gas cleanup is greatest for the adiabatic combustor configuration, since all the working fluid passes through the bed and therefore must be cooled and cleaned. Future equipment, capable of handling higher product gas temperature, could reduce the performance penalties associated with cold gas cleanup and probably justify the additional hard- ware complexity. The systems using air and water cooled combustors appear to be capable of using current cold gas cleanup techniques with fairly small system performance penalties (1 to 2%). The Phase II EGAS studies (Lewis Research Center, 1977 and General Electric 104 ------- AIR IN o tn DUAL ADMISSION STEAM TURBINE FUEL IN Figure 33a. Pressurized fluidized bed combustion system with dual admission steam turbine. ------- 269T AIR IN 872T FUEL IN ASH 1 - 802' GEN. r f f 'HP ' HIGI SUPHTF If "^ V T r»i*r PRES. rEVAP. 1 3. HIGH PRES. * — FTHM * — 550P 0 A > P - PRESSURE, PSIA T - TEMPERATURE, F E Figure 33b. Pressurized fluidized bed combustion system with dual admission steam turbine cold gas cleanup - low pressure evaporator added for heat recovery. DUAL ADMISSION STEAM TURBINE ------- Company 1976) showed the PFBC boiler process with hot gas clean- up to have a 7% thermal efficiency advantage over conventional coal-fired boilers with wet scrubbers for SO control. J\. In order to fully assess the cold cleanup alternatives, recuperative heat exchangers must be studied more closely, es- pecially regarding effectiveness, availability and cost for high temperature and pressure applications. Further economic evaluation of hot versus cold gas cleanup must consider the cost and effectiveness of high temperature-high pressure and low temperature-high pressure particulate control devices, recuperator performance and cost, and the specific par- ticulate control requirements. Much more development work is required to provide this information. Post-Turbine Particulate Control If gas turbines can be developed which have relatively high tolerance for fine (<5 ym) particles, then it may be fea- sible to use conventional cyclones and multiclones to protect the turbine. In such cases the emissions regulations would have to be met by applying conventional particulate control equipment downstream from the gas turbine. Using the Westinghouse EGAS Phase II PFBC design (Beecher, et al. 1976), each gas turbine would handle 345 kg/s of gas flow. At a stack temperature of 150°C, this would correspond to 24,900 m3/min (879,000 ACFM) of gas to be controlled. Data from the Exxon miniplant indicate that about 0.23 to 2.3 g/Nm3 (0.1 to 1.0 gr/SCF) of particulate matter penetrates the second stage cyclone. The proposed New Source Performance Standard for coal-fired boilers of 0.05 lb/106BTU corresponds to about 0.046 g/Nm3 (0.025gr/SCF) for the Exxon system. There- fore collection efficiencies of 80 to 98% may be required down- stream from the turbine. The estimating curves presented by Neveril, et al. (1978) were used to estimate the cost of electrostatic precipitators with design efficiencies of 80, 90, 95, and 98%. Typical effec- tive migration velocities (precipitation rate parameters) of 9 and!2 cm/s (0.3 and 0.4 ft/s) were assumed for these predictions. 