JOURNAL OF GEOPHYSICAL RESEARCH, VOL. 92, NO.

D2, PAGES 2181-2187, FEBRUARY 20, 1987

The Production

of Methane

From

Solid Wastes

H. G. BINGEMER AND P. J. CRUTZEN

Max Planck Instituter or Chemistry,Mainz, Federal Republic of Germany An analysisis presentedof possibleworldwide production of methane from anaerobic decay of organic municipal and industrial wastesin landfills. The amount of methane releasedto the atmosphere from this

source may now be in the rangeof 30-70 x 106T/yr, whichis between and 18% of the total CH, 6%
source. By far, most of this emission comes from the industrialized world. Release rates from these

countries have been increasing steadily during the past decades,but growth rates are now gradually stagnating. the future, the contributionfrom developingnationsis expectedto grow rapidly because In of increasingpopulation and urbanization. Consequently,methane releasefrom landfills may become one of the main sourcesof atmosphericmethane in the next century.

and sink inventories have been compiled by several authors Methane(CH), mostabundant the and stable hydrocarbon [e.g., Ehhalt and Schmidt, 1978; Sheppard et al., 1982; Seiler, 1984; Crutzen, 1986]. Table 1 givesan overview of the individgas in the atmosphere,plays an important role in the photochemistry of the background troposphere.The photochemical ual source strengthsthat are currently estimated. In this paper we analyze especiallythe global significanceof oxidation of methane, which is initiated by reaction with the the production of methane from anthropogenicwaste carbon. hydroxyl (OH) radical, sets up an important chain of reacA significant fraction of the carbon that is cycled through the tions, leading to carbon monoxide and carbon dioxide [McConnell et al., 1971; Levy, 1971]. The effects of these reactions environment by man's activities consists of domestic and inon tropospheric photochemistry depend strongly on con- dustrial wastes. As an appreciable fraction of this carbon is centrations of NO x. In low NO x environments,the methane dumped in landfills that develop anaerobic conditions, the oxidation chain of reactionsis an important sink for hydroxyl decay of this organic carbon is a potential source of methane and perhydroxyl (HO2) radicals. high NO x environments, [Sheppard et al., 1982]. It is estimated that throughout the In which are mainly located at mid-latitudes in the northern world, more than 80% of the municipal solid wastes (MSW) hemisphere the vicinity of pollution sources, in methane oxi- collected from urban areas is deposited in landfills or in open dation contributes substantially to ozone formation [-Crutzen, dumps [Flintoff, 1976]. Sanitary landfilling near urban centers 1973, 1986; Chameidesand Walker, 1973; Lotan et al., 1981; is the main method in industrialized countries; crude dumping is common in the developing world. Thompson and Cicerone, 1986]. Atmospheric methane con-

1.

INTRODUCTION

centrations have been rising over the past three decadesat an

averagerate of approximately1-1.2% yr- [Rasmussen and

Khalil, 1984; Seiler, i984; Blake and Rowland, 1986]. The response of the atmospheric photochemical system to such changesin atmosphericmethane is thereforeexpectedto result in lower average global OH concentrations, being most pronounced in tropical regions and in the southern hemisphere, and in increasing concentrations of ozone at northern hemispheremid-latitudes [Crutzen, 1986]. In addition to its influence on the background photochemical system, methane affects the earth's thermal budget by absorbing infrared radiation around 8 #m. It is suggested [Dickinsonand Cicerone,1986; World MeteoroloticalOrtanization, 1982] that, at its current rate of increase,by the middle of the next century the "greenhouse"heating by methane

2.

CHEMISTRY

OF METHANE

FORMATION

IN LANDFILLS

After dumping, biochemically degradable carbon compounds in the wastes are first attacked by aerobic bacteria. These convert organic substances primarily to carbon dioxide, water, and heat, consuming oxygen. Because of the dumping of large amounts of wastes, the oxygen availability soon declines, and the decay is taken over by anaerobic microorganisms. The anerobic decomposition of biomass is based on the interaction of different kinds of bacteria. In a first step, com-

plex organic substances are transformed to compounds like

amino acids, sugars,and fatty acids. These are further convert-

would be one quarter of that arising from increasingCO2

concentrations. It is therefore clear that there is an obvious

need to identify the processes contributing to the observed trend in atmosphericmethane. Methane is released into the atmosphere by a variety of

ed to H2, CO:, CH3COOH, HCOOH, and CH3OH, which form the substratesfor methanogenicbacteria. The resulting biogas consistsof about 50% CO: and 50% erie, although landfill gas may contain less CO2 becausepart of the CO
becomes dissolvedin the landfill water [Tabasaran, 1982; Gunnersonand Stuckey,1986-[. The degradable organic carbon (DOC), i.e., the organic

