Resources and Conservation, 6 (1981) 117-136 Elsevier Scientific Publishing Company, Amsterdam -

Printed in The Netherlands

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A REVIEW OF BIOCONVERSION SYSTEMS FOR ENERGY FROM MUNICIPAL SOLID WASTE PART II: FUEL GAS PRODUCTION

RECOVERY

D.L. WISE, R.G. KISPERT and E.W. LANGTON Dynatech R/D Company, Cambridge, Massachusetts 02139 (U.S.A.)

(Received 27th October, 1980; accepted in revised form 5th April, 1981)

ABSTRACT A review was made of the use of anaerobic digestion processing techniques to produce fuel gas from municipal solid waste (MSW). The objective was to provide insight into current status and research needs. The MSW bioconversion processes reviewed were a) conventional anaerobic digestion, b) uncontrolled landfill gas recovery, and c) enhanced or controlled landfill gas recovery. It appears from this review that emphasis should be placed on improved technology for enhancing methane recovery from landfills as an apparently practical way to recover energy from MSW. This technology appears to have substantially greater potential than continued efforts to process MSW using conventional sludge digestion technology.

INTRODUCTION

The purpose of this paper is to review advances in bioconversion processes to produce methane from municipal solid waste, including research using MSW as the primary feedstock and other processes. The background of conventional and novel processes to produce methane is presented, also of processes to upgrade the gas. The status of pretreatment technology, which is applicable to some digestion processes, has been reviewed in Part I [ 11. Bioconversion of municipal solid waste for the production of methane includes four major elements: pretreatment, digestion, gas purification, and residue treatment, Pretreatment of the solid waste is desirable to separate out inorganic matter and materials which disrupt mechanical operation of the digester and to increase the biodegradability of the substrate. The digestion process results in the decomposition of organic matter and production of gas. The gas produced is purified by removing carbon dioxide, leaving pipeline quality methane gas for the commercial market. The undigested residue is dewatered and disposed of in a landfill or incinerator, or possibly used as a soil conditioner. A conceptual process design of an anaerobic digestion system developed in 1974 [ 21 is generally accepted as the baseline configuration for bioconver-

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sion of municipal solid waste and sewage sludge to produce methane. This anaerobic digestion system is summarized below and serves here as the example of conventional digestion.
PRETREATMENT

Refuse is prepared for digestion by size reduction and classification. Size reduction fulfills two primary functions: 1) to enable more efficient separation of organic materials from inorganic matter found in municipal waste, and 2) to allow the feed to solubilize more readily during digestion. Classification of the refuse by either wet or dry separation processes provides the feedstock with a high concentration of digestible matter, relatively free of metals, glass and grit. The dry separation processes offer the advantage of flexibility in selecting the desired water content of the feed to the digesters. Wet separation processes necessarily operate at low solids concentrations in aqueous slurries, and hence have the disadvantage of requiring a dewatering step whenever a concentrated feed to the digesters is desired. Digestion Before entering the digesters, the organic feedstock is mixed with nutrients and control chemicals. The nutrients are supplied by raw sewage sludge. Lime and ferrous salts are added for pH and hydrogen sulfide control. Dilution water may also be added to facilitate mixing and pumping the slurry. Either raw water or recycled filtrate from the process may be used. The resulting mixture is then pumped into the digesters. Each digester operates at mesophilic conditions (37 C). The tank is stirred continuously by one or more digester mixing devices (gas recirculation, liquid recirculation, or mechanical agitation) and is equipped with a floating cover to maintain the system at constant pressure. The conversion occurs in two steps: 1) solids are solubilized or digested by enzymic action, then 2) the soluble products are fermented in a series of reactions producing methane and carbon dioxide. The products of digestion consist of two streams. The gas stream is composed of approximately equal volumes of methane and carbon dioxide. The slurry stream is composed of an aqueous suspension of undigested organic matter which must be disposed of appropriately. Gas treatment and handling The product gas from the digester contains methane, carbon dioxide and trace quantities of hydrogen sulfide. The two acid gases must be removed if the gas is to meet pipeline standards. A standard method of removing acid gases from natural gas is by absorption with monoethanolamine (MEA). The gas leaving such an absorber has essentially no residual carbon dioxide or hydrogen sulfide. The MEA is then regenerated and recirculated. Before the

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methane can be sold, it must also be dried. This may be accomplished by a glycol dehydration process in which the moisture is absorbed in dry glycol, which is also regenerated and recirculated. If used off-site, the gas must also be pressurized. Effluent handling and disposal During steady-state operation in the waste digestion system, it is necessary to bleed the system continuously. Water and non-digestible matter must be removed at a rate equal to their rate of feed. Because the digesters are reasonably well-stirred, the composition of the effluent is essentially the same as that of the contents. In addition to water and indigestible matter, the effluent from the digesters contains undigested digestible solids, organic matter in solution and a viable biological mass. This slurry is best disposed of by separating the solids from the liquid and either recycling the liquid or returning it to a sewage treatment plant for final disposal. The solids, in the form of a moist sludge or cake obtained from a filter or centrifuge, are then incinerated or sent to a landfill.
METHANE PRODUCTION PROCESSES