107 ------- The results are shown in Table 23, along with the costs for high temperature and pressure particulate control equipment reported by Beecher, et al. All prices have been adjusted to mid-1978 dollars using the Marshall and Stevens equipment cost index. When interpreting Table 23 it should be remembered that the granular bed filter costs are highly speculative in that they are based on an unproven technology at high temperature and pressure. Also the electrostatic precipitator costs assume that there are no problems with using standard cold-side designs for this appli- cation. High resistivity problems necessitating hot-side electro- static precipitation will cause the estimated costs to increase by a factor of two or more. The cost of post-turbine cleanup equipment is noticeably less expensive than hot gas cleanup. However, the post-turbine equip- ment costs are significant and must be considered in the overall capital cost for gas cleaning equipment. Any economic advantages associated with using post-turbine cleanup very likely will depend on the cost and availability of gas turbines which can tolerate relatively heavy loadings of fine particulate matter. LOW-BTU COAL GASIFICATION PROCESSES The incentives for hot gas cleanup in coal gasification pro- cesses are different than for PFBC processes. The major differences are: 1. The available sensible heat in the coal gas is only about 20% or less of the total energy available from the gas. Therefore heat transfer inefficiencies associated with the cold gas cleanup approach are less severe. 2. Maximum turbine inlet temperature is assured because of the heat released by combustion of the gas. 3. High temperature particulate removal is coupled to hot H2S removal. There is little incentive for hot particulate removal if the gas must be cooled for HZS removal. 108 ------- TABLE 23. COMPARISON BETWEEN PRE-TURBINE AND POST-TURBINE EQUIPMENT COST CONTROL DEVICE (Number per Turbine) A. HOT GAS CLEANUP:* 1. Primary Cyclones (8) 2. Multiclones (2), including bleed lines 3. Granular Bed Filters (8) TOTAL ESTIMATED MAJOR COMPONENT COST PER TURBINE, $ 1,140,000 2,360,000 2,980,000 B. POST-TURBINE CLEANUP: Electrostatic Precipitators : (Cold Side) 1. 80% collection 2. 901 collection 3. 95% collection 4. 98% collection Migration Velocity 9 cm/s 12 cm/s 400,000 500,000 530,000 630,000 640,000 750,000 750,000 960,000 *From Beecher, et al. (1976) converted to mid-1978 dollars. 109 ------- 4. In some processes quenching is required to remove tars. The presence of tars can plug hot gas cleanup devices unless the tars can be prevented from condensing. Quenching loses the gas sensible heat and the heating value of the tars which can be as much as 20% of the total heating value of the fuel (MERC, 1978). Also tar disposal or recovery from the scrubber liquor can present problems. Hot gas cleanup which enables the tars to be burnt in the gas turbine combustor is highly desirable. Jones and Donohue (1977) reported on a comparative evalua- tion of high and low temperature gas cleaning for coal gasifica- tion combinedrcycle power systems. They were concerned primarily with hot H2S removal and for the purposes of their evaluation they assumed that suitable high temperature and pressure parti- culate control equipment would be developed. However, they noted that it is impossible to develop better than rough cost estimates for hot gas cleanup equipment at the current state of development. Process evaluations were performed for five different coal gasification schemes. 1. Air blown, dry ash, moving bed gasifiers (Lurgi) 2. Oxygen blown, dry ash, moving bed gasifiers (Lurgi) 3. Oxygen blown, slagging, moving bed gasifier (British Gas Corporation) 4. Oxygen blown, two-stage entrained bed gasifier (Foster-Wheeler) 5. Air blown, two-stage entrained bed gasifier (Foster-Wheeler) The air blown systems and the oxygen blown slagging gasifier system are illustrated in Figures 34, 35 and 36. The Morgantown iron oxide system was used for hot HaS removal. The CCNY (Squires) granular bed filter system was used for hot particulate control. Cold HaS removal was achieved using the proprietary Benfield pro- cess. Wet scrubbers were used for low temperature particulate removal. The results of their study are summarized in Table 24. It appears that the greatest thermal benefits are to be derived from applying hot gas purification to Lurgi gasifiers. It is 110 ------- TABLE 24. SUMMARY OF ESTIMATED THERMAL EFFICIENCIES FOR HOT VERSUS COLD GAS CLEANUP IN COAL GASIFICATION PROCESSES (FROM JONES AND DONOHUE, 1977) PURIFICATION COLD GAS CLEANUP HOT GAS CLEANUP COLD GAS CLEANUP HOT GAS CLEANUP Gas Turbine Inlet Temperature, °C Lurgi (02) 1,063 1,063 1,315 Thermal Efficiency, %* Heat Rate, BTU/kW-hr 1,315 Thermal Eff. Heat Rate Lurgi (Air) Thermal Eff. Heat Rate Slagging (02) Thermal Eff. Heat Rate Entrained Bed (Air)** Thermal Eff. Heat Rate Entrained Bed (02)** Thermal Eff. Heat Rate 29.4 11,628 31.0 10,994 36.5 9,352 38.0 8,982 35.4 9,641 35.4 9,630 37.0 9,223 37.5 9,095 38.4 8,879 36.6 9,334 32.4 10,544 34.5 9,907 39.6 8,624 40.8 8,359 37.8 9,028 39.9 8,558 41.2 8,285 40.6 8,409 41.6 8,215 39.3 8,688 'Thermal Efficiency (%) » (Delivered kW) (3412.75) (100) (Coal Ib/hr) (Coal HHV BTU/lb) **Foster Wheeler Gasifier. The notation Air or Og indicates the oxidant employed in each type of coal gasifier. Ill ------- BENFIELD H2S REMOVAL PLANT ts) COAL • H2S ABSORBER H2S STRIP .LP STN BENFIELD SOL'N SULFUR RESATURATOR QUENCH SCRUBBER / V STACK WATER TREATMENT GAS TURBINE HEAT RECOVERY NAPHTHA OILS,PHENOLS ^ COMPRESSOR NHs STEAM SOL'N TURBINE AIR Figure 34a. Lurgi air blow gasifier - cold purification case. ------- COAL AIR MP STM COMPRESSOR REMOVAL REMOVAL REGENERATION SULFUR TURBINES STACK Figure 34b. Lurgi air blown gasifier study - hot purification case. ------- BENFIELD H2S REMOVAL PLANT COAL TRANSPORT GAS MP STEAM GLAUS PLANT OFFGAS TO BOILER SULFUR WATER PLANT 1 20% AMMONIA SOLUTION AIR & STEAM TURBINES j COMPRESSOR ^> TRANSPORT GAS TO GASIFIER Figure 35a. Air blown entrained bed gasifier study - cold purification case. ------- ENTRAINED PARTICLE REMOVAL AIR COAL BED GASIFIER COMBUSTOR COMPRESSOR BFW HOT IRON OXIDE H2S REMOVAL TRANSPORT GAS, CHAR HOPPER TURBINE GUARD FILTER REDUCING GAS HEAT RECOVERS SLAG COMPRESSOR STEAM TURBINES IRON OXIDE REGEN. CYCLE RECYCLE SYSTEM OXYGEN PLANT MP STM Figure 35b. Air blown entrained bed gasifier study - hot purification case. ------- BENFIELD H2S REMOVAL PLANT COAL MP STEAM STEAM TURBINES Figure 36a. Slagging gasification study - cold purification case. ------- AIR MP STM J COMPRESSOR HOT IRON PARTICLE OXIDE BTIIB PAC REMOVAL H,S REMOVAL FLUE GAS «~ 2 STACK STE/ TURBINES Figure 36b. Slagging gasification study - hot purification case. ------- important to remember that the underlying assumption used for these cases is that tars will pass uncondensed through the hot iron oxide beds directly into the gas turbine combustor. For all cases other than the Lurgi dry ash gasifiers, thermal efficiency advantages associated with hot gas cleanup appear to be marginal (1 to 2%). The Phase II EGAS studies (Lewis Research Center, 1977 and General Electric Co., 1976) showed the LBCG combined-cycle system to have a 7% advantage over conventional coal-fired boilers with stack gas scrubbing for SO control. JC There are two major reasons why high temperature purifi cation proved to be of such benefit to the Lurgi systems and of little advantage to the other gasification systems studied: 1. The Lurgi gasifiers were the only systems considered to have a net production of tars. Tars produced by the BGC slag- ger were separated from the gas stream prior to desulfurization and were recycled to extinction to the gasifier. Tars were considered to be absent in the crude gas from the entrained gasifier. The presence of tars in a crude fuel gas has major impact on the com- parison between high and low temperature cleaning schemes. For the high temperature case, tars are assumed to pass through the iron oxide system and are converted to electricity at combined- cycle efficiency, (40-50%). With low temperature cleaning systems, tars are scrubbed from the crude gas by direct quench and are eventually converted to electricity at only the steam cycle effi- ciency, (30-40%) . 2. The Lurgi gasifiers consume large quantities of steam to prevent ash matter from clinkering in the bottom. Most of this steam passes through the gasifier unconverted and is condensed in the gas quench operation necessary for low temperature gas cleaning. Therefore, if a quench is necessary, most of the sen- sible heat in the steam is unavailable for power generation. If high temperature desulfurization is employed, the steam passes through the iron oxide beds, and its sensible heat is converted into electricity in the combined-cycle plant. 118 ------- The BGC slagger required only 13% of the steam required by the dry ash oxygen blown Lurgi gasifier due to the higher bottom temperature required for ash slagging. It also converts approximately 901 of the gasifier steam to hydrogen and carbon monoxide. Therefore, steam losses due to cooling of the slagging gasifier effluent in the quench operation are negligibly small. Steam consumed by both the air and oxygen blown entrained gasifier is approximately the same as that consumed by the slag- ger resulting in the same negligibly small steam losses on gas cooling. Thermal efficiency advantages for hot gas cleanup may be even lower than predicted if satisfactory high temperature particulate removal cannot be achieved without significant temperature and pressure losses. Also both HTP H2S and particulate removal systems are required. Therefore technology development needs may be greater than for combustion processes. Existing technology is capable of satisfying cold gas cleanup needs. This should be sufficient for first generation LBCG processes. The development of HTP particulate and HaS removal systems may be helpful in improving the performance of second generation systems. HTP control equipment also will make the fixed or moving bed processes more economically competitive by enabling the conversion of sensible heat and tar heating value into electri- cal energy at combined-cycle efficiency. 119 ------- REFERENCES Beecher, D., et al. Energy Conversion Alternatives Study (EGAS). Westinghouse Phase II Final Report, Volume III. Summary and Advanced Steam Plant with Pressurized Fluidized Bed Boilers. NASA CR-134942, NSF/RA-760590, NTIS PB 268-558. November, 1976. Bertrand, R.R., et al. A Regenerative Limestone Process for Fluidized Bed Coal Combustion and Desulfurization. Monthly Report Nos. 101-103 on EPA Contract No.68-02-1312. July-Sept. 1978. Bertrand, R.R., et al. Shakedown and Operation of Fluidized Bed Combustion Miniplant. Monthly Report No. 93, EPA Contract No. 68-02-1312. November,1977. Billings, C.E., and J.E. Wilder. Handbook of Fabric Filter Technology. EPA APRD 0690. NTIS PB 200-648. December, 1970. Billings, C.E., W.D. Small and L. Silverman. Pilot-Plant Studies of a Continuous Slag-Wool Filter for Open-Hearth Fume- J. APCA, Vol. 5, No. 3, p. 159, November, 1955. Brown, R.F., and A.B. Walker. Feasibility Demonstration of Electrostatic Precipitation at 1,700°F. J. APCA, Vol. 21, No. 10, p. 617, 1971. Bush, J.R., P.L. Feldman, and M. Robinson. Development of a High Temperature/High Pressure Electrostatic Precipitator. EPA 600/7-77-132. NTIS PB 276-626/9BE. November, 1977. Calvert, S. R.G. Patterson, and D.C. Drehmel. Fine Particle Collection in the A.P.T. Dry Scrubber. Proceedings of the EPA/DOE Symposium on High Temperature/High Pressure Parti- culate Control. EPA 600/9-78-004. September, 1977. Calvert, S., et al. Scrubber Handbook. EPA R2-72-118a. NTIS PB 213-016. August, 1972. Ciliberti, D.F. High-Temperature Particulate Control with Ceramic Filters. EPA 600/2-77-207. NTIS PB 274-485/2BE. October, 1977. Ciliberti, D.F. and B.W. Lancaster. An Improvement of the Simple Method for Rotary Flow Cyclones. AIChE J., Vol. 22, No. 6, p. 1150. November, 1976. 120 ------- REFERENCES,,continued Ciliberti, D.F., and B.W. Lancaster. Performance of Rotary Flow Cyclones. AIChE J. Vol. 22, No. 2, p. 394. March, 1976. Davies, C.N. Air Filtration. Academic Press, New York, 1973. Ensor, D.S., et al. Determination of the Fractional Efficiency, Opacity Characteristics, Engineering and Economic Aspects of a Fabric Filter Operating on a Utility Boiler. EPRI FP-297. November, 1976. Fedarko, W., A. Gatti, and L.R. McCreight. High Temperature Glass Entrainment of Fly Ash. Presented at the Symposium on the Transfer and Utilization of Particulate Control Technology, Denver, Colorado. July, 1978. Feldman, P., J. Bush and M. Robinson. High Temperature, High Pressure Electrostatic Precipitation. Presented at the Symposium on the Transfer and Utilization of Particulate Control Technology, Denver, Colorado. July, 1978. First, M.W-, et al. High Temperature Dust Filtration. Industrial and Engineering Chemistry. Vol. 48, No. 4, p. 696. 1956. General Electric Co. Energy Conversion Alternatives Study (EGAS) Phase II Final Report. Vol I and II. NASA-CR-134949. NTIS PB 268-466, 268-379, 268-350, 268-467. December, 1976. Hoke, R.C., et al. Miniplant Studies of Pressurized Fluidized Bed Coal Combustion: Third Annual Report. EPA 600/7-78-069. April 1978. Jones, C.H. and J.M. Donohue. Comparative Evaluation of High and Low Temperature Gas Cleaning for Coal Gasification- Combined Cycle Power Systems. EPRI AF-416. April, 1977. Kalen, B., and F. A. Zenz. Filtering Effluent from a Cat Cracker. Chemical Engineering Progress. Vol. 69, No. 5, p. 67. June, 1973. Kane, L.J., G.E. Chidester, and C.C. Shale. Ceramic Fibers for Filtering Dust from Hot Gases. Bureau of Mines, Report of Investigation No. 5672, 1960. Keairns, D.L., et al. Fluidized Bed Combustion Process Evaluation Phase II: Pressurized Fluidized Bed Coal Combustion Develop- ment. EPA 650/2-75-027c. NTIS PB 246-116. September, 1975. Klett, M.G,, N. Szwab, and J.P. Clark. Particulate Control for Pressurized Fluidized Bed Combustion. FE-2220-16. Jan. 1977. 121 ------- REFERENCES, continued Koller, L.R. and H.A. Fremont. Negative Wire Corona at High Temperature and Pressure. J. of Applied Physics, Vol. 21, p. 741. 1950. Lee, K.C., et al. Panel Bed Filter. EPRI-AF-560, 1977. Lewis Research Center (NASA). Evaluation of Phase II Conceptual Designs and Implementation Assessment Resulting from the Energy Conversion Alternatives Study (EGAS). NASA TMX- 73515, NSF/RA-770133. NTIS PB 270-017. April, 1977. Lewis Research Center (NASA). Comparative Evaluation of Phase I Results from the Energy Conversion Alternatives Study (EGAS). NASA TM-X-71555. NTIS N76-20631. February, 1976. Lundgren, D.A. and T.C. Gunderson. Filtration Characteristics of Glass Fiber Filter Media at Elevated Temperatures. EPA 600/2-76-192. July, 1976. McCabe, J.T. Cyclocentrifuge Development for Particulate Control; Phase I: Feasibility Study. Proceedings of EPA/DOE Sympo- sium on High Temperature/High Pressure Particulate Control. EPA 600/9-78-004. September, 1977. McCain, J.D. Evaluation of Rexnord Gravel Bed Filter. EPA 600/2-76-164. NTIS PB 255-095. June, 1976. McCreight, L.R., et al. Hot Gas Cleanup by Particle Entrainment in Coal Slag Based Glasses. Proceedings of EPA/DOE Symposium on High Temperature/High Pressure Particulate Control. EPA 600/9-78-004. September, 1977. Moore, R.H., et al. Molten Salt Scrubbing for Removal of Parti- cles and Sulfur from Producer Gas. Proceedings of EPA/DOE Symposium on High Temperature/High Pressure Particulate Control. EPA 600/9-78-004. September, 1977. Morgantown Energy Research Center. MERC Hot Gas Cleanup Task Force. Chemistry of Hot Gas Cleanup in Gasification and Combustion. MERC/SP-78/2. February 1978. Neveril, R.B., J.V. Price and K. L. Engdahl. Capital and Opera- ting Costs of Selected Air Pollution Control Systems. I-IV. J. APCA. Vol. 28, No. 8-11. Aug-Nov., 1978. Oglesby, S. and G.B. Nichols. A Manual of Electrostatic Preci- pitator Technology, Part I and II. NTIS PB 196-380. August, 1970. Parent, J.D. Efficiency of Small Cyclones as a Function of Loading, Temperature and Pressure Drop. Transactions of the AIChE. Vol. 42, p. 989, 1946. 122 ------- REFERENCES, continued Parker, R.D. and S. Calvert. High Temperature and High Pressure Particulate Control Requirements. EPA 600/7-77-071. NTIS PB 271-699/1WP. July, 1977. Patterson, R.G., S. Calvert and B.C. Drehmel. A.P.T. Dry Scrubber for Particle Collection at High Temperature and Pressure. Presented at the Symposium on the Transfer and Utilization of Particulate Control Technology. Denver, Colorado. July, 1978. Pich, J. Theory of Aerosol Filtration by Fibrous and Membrane Filters. In Aerosol Science, C.N. Davies, ed. Academic Press, New York, 1966. Poe, G.G., et al. Evaluation of Melten Scrubbing for Fine Particulate Control. EPA 600/2-77-067. NTIS PB 266-092. March, 1977. Poe, G.G., et al. Evaluation of Ceramic Filters for High Temperature/ High Pressure Fine Particulate Control. EPA 600/2-77-056. NTIS PB 266-093. February, 1977. Robinson, M. Electrostatic Precipitation at High Temperature and Pressure: Capabilities, Curiosities and Questions. Presented at the Symposium on the Transfer and Utilization of Particulate Control Technology, Denver, Colorado. July, 1978. Shackleton, M.A., and D.C. Drehmel. Barrier Filtration for HTHP Particulate Control. Presented at the Symposium on the Transfer and Utilization of Particulate Control Tech- nology, Denver, Colorado. July, 1978. Shackleton, M.A. and D.C. Drehmel. High Temperature Filtration. Proceedings of the Particulate Control Workshop, Julich, West Germany. March, 1978. Shackleton, M. and J. Kennedy. Ceramic Fabric Filtration at High Temperature and Pressure. Proceedings of EPA/DOE Symposium on High Temperature/High Pressure Particulate Control. EPA 600/9-78-004. September, 1977. Shale, C.C. and G.E. Fasching. Operating Characteristics of a High Temperature Electrostatic Precipitator. Bureau of Mines, Report of Investigation No. 7276, July, 1969. Silverman, L. and R.A. Davidson. High Temperature Filtering Medium. U.S. Patent No. 2,758,671. August, 1956. 123 ------- REFERENCES, continued Silverman, L. Method and Apparatus for Forming and Utilizing a Filter Medium. U.S. Patent No. 3,063,216. November, 1962. Stern, A.C. Air Pollution, 3rd edition. Volume 4: Engineering Control of "Air Pollution. Academic Press, New York, 1977. Sverdrup, E.F., D.H. Archer and M. Menguturk. The Tolerances of Large Gas Turbines to Rocks, Dusts and Chemical Corro- dents. Proceedings of the EPA/DOE Symposium on High Tem- perature/High Pressure Particulate Control. EPA 600/9-78-004 September,. 1977. Thomas, J.B. and E. Wong. Experimental Study of DC Corona at High Temperatures and Pressure. J. Applied Physics. Vol. 29, No. 8, p. 1,226. 1958. Wade, G., et al. Granular Bed Filter Development Program: Final Report. CPC Report to DOE. FE-2579-19, April, 1978. Westinghouse Electric Corp. Clean Power Generation from Coal. OCR 84. NTIS PB 234-188. April, 1974. Yellott, J.I. and P.R. Broadley. Fly Ash Separators for High Pressures and Temperatures. Ind. § Eng. Chemistry. Vol. 47, No. 5, p. 944. 1955. Yung, S.C., S. Calvert and H.F. Barbarika. Venturi Scrubber Performance Model. EPA 600/2-77-172. PB 271-515/9BE. August, 1977. Yung, S.C., et al. Granular Bed Filter for Particle Collection at High Temperature and Pressure. Proceedings of EPA/DOE Symposium on High Temperature High/Pressure Particulate Control. EPA 600/9-78-004. September, 1977. Yung, S.C., et al. Granular Bed Filters for Particulate Removal at High Temperature and Pressure. Presented at the Fifth International Conference on, Fluidized Bed Combustion. Washington, D.C. December, 1977. Yung, S. C., et al. A Granular Bed Filter Systems Study. EPA No.-600/7-79-020, January 1979. 124 ------- TECHNICAL REPORT DATA (Please read Instructions on the reverse before completing) 1. REPORT NO. EPA-600/7-79-019 2. 3. RECIPIENT'S ACCESSION NO. 4. TITLE AND SUBTITLE Alternatives for High-temperature/High-pressure Particulate Control 5. REPORT DATE January 1979 6. PERFORMING ORGANIZATION CODE 7. AUTHOR(S) Richard Parker and Seymour Calvert 8. PERFORMING ORGANIZATION REPORT NO. 9. PERFORMING ORGANIZATION NAME AND ADDRESS Air Pollution Technology, Inc. 4901 Morena Boulevard, Suite 402 San Diego, California 92117 10. PROGRAM ELEMENT NO. 1NE624 11. CONTRACT/GRANT NO. 68-02-2190 12. SPONSORING AGENCY NAME AND ADDRESS EPA, Office of Research and Development Industrial Environmental Research Laboratory Research Triangle Park, NC 27711 13. TYPE OF REPORT AND PER Final; 10/77 - 10/78 ERIOD COVERED 14. SPONSORING AGENCY CODE EPA/600/13 15. SUPPLEMENTARY NOTES EERL-RTP project officer is Dennis C. Drehmel, MD-61, 919/541- 2925. 16. ABSTRACT The report gjves tne status of the most promising high-temperature/high- pressure (HTP) particulate control devices being developed. Data are presented and anticipated performance and development problems are discussed. HTP particulate control offers efficiency and potential economic advantages over cold gas cleanup in pressurized fluidized-bed combustion (PFBC) and low-Btu coal gasification (LBCG) combined-cycle power generation systems. However, considerably more develop- ment will be necessary in order to demonstrate the technical and economic feasi- bility of HTP gas cleanup commercially. The alternative of recuperative heat ex- change coupled with low-temperature/high-pressure particulate control is reviewed with regard to power system efficiencies for PFBC and LBCG combined-cycle pro- cesses . Successful hot gas cleanup has clear efficiency advantages (1-7%) over cold gas cleanup. The economics of hot gas cleanup, however, are very speculative at the current state of development. 17. KEY WORDS AND DOCUMENT ANALYSIS DESCRIPTORS b.lDENTIFIERS/OPEN ENDED TERMS C. COS AT I Field/Group Pollution Coal Gasification Dust Gas Scrubbing High Temperature Tests High Pressure Tests Combustion Fluidized Bed Pro- cess ins; Pollution Control Stationary Sources Particulate High Temperature/ Pressure Control Gas Cleanup Combined-cycle systems 13B 11G 14B 21B 13H.07A 18. DISTRIBUTION STATEMENT Unlimited 19. SECURITY CLASS (ThisReport) Unclassified 21. NO. OF PAGES 155 20. SECURITY CLASS (Thispage) Unclassified 22. PRICE EPA Form 2220-1 (9-73) 125 ------- |