biogenicand abiogenic processes, most prominentbeing the

enteric fermentation by ruminants, release from both natural wetlandsand rice fields,burning of biomass,coal mining operations, and leakage of natural gas during transmission. The biogenicproduction generally resultsfrom bacterial decomposition of organic matter under anaerobic conditions. Source
Copyright 1987by the AmericanGeophysical Union.
Paper number 6D0664. O148-0227/87/006D-0664505.00
2181

carbon that is accessible biochemical decomposition,Co, to can be dividedinto one part Coe, which is dissimilated, and the rest Co - Coe, whichis assimilated into microbialcell material.
With increasing temperature, the rate of dissimilation grows

faster than the rate of assimilation,so that the ratio Coe/C o

can be approximated by the equation [Tabasaran, 1982]

Coe -- 0.014T + 0.28 Co

(1)

2182

BINGEMER AND CRUTZEN: METHANE FROM SOLID WASTES

TABLE

1.

Estimates of Global

Sources and Sinks of Methane

Methane,

10a T/yr
Sinks

Reference

Tropospheric reactions with OH Stratospheric reactions with OH Uptake on aerobic soils

290--350 25-35 10--30

Annual growth ( 1.1%/yr)

50--60

Crutzen and Gidel [1983] Crutzen and Schmailzl [1983] $eiler et al. [1984], Keller et al. [1983], and Harriss et al. [1982] Rasmussenand Khalil [1984], Khalil and Rasmussen [1986], and Blake and Rowland [1986]

Total required sources (sum of above)

Sources

375-475

Domestic

animals

70--80

Natural gas leaks Coal mining

Landfills

<_35
35

30--70

Biomass burning
Wild ruminants

30-- 100
2-6

Other fauna (e.g., insects) Decay of animal wastes

Rice fields and natural wetlands

<30
?

> 44-228

Crutzen et al. [1986] Crutzen [ 1986] Ehhalt and Schmidt [1971] and Crutzen [1986] This study Crutzen [1985, 1986] Crutzen et al. [1986] Crutzen et al. [1986] This study (by difference)

T being the temperature in the anaerobic zone in degrees therefore produces about 100 kg CH, [see also Stegmann, 1978]. A more thorough analysis for other parts of the world Becauseanaerobic digestion is exothermic, landfill temper- will follow. Various types of wastes decay with different rates. atures are higher than the ambient air temperatures[Gunnersonand Stuckey,1986]. The temperature in the anaerobiczone According to Rovers et al. [1977], food and garden wastes depends mainly on microbial activity, on fill geometry and decomposewithin 1-5 years,paper has an intermediate rate of depth, and to some extent, on air temperature. For a large breakdown of 5-20 years, and the 70% nonlignin fraction of landfill in Germany, RettenberTer and Tabasaran [1980] wood may last 20-100 years.However, much faster rates have report temperaturesof the anaerobiczone to be in the region also been reported [Gunnersonand Stuckey, 1986]. In estimateriof mesophilicdigestionat 30-40C.Stegmann[1986] givesa mating the methanereleaserates from biodegradable als, we will not take into account any time delay functions.In temperature of 35-45C as an average for fill depths larger than 4 m under similar climatic conditions. At depths exceed- other words, we approximate the actual situation by assuming ing 2 m the temperature was found to be independentfrom present dumping rates and instantaneousmethane release. the ambient air temperature [Rettenberger and Tabasaran, With annual growth rates of MSW of 5% in the 1960's and 1980]. Roverset al. [1977] report that field observationsfrom 2% in the 1970's, reported for the United States [Council on deep landfills even in temperate climates in Canada and the Environmental Quality (CEQ), 1982], this assumption may overestimatepresent CH, release rates by at most 20% if, northern United States do not show much variation in methane production between winter and summer conditions. The according to Rovers et al. [1977], an average decay rate of temperature of the anaerobic zone may thus regulate at about 10 years is assumed for paper, which is the main around the optimum of mesophilic digestion at 35C [Gunner- organic component of MSW in the developedworld [Amerison and Stuckey, 1986], if external heating or cooling is not can Chemical Society, 1972; Cointreau, 1984]. Oxidation by aerobic bacteria [Rudd and Hamilton, 1978] excessive. temperature of 35C may therefore be a fair estiA mate for the average temperature of the anaerobic zone both could be a sink for the methane in the landfill during its for deep landfills in the industrialized world and dumps in diffusive transport to the atmosphere. However, there is some evidencethat oxidation in the top layer of landfills may not be developingnations. At 35C, almost 80% of the DOC may be dissimilated. We a major sink for methane. The gradient of methane toward the will therefore assume that about 80% of the DOC will be atmosphere, measured within much of the upper 1.5 m of a converted into biogas, containing about 50% by volume of landfill ['Rettenberger and Tabasaran, 1980; Rettenberger, methane. Consequently, kg CH, could be producedper 1985], parallelsthe gradient of CO 2, so that the ratio of CH 4 0.5 kilogram of biodegradable waste carbon. However, for long- to CO 2 molar concentrationsremains constant.This indicates term considerations the assimilated carbon also remains availthat dilution with outsideair determinesthe ratio of CH 4 to able as decomposable carbon and might likewiseeventuallybe CO 2 rather than conversion of CH 4 to CO 2. From fluxchamber measurements at several sites on a soil-covered landdissimilated [Doedens, 1985]. The MSW that is collected in West Germany contains fill, Jager and Peters [1985] derived a total methane emission about 20% degradable organic carbon [Tabasaran, 1982; through the top layer that equals 70% of the estimatedCH 4 Stegmann,1978]. This does not include such organic materials production in the landfill. Because of the difficulties that are and in the estimationsof CH 4 as plastics,rubber, and the 30% lignin fraction of wood [Koll- involved in such measurements mann and Cot, 1968], which do not decay at all or only very production rates, we will assumethat all methane that is proslowly [Braun, 1982]. One ton of MSW in West Germany duced in landfills will escapeto the atmosphere. We do, howCelsuis.