Methane gas can be produced from municipal solid waste by anaerobic digestion in a processing facility such as described above, or it can be recovered from landfills. Alternative digestion processes include conventional digestion, high solids digestion, multi-stage digestion processes, and plug flow digestion, Methane can be extracted from existing landfills, or the landfill can be designed specifically for the dual purpose of refuse disposal and methane production; this latter process is termed controlled landfilling.
CONVENTIONAL DIGESTION

Anaerobic digestion has been used as a means of treating sewage solids since the nineteenth century. Municipal facilities have been operated for many years, stabilizing sludge and producing a low calorific content gas used to provide a portion of heat and power requirements of the treatment plant. In the late 196Os, renewed interest in anaerobic digestion technology was generated by the potential production of energy from the process. Golueke was the first of the most recent workers to study anaerobic digestion of solid waste. A five-year program under his direction examined the technical feasibility of digestion of municipal waste with large quantities of animal waste [ 31. Further work by Pfeffer demonstrated the feasibility of methane production from municipal solid waste, with limited additions of sewage sludge [4]. This work included an evaluation of gas production as a function of pH, temperature, solids loading, retention time and slurry concentration, and an evaluation of the costs and net economic benefit of the system.

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In 1969, laboratory and engineering evaluations of fuel gas production from municpal solid waste were initiated by Consolidated Natural Gas Service Company at Dynatech R/D Company. Laboratory experiments confirmed the technical feasibility of utilizing the basic anaerobic digestion process to convert organic wastes to pipeline quality fuel gas. A comprehensive model of a 1,000 Mg per day municipal waste digestion system was developed for the National Science Foundation to evaluate the system s economic feasibility [ 21. In 1975, Waste Management, Inc., of Oak Brook, Illinois, was selected by ERDA (now DOE) to provide full-scale production of methane gas from solid waste, including design, construction and operation at Pompano Beach, Florida. This process is known as Refuse Conversion to Methane (RefCOM). The process design includes primary shredded refuse storage, magnetic separation, secondary shredding, air classification and pneumatic transport to the digester, anaerobic digestion, mixing of recycling digester gases, residue dewatering, nutrient addition, filtrate recycle and gas flaring. The digester design allows the investigation of thermophilic and mesophilic modes of anaerobic fermentation covering an average solids retention span of 4 to 20 days [5]. The RefCOM facility is the only large MSW anaerobic digester operating in the United States. The primary technical objective of this facility is to demonstrate long-term gas production at rates sufficiently high to result in attractive economics. At present, the RefCOM facility is operating at a 10% feed solids concentration, 2% digester concentration, with a 20- to 30-day average solids retention time. Significant improvements may be achieved during the ensuing experimental program, but the process is not economically attractive under the present operating conditions. The RefCOM facility has experienced a variety of mechanical problems, some common to most resource recovery systems, some unique to anaerobic digestion. The former include failures in the size reduction and separation equipment. The air classification equipment has not performed as expected. Problems have arisen in pumping the slurry to the digester and in mixing the sewage solids and solid waste. Plastics and textiles have become entangled in impellers. As a result, the experimental program has lagged. The experimental program was planned to establish optimum operating criteria for the production of methane at the facility. Five goals of the proofof-concept experiment have been defined [ 51: (1) To establish information concerning the gas product quantities and values. (2) To evaluate process reliability and economics. (3) To determine optimum design and operation parameter values for each process stage and method of operation. (4) To establish a basis for comparing the process to other means of energy production and/or resource recovery from urban waste. (5) To establish the technological and economic basis for commercial utilization of the process.

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The potential environmental impact of anaerobic digestion of municipal solid waste has been evaluated at some length in the laboratory. However, few field data are currently available. The character of the filtrate/centrate produced during dewatering was documented by Pfeffer [ 41. Tests run with chemical coagulants indicated that a relatively pure supernatant could be produced. Concurrent tests of leachate produced when the dewatered residue was landfilled indicated that the quality of leachate was better than that found in conventional landfills. There are no known data available to characterize emissions from an incinerator processing the residual cake, but the chemical composition is expected to be no more objectionable than with any other solid waste systems. Any detailed evaluation of research, development, and demonstration needs is premature until the initial experimental program using the RefCOM facility is completed. The completion of this program and thorough evaluation of the results, with the objective of establishing a state-of-the-art configuration, is essential to determine the technical and economic feasibility of the process. Pending this evaluation, research, development, and demonstration should focus on improved understanding, efficiency, and cost effectiveness of pretreatment, digestion, end use, and effluent/residue processing unit operations.
HIGH SOLIDS DIGESTION

One of the most significant drawbacks to conventional anaerobic digestion of municipal solid waste is the large digester volume required. The concentration of solids fed to the digester is one of the most important design parameters from the standpoint of capital and operating costs and of the material and energy balance. Several concepts, based upon packed and fluidized bed technology, have been proposed to employ high solids concentrations in the digestion process. This technology is a derivative of the anaerobic filter concepts formulated by Coulter [6] and McCarty and Young [ 7, 81. Anaerobic filters have been applied to wastewater treatment (e.g., the ANFLO process, developed recently at Oak Ridge National Laboratory, Oak Ridge, Tennessee) and, more recently, packed and fluidized beds have been investigated for application to municipal solid waste and biomass. The packed bed digester is comprised of a containment vessel, inert bed material which supports biological growth, circulating fluid, substrate (e.g., municipal solid waste), pumping system and, in some cases, an extraction/purification system [9]. The process has been used to produce methane, liquid fuels, and chemicals from organic waste materials [9]. The fluidized bed system is similar in design, except that the inert bed material is fluidized by the substrate. Rioconversion systems employing fixed and fluidized bed techniques are still in the formative stages of development. Initial work employing municipal solid waste as a substrate was carried out in 200 Q drums containing about 23 kg of material [lo]. Methane was the primary end product. More

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recently experiments have been conducted on aquatic biomass to investigate production of liquid fuels and chemicals. These experiments have been carried out in batch fluidized bed reactors containing approximately 80 kg (175 pounds) of material [ 91. To date, results of these experimental programs show significant potential for reducing the cost of anaerobic digestion systems with advantages of: reduced digester capital cost; reduced water requirements; reduced energy requirements for mixing, heating; higher solids reduction/energy yield; reduced residue disposal costs; and reduced wastewater treatment costs. The packed and fluidized bed digestion technique appears to produce no more adverse effect on the environment than do conventional stirred tank reactor systems. On the contrary, it offers the potential to reduce land requirements and can significantly reduce residual disposal and wastewater treatment requirements. Initial experiments with packed and fluidized bed digestion systems have shown that the process offers considerable promise to improve the economics and energy yield of conventional anaerobic digestion systems. Bench-scale experimental research using municipal solid waste as the substrate and a detailed conceptual design or cost analysis are warranted.
MULTI-STAGE DIGESTION

Two-stage digestion incorporates a combination of conventional, high rate digestion and unmixed digestion. The first stage is a continuously fed, completely mixed, temperature controlled, biological unit from which methane and carbon dioxide are collected. The second stage is a quiescent unit for solids separation and concentration. There is less gas production from the second stage than from the first. Two-stage digestion is currently common practice in municipal sewage treatment systems. The first digester functions to optimize conditions for maximum biological decomposition of the sludge and hence maximize gas production. Digested sewage sludge containing about 5% solids is then pumped into the second vessel where the solids settle to the bottom and a scum layer forms on the top. The supematant is then easily removed. The two-stage digester provides significant improvements over single stage high-rate digesters or unmixed digesters [ 11-161. Most important is the reduction of retention time. Since mixing in high-rate digestion is not compatible with thickening, a 30- to 60-day retention time is needed for one-stage digestion, whereas in a two-stage system of sewage sludge, a lo- to 2O-day retention time is needed for digestion and thickening. The technology for two-stage digestion is well-established on an industrial scale for sewage treatment. Since the function of the second stage is to facilitate solids separation and concentration, the process is applicable to any low solids feedstock. Addition of urban refuse in moderate amounts is not expected to alter operation of the system. Further research is not, therefore, considered necessary for commercialization of the process.

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Two-phase digestion In contrast to two-stage digestion, two-phase digestion involves two biologically active digesters in series. Both digesters function to optimize conditions for active metabolism of microorganisms. In the first phase, complex organic substances such as fats, proteins and carbohydrates are hydrolyzed, fermented and biologically assimilated by facultative anaerobes and strict anaerobes. These bacteria are referred to collectively as acid-forming bacteria since the primary end products of the first-phase conversion are volatile fatty acids. During the second phase, organic acids are converted by several different obligate anaerobes, referred to collectively as methanogenic bacteria, to produce primarily the gaseous end products, methane and carbon dioxide. Since the acid former-s and the methane formers have different physiological characteristics, nutritional requirements, growth kinetic capabilities, and sensitivity to environmental stress, operation of each of the digesters is geared to meet the needs of specific microorganisms. The parameters which can be controlled include temperature, nutrients, mixing, pH and loading rates. As the acids used by the methane formers are produced by the acid former-s, the key to the success of a two-phase system is obtaining a strict balance between the two groups of microorganisms. When the system is in balance, the methane bacteria use the acid intermediates as rapidly as they are produced by the acid bacteria. If the methane bacteria are not present in suitable numbers, or their action is slowed due to unfavorable environmental conditions, the volatile acids will not be utilized. Therefore, successful application of this concept depends upon maintaining dominant cultures of acidogenic and methanogenic bacteria. A number of methods to achieve two-phase separation have been attempted. These include: (1) membrane dialysis separation of the two groups of bacteria, (2) selective inhibition of methane bacteria in the acid digester, and (3) kinetic control of both groups of bacteria. Membrane dialysis separation of acid and methane bacteria has proved successful in laboratory studies. Although the bacteria are physically separated, there is rapid interchange of nutrients and metabolic waste products throughout [ 17, 181. Due to operational difficulties with dialysis membranes, however, the potential for this method is limited for large-scale anaerobic digestion. Suppression of methane forming bacteria can be achieved by two general types .of inhibitors: (1) those that act as alternative acceptors of hydrogen, such as viologen dyes, long-chain fatty acids, propanediol and sulfate ions, and (2) chemicals that directly interfere in the metabolic pathway of methane formation such as methane analogues (i.e., the halogens, chloroform, carbon tetrachloride, bromochloromethane, chloralhydrate) and molecules resembling a coenzyme involved in methane formation (i.e., bro-

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moethanesulfonic acid), and (3) selected antibiotics such as monensin [ 191. Experimental studies in vitro and in uiuo using cattle as a host have demonstrated that selective inhibition of methane formation is feasible. In a recent study at the University of Illinois, 100% methane suppression was obtained using bromoethanesulfonic acid [ 201. Selective inhibitors of methane production in cattle which improve feed efficiency are currently being developed by the pharmaceutical industry. There is little published research on the effectiveness of those methane suppressors for application in two-phase digestion. The drawback is that the inhibitor must be deactivated to enhance methane production in the second phase. Kinetic control of the growth of acidogenic and methanogenic bacterial populations can be achieved by adjustment of dilution rate and cell mass recycling in both phases of the digestion process. This method of two-phase separation has been successfully applied to soluble and insoluble substrates [ 21-231. Research initiated in 1971 defined the kinetics of biological reactions in two-phase digestion using batch, semi-continuous, or continous culturing methods. The reactions studied included the production of acids from glucose, hydrolysis and acid production from activated sewage sludge, hydrolysis of cellulose, and production of methane from acetic acid. The feasibility of phase digestion by controlling kinetic parameters was demonstrated on a laboratory scale using two 10 Q digesters [24]. The process has since been operated using a 100 Q acid digester and a 400 Q methane digester v51. Based on the results of laboratory studies, projections of operating characteristics for two-phase digestion of urban refuse have been made [ 241. With a feedstock of cellulose, the acid digester will require a retention time of one to two days. Longer retention times may be necessary for the acidification of high-cellulose refuse feeds and with increasing cellulose particle size. The retention time for the methane digester is expected to be as high as 5 to 8 days. Several processes have been investigated with the intention of reducing the retention time required in the acid stage of urban refuse digestion. Klass et al. [ 261 patented a process involving recycle of indigenous enzymes. The microbial cells within the system are ruptured so that enzymes are released. The enzymes then act to degrade untreated refuse, thus improving digestion efficiency and hence, methane yields. Methods of cell rupture cited in the patent include sonic methods, mechanical rupture by shearing and forcing re. fuse through orifices and cycle pressurizaton-depressurization. The effectiveness of enzyme recycle in reducing retention time has not yet been reported. Reduction in retention time of the acid phase has been attained using a plug flow system for hydrolysis and acid production of an urban refuse/ sewage sludge feedstock [27]. Plug flow digestion was simulated by ten 208 Q steel reactors with a 2080 Q total working volume for the acid phase. These reactors were maintained at 37 C with minimal mixing. Acidified re-

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fuse was pressed to separate residual solids and the liquid fraction was fed to the methane digester. The methane phase was operated using a 2270 Qcontinuously stirred tank reactor (CSTR) unit maintained at 37 C. The system was operated at a retention time of 10 days and 15 days for the acid and methane phases, respectively. However, acid production levels in the plug flow systems tended to level off after 5 days and significant solubilization of the solid waste was obtained within 3 days. Work on manure digestion systems [ 28-321 is supportive of the plug flow digestion concept. Preliminary process design and mass and energy balances have been developed for a hypothetical two-phase sludge digestion plant equivalent to the Stickney high-rate digestion plant of the Metropolitan Sanitary District of greater Chicago in terms of daily solids loading [ 241. Comparison of these results with the actual operating data from the Stickney plant indicate that a two-phase plant can produce up to 80% more methane than the conventional plant, while the total digester volume for the two-phase system is only about 35% of the total volume of the high-rate digester. Similar engineering designs are not yet available for two-phase digestion of urban refuse. However, an engineering analysis for a system planned for the City of Pittsburgh is being undertaken [ 331. The advantages of two-phase digestion over conventional high-rate digestion are: increased control over the growth of acidogenic and methanogenic bacterial populations; substantial reduction in total reactor volume and hence reduction in capital and operating costs; decreased heat requirements and increased thermal efficiency; high rates of solids stabilization; increased methane yield and higher percentage of methane in the product gases; and reduction of the nitrogen content of the system effluent by simultaneous liquefaction and denitrification of waste feeds in the acid digester. The disadvantages of two-phase digestion are the necessity for skilled operators and increased instrumentation to monitor and control microbial population growth. The key to success of two-phase digestion is the optimization of the acid and methane phases. Research emphasis should, therefore, be placed on economical methods to maintain high growth of uncontaminated cultures [34] . Thus far, the most successful approach has been by control based on kinetics. Bench-scale experimentation with two-phase digestion of urban refuse should focus on identification of optimal conditions for the maintenance of microbial populations for maximum production of methane using kinetic control. Methods to reduce retention time by increasing biodegradation should be investigated. A detailed engineering and cost analysis of twophase digestion of urban refuse should be completed.
PLUG FLOW DIGESTION

The concept of a plug flow digestion system can be visualized as a cylinder lying on its side through which digester substrate continuously moves. Feed-

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stock is continuously loaded from one end, and effluent is continuously discharged from the other. Plug flow of material through the digester is managed such that an increment of solid material in the system contacts only solid material entering directly before and directly after it. There is virtually no blending or mixing of solids. Liquids trickle downward by gravitational forces, but essentially remain with the solids that were introduced at the same time as the liquid. Simple plug flow digesters operated with diluted and undiluted wastes, maintained at mesophilic temperatures without mixing, have proved to be effective and economical for production of methane from cattle and dairy farm wastes. Some commercial-scale systems have been developed, but little operating information is available [ 321. Two plug flow, mesophilic, unmixed systems were designed and constructed under the supervision of Agricultural Energy Corporation, Luddington, Michigan. The more economical of the two systems, built in Custer, Michigan, is made of a fabric-reinforced rubber bag supported by a V-shaped concrete-lined channel dug in the ground. The top of the bag is a flexible membrane which expands as biogas is produced. The digester is insulated with Styrofoam sheets which float on the surface of the plastic material. The digester is claimed to be low in cost, easy to install, capable of withstanding low temperatures and relatively trouble-free. The other plug flow system at Rice Lake, Michigan, is a galvanized metal tank laid in a trench and insulated on the top by soil. Fluid which accumulates in the bottom is pumped for recycle to the influent. The gas produced is used to drive an engine/generation set, and the waste heat from the generator units provides heat for the digester. Most of the operational information available on plug flow digesters has resulted from a three-year research program at Cornell University to develop improved low-cost anaerobic digestion technology for use on small farms in the United States [30,31]. The feasibility of maintaining high methane yields by plug flow digestion of dairy cow manure was demonstrated on a bench scale using completely mixed fermenters in series. Optimum conditions for plug flow digestion have been identified using the bench-scale system and three pilot plants (5 m3 volume each). Variables being evaluated presently include: temperature of operation (25 C, 35 C), straw and sawdust bedding addition, intermittent feeding, mixing, and moisture content. A fullscale plug flow reactor (35 m3) capable of handling wastes from 65 dairy cows when operated at a 1Oday hydraulic retention time has been operated for more than one year. Preliminary analysis indicates that more efficient solids conversion is attained with the plug flow digestion than with high-rate digestion. Under operating conditions of 35 C, 30 days hydraulic retention time and 10-l!% total solids dairy manure feed, the full-scale reactor produces 1.26 m3 biogas/m3 day per reactor. The completely mixed control unit of similar size produces 1.13 m3 biogas/m3 day per reactor. The primary operational problem with plug flow digestion at Cornell has been temperature control in cold weather and subsequent plugging of the system. Significant bene-

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fits have been realized from insulating the top gas collection liner of the reactor [ 401. The feasibility of plug flow digestion of a mixture of urban refuse and sewage sludge has been demonstrated on a bench scale [27]. The plug flow design was employed as the acid phase of a two-phase system. Acids extracted from the residue were then fed into a CSTR for the production of methane. The plug flow reactor was simulated using ten unmixed digesters. The operation procedure was as follows : sewage sludge (5% solids) was added to urban refuse so that sludge solids comprised 10% by weight of total solids in each jar. One digester was filled with feedstock each day for 10 days. On the eleventh day effluent from the first digester was pressed and the acid liquid loaded into the CSTR. Each following day the successive digester effluent was pressed and the liquid loaded into the CSTR. The results indicated that significant solubilization of solid waste occurred within three days retention time of the acid phase. Approximately one third of the total volatile solids introduced to the system was converted to biogas [ 271. Plug flow digestion appears to have been highly successful for methane production from manure due to reduction in capital and operating costs and higher gas yields when compared to high rate digestion. Bench-scale studies need to be initiated using a mixture of urban refuse and sewage sludge to determine the feasibility of one-phase digestion using plug flow. Emphasis should be placed on the effects of moisture content on material flow.
LANDFILL GAS EXTRACTION

The world s first commercial landfill methane recovery facility started in 1971 when the Los Angeles County Sanitation District constructed wells to prevent gas migration to adjacent residential properties at the Palos Verdes landfill, in California. Since that time a number of other projects have been initiated. Sixteen of these, with operational information, are listed [35]. In addition to the Palos Verdes landfill, the ones in commercial operation include the Mountain View landfill (Mountain View, California), the AzusaWestern landfill (Azusa, California), and the Sheldon-Arleta landfill (Sun Valley, California). Other landfills on line include Ascon, California; City of Industry landfill, California; Operating Industries landfill, California; and Cinnamanison landfill, New Jersey [ 371. Successful operation of gas extraction from existing landfills is highly sitespecific [36]. Therefore, the primary question to be answered is: from which existing landfills will the extraction of gas be profitable? The answer depends on a number of technical and economic factors which influence the cost and potential success of the extraction process, including the location and composition of the landfill, the type of drilling and extraction equipment necessary, the gas production rate, local restrictions and regulations, gas processing, and marketing. Few of these factors are adequately understood.

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When the potential hazards of gas leakage from landfills were first realized, investigation centered on the identification of gas composition in relation to landfill age and on gas movement through the landfill. Before extensive gas extraction is undertaken, a test well and supporting wells are drilled, and a series of tests is run to evaluatelandfill pressure profiles, gas composition and heating values, and stability of withdrawal rates [ 38,391. The results of these analyses are valuable in determining efficient operating parameters for the particular landfill, but it is still not possible to predict the quantity of methane obtainable from the landfill. It is well documented that gases move horizontally and vertically through the landfill at velocities of about 7 cm/day [40]. The rate may vary, however, depending on the landfill composition. Movement downwards results from molecular diffusion plus density differences, whereas movement to the sides and upwards to the atmosphere results from diffusion alone [41]. Carbon dioxide can move into the soil beneath a landfill as well as upward, while methane tends to rise through the landfill and not dissolve into groundwater [42]. To determine the most efficient design of wells, a model is needed which defines diffusion rates of gas through various soils and refuse substrates. After drilling, the gas extraction wells are typically lined with a perforated casing and packed with sieved gravel. Collection manifolds connect the wells, bringing the biogas to a common site. This method has proved to be generally satisfactory, but other less expensive methods should be investigated. In early well systems, a differential settlement in the fill led to broken pipes and collapsed wells. Development of specialized drilling equipment may be necessary. Removal of gases from existing landfills has been accomplished by the same principle that is involved in the extraction of ground water. Pumps are manifolded to the wells, creating a pressure gradient within the landfill which draws the gas through the collection systems. In some cases, sufficient negative pressure has developed so as to draw air into the fill. Oxygen can inhibit the anaerobic process, while nitrogen dilutes the fuel gas. Extensive experiments have been conducted at Palos Verdes and Mountain View, California, to develop optimum pumping rates for each fill. A problem with the extraction system at Palos Verdes has been corrosion of pipes believed to be due to industrial wastes deposited in the landfill. Further investigation of corrosion problems and alternate extraction systems should be encouraged. From the standpoint of commercialization of the technology, it is imperative that a method for predicting methane generation rates and yields be developed. This is necessary in order to design the recovery system and to evaluate the economic feasibility of methane recovery at any specific site. The model will need to take into account geological and meteorological conditions, refuse composition, and operating conditions. Potential methane production can possibly be determined by evaluation of leachate com.position.

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After extraction the gas may be upgraded. A typical system consists of dehydration by compression and cooling, pretreatment for hydrogen sulfide and free water removal in molecular sieve towers, followed by another series of molecular sieve absorption towers to remove carbon dioxide. The resulting methane gas (35 GJ/m3) is pressurized to 2.5 MPa and injected into a pipeline distribution system. Corrosion problems have been encountered in field installations. However, it is expected that corrosion can be eliminated with the injection of inhibitors into the biogas before processing. As noted earlier, evaluations have been made of the extraction of methane from existing uncontrolled landfills for the Mountain View Project [ 421, the project at Palos Verdes, and by the Los Angeles Bureau of Sanitation [43]. The low rate of methane production results in high costs for the gas. Typical gas production from existing uncontrolled landfills is in the range 3.8-14.3 m3/Mg year of deposited waste, with a methane content above 50%. Costs were based on a 20-year life of a gas recovery system at an existing landfill. Without enhancement, a landfill undergoes active degradation over a period of many years, the time primarily depending on the moisture content of the fill. Thus, problems associated with a given landfill (e.g., methane migration, ground water contamination) are likely to continue far beyond the termination of refuse placement, and indeed may not appear for some time after fill completion. Postconstruction maintenance and monitoring of a completed landfill site, to assure that it maintains its integrity and does not become a source of pollution, can therefore be a long-term source of concern. Another disadvantage of slow degradation is the long period of time required for gas extraction and the low annual methane yields per mass of refuse. Significant cost saving could be realized by increasing the rate of degradation within existing landfills. Further, research to date has indicated that higher ultimate gas yields are possible in controlled landfills.
METHANE ENHANCEMENT IN CONTROLLED LANDFILLS

The concept of enhancing methane production in landfills, controlled landfilling as it is sometimes known, has been developed by considering the landfill as a large batch anaerobic digestion system in which optimum conditions for methane production are provided. Urban refuse, which may have been separated, shredded, or baled is combined with nutrients, buffer and inoculum before its deposition into the landfill for the purpose of sustaining high reproductive rates of bacteria during decomposition. The landfill is constructed to allow for a gas recovery system and a moisture control system, and to optimize refuse cell sizeand geometry. The gas is extracted once the refuse cell is anaerobic and decomposition begins [ 441. As with the other digestion processes, the composition of the refuse directly affects the rate of methane production and subsequently the methane yield. It is advantageous for .the refuse to have a high concentration of biodegradable materials, such as food, garden wastes, and paper. Sewage

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sludge mixed with the refuse increases the percentages of biodegradable materials in the landfill, and at relatively low concentrations (75-400 mg/l), stimulates gas production. At higher concentrations, however, inhibition may result [ 451. Methane production may also be inhibited by industrial wastes containing high concentrations of sodium chloride, sulphate, potassium, magnesium, calcium, ammonia, carbon tetrachloride, or chloroform. However, conclusive evidence for the inhibitory effects of such materials in landfills is not available [46,47]. Contradictory results have been obtained regarding the importance of particle size reduction for increasing methane production. Particle size reduction by shredding exposes more surface area for contact of nutrients and microorganisms. Research has indicated that particle size reduction increases methane production in laboratory digesters. DeWalle et al. [44] demonstrated that by reducing nominal particle size from 25 to 2.5 cm through shredding and milling, gas production was increased by more than a factor of four. Most of the gas produced, however, was carbon dioxide and not methane. In fact, the experimental system with the highest methane production was one which used unshredded refuse. The value of shredding urban refuse has not been accurately assessed by small-scale experimentation, since reduction in particle size also affects the rate of oxygen depletion, density of the fill, and percolation of water, nutrients, and buffer into deeper layers. Due to the heterogeneous nature of the unshredded refuse, channels may form by infiltrating water, resulting in an uneven distribution of nutrients and buffer. On the other hand, shredded refuse covered daily with soil compacts tighter than does unshredded refuse and may retard the percolation of water, nutrients, and buffer to deeper layers of the landfill. As implied above, refuse density (in-place) affects mass transfer. Density also affects the onset of anaerobic conditions. Research on the effects of baling refuse is underway, but the optimum density for methane production has not yet been determined. The nutrients, buffer, and inoculum may be provided either by chemicals, sewage sludge, or selected industrial wastes which are mixed or layered with the MSW before its deposition into a landfill, or by recycling leachate through the landfill, or by a combination of these methods. Since the bacteria which carry out the biodegradation process grow best within a narrow pH range, the pH within the landfill should be controlled. The optimal pH range of 6.25 to 7.5 has been controlled by the addition of calcium carbonate, a buffering agent, in simulated landfill cells [ 483. Based on a bacterial cell formula of C5H,N02, about 12.4% by weight nitrogen is needed for cell growth, while one-fifth of that value of phosphorus is required [ 511. The nutrient value of recycled leachate depends on the landfill composition. Evidence suggests that leachate material could provide only a portion of the nutrient requirements; thus addition of sewage or artificial nutrients may also be necessary. However, it has been shown by others that

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macro nutrient supplementation, i.e., N, P, S, is unnecessary [49]. The application of sewage sludge and recirculation of leachate on controlled landfills is a potential health hazard for spreading bacteria and viruses, and a potential odor nuisance to nearby residents. The health and environmental effects of a controlled landfill need to be determined. The two most important factors affecting methane production rates in landfills are temperature and moisture content. Methane production is severely limited at temperatures below 15 C, but increases with increasing temperature to an optimal temperature of 30-40 C. This parameter cannot be easily controlled in landfills, but many researchers believe that even in colder climates significant temperatures can be reached due to thermal insulation from surrounding soil and refuse [ 531. High temperature areas are expected to be non-homogeneous in distribution. Temperature measurements from full-scale, enhanced landfills are needed to determine the extent of changes in temperature within actively decomposing landfills. The refuse moisture content should be at least 50%, and preferably about 80%, for high methane yields [48]. Methane production increases exponentially with increases in moisture content in batch digestion [ 441. Moisture content of refuse (normally 25%) may be increased by the addition of water, sewage sludge, industrial wastes, or leachate material before deposition into the landfill. Alternatively, the natural ground water supply could provide water during digestion, but this may contaminate the water as discussed above. Although methods for water addition have been evaluated, large scale implementation of moisture control systems is needed. Whatever the source of moisture, the landfill must be designed to retain moisture and to obstruct the flow of polluting leachate material. Impermeable or low-permeable barriers, such as certain types of soils or synthetic liners, can be placed on the bottom and sides of the landfill area; these barriers are commercially available. The landfill should slope towards a point where leachate material can be collected for treatment or collection. If the topography of the landfill site does not provide for natural drainage, recontouring the land, probably at great expense, is necessary. Evaluations of landfill size and geometry have indicated that economy of scale characteristics apply [authors calculations] . Minimum size or volume of a landfill for economic gas production is not directly related to gas generation, but rather by the economics of gas recovery wells and collection system, processing equipment, delivery system, and final gas use. Similarly, the shape of the landfill should be square or rectangular for optimal coverage of recovery well influence areas [42]. Significant economic savings could be realized by increasing the efficiency of gas recovery wells and collection systems. The enhancement concept appears to be a potentially effective method for producing methane from municipal solid waste. Experimentation using laboratory test ,cells has provided information on the effects of controlled conditions on methane production, however, the quantitative effects of

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water, temperature and refuse density remain to be elucidated at a landfill site. Large-scale field studies are now necessary to answer many of the remaining questions and to verify the application of results from laboratory studies to commercial use. Landfills need to be designed and constructed specifically to study the effects of key parameters on methane production with provisions made for monitoring biological activity at different depths. Experiments should be designed to make a comparison between the effects of adding nutrients, buffer, and moisture before deposition of refuse. The comparison should include both leachate and sewage as nutrient and inoculum sources. An engineering and cost analysis of controlled landfill systems should also be prepared.
METHANE END USE TECHNOLOGY

Most problems encountered to date in gas utilization have been with construction materials. Large-scale experience with municipal solid waste in stirred tank digesters is very limited - only preliminary data are available from the RefCOM facility where the gas is flared. On the other hand, there is a large body of experience with digester gas from wastewater sludge. Experience with fuel gas production from novel systems such as plug flow or packed bed techniques is confined to small pilot-scale systems. Since 1972, experiments have been conducted to draw methane off landfills, but again there is little commercial-scale experience with such systems. Most problems encountered to date in gas utilization have been with construction materials. A critical factor in evaluating the viability of fuel gas production from solid waste is the determination of the relative merits and the technical and economic feasibility of utilizing the gas as-received versus upgrading it to a high-Btu equivalent of pipeline quality. A number of commercial systems are available to remove CO2 and other possible contaminants from the digester or landfill gas. Purification experience with systems operating on solid waste gas is limited to relatively few in California. A recent review of available gas purification technologies [SO] indicated that available methods for treatment of digester gas include physical absorption, chemical absorption, adsorption and membrane separation processes. Simple physical absorption, water scrubbing and membrane separation were found to be most attractive based upon data available at the time. The membrane process may have important practical considerations which could rule in its favor, but there is little large-scale experience with this system. More experimental data are required on membrane and phosphate buffer systems, as well as a more careful analysis of CO2 recovery proposals before final recommendations can be made.

133 BIOMETHANATION

Many processes, including municipal refuse pyrolysis, produce a gas consisting of methane, carbon dioxide, carbon monoxide and hydrogen, and having a low calorific value. At times this gas may be burned directly; however, in many instances it is desirable to upgrade the gas to pipeline quality methane by shifting the CO to COZ and Hz and methanating to methane (using coal gasification terminology). This upgrading may be accomplished either catalytically, as in coal gasification, or biologically. The latter process has been termed biomethanation [ 511. In biomethanation, the gases are cooled to 60 C and sparged into a pressurized fermentation vessel. The fermenter contains nutrients, buffer and the microorganisms which carry out the conversion. A series of reactors is required to reduce carbon monoxide concentrations to pipeline standards. Because the carbon dioxide, which is usually present in excess, is more soluble in the broth than in the methane product, the fermenter also acts as an acid gas scrubbing system. An external recirculation loop is used to separate, concentrate, and recycle the microorganisms, and to flash desorb the carbon dioxide from the broth. The biomethanation concept has been evaluated, experimentally at the bench scale as a process to upgrade coal and biomass gasification synthesis gas [ 511. Microorganisms were selected which carried out both the shift and methanation reactions. Operation at high conversions (to 240 volumes of methane per volume of reactor per day) and high pressure (3 MPa) was demonstrated. Unlike catalytic processes, the process was shown to be sulfur tolerant; a feed gas with up to 6% H# presented no problems. More recently, a study was carried out to evaluate the economic feasibility of applying biomethanation to solid waste pyrolysis gases [ 521. The incremental cost for upgrading by biomethanation was estimated as being less than catalytic methanation.
ACKNOWLEDGEMENT

This work was carried out at Dynatech R/D Co. under subcontract from the Mitre Corporation, Bedford, Massachusetts which held a prime contract from the Urban Waste Technology Branch, U.S. Department of Energy.
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136 49 Le Roux, N. and Wakerly, D. The microbial production of CH, from the putresible fractions of solid household waste. Proc. 1st Recycling World Congress, ME. Henstock, (Ed.), Basel, Switzerland, 1978. Ashare, E., Young, J.C., Hossan, R.J. and Duret, G.L., 1978. Evaluation of systems for purification of fuel gas from anaerobic digestion. Dynatech Report no. 1628, submitted to U.S. Department of Energy under contract EY-76-C-02-2991.*000, July 30,1978. Dynatech R/D Company, Cambridge, MA. Augenstein, D.C., Wise, D.L., Wentworth, R.L., GaBaher, P.M. and Lipp, D.C., 1977. Investigation of converting the product of coal gasification to methane by the action of microorganisms. Final Report no. FE-2203-17 under contract no. E.(49-18-)-220. Dynatech R/D Company, Cambridge, MA. Ashare, E., Sharon, A.C. and White, S.R., 1979. Engineering economic analysis of biomethanation of pyrolysis gas. Final Report on Contract EM-78-C-01-5154, Dynatech Report no. 1885. Dynatech R/D Company, Cambridge, MA. Reee, J.F., 1980. Journal Chemical Tech. & Biotechnology, 30: 468-465.

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