BINGEMERAND CRUTZEN.' METHANE FROM SOLID WASTES

2183

TABLE 2.

Content of Biodegradable Components and of Carbon in MSW of Various Regions of the

World

Composition by Weight of Biodegradable Components and

Carbon Industrialized
Carbon Content

in Fresh Countries

MSW

Type of Material
Paper and paperboard
Textiles Wood and straw

in Percent of Fresh Weight

40% C
40% C

OECD
18-42%
7-17% C

USSR and Eastern Europe

-- 16%
6% C

Developing Countries
2-4%
C 1-4% 0.4-1.6% C 1-4% 0.3-1% C 1-2%

30% C*

2% -- 1% C 2-5% --, 1-2% C

3'3/0 -- 1% C --,3% --, 1% C

Garden and park waste

Food waste

17/,,C
15% C

12-18%
2-3% C C

--, 10%
,2% C

20-50%
3-8%

--,45%
--,7%

C
C

40-80%
6-12% C

Range of DOC
in MSW

14-31% C

,, 17% C

8-17% C

Data derived from Cointreau [1984], Bowerman et al. [1977], Environmental ResourcesLtd. [1983], and American Chemical Society [1972]. Data for centrally planned economies are estimated (see text). Specific C contents of waste components are from Mantell [1975], Bowerman et al. [1977], and Suess [1985]. *Excluding lignin C.

ever, not exclude the possibility that the aforementioned studies may not apply to landfills in climates drier than in Germany, under which conditions diffusion of oxygen into the landfill may be more favorable. 3. QUANTITATIVEESTIMATES WASTECARBON OF
DISPOSAL ON LANDFILLS

cluding incineration and compositing) was available from the OECD [1985] and Mantell [1975]. On the average, approximately 85% of the MSW generated in the OECD nations is

landfilled, yielding a total flux of about 56 x 106 T C/yr to

municipal landfills. For the USSR and Eastern Europe, no data were available, so that the MSW generation rates were estimated in the following manner. (1) For the generation of waste paper and paperboard, the weighted average per capita generation rate derived for the OECD countries was scaled down by a factor of 4.2, which is the ratio between the annual per capita production of wood pulp in the OECD nations to that in the USSR and Eastern Europe [United Nations, 1981]. This yields 14 kg of carbon per capita per year (C/cap/yr) of waste paper. (2) For the generation of waste carbon other than paper (e.g., food waste, garden and park waste, textiles, wood) the weighted average generation rate as derived for the OECD nations other than the United States, Canada, and Australia was adopted: 24 kg C/cap/yr. The total DOC generation rate thus adds up to 38 kg C/cap/yr. It is assumedthat 85% of the total

3.1.
In

Municipal Solid Waste

order to estimate the worldwide formation of methane

from municipal wastes it is necessaryto establish the amount of biodegradable carbon that is buried under anaerobic conditions. The amounts generated per capita were obtained from statistics on the generation rates and composition of municipal wastes that are available for many individual countries. These were combined with population data for the individual
countries to obtain estimates of the amount of waste carbon

that is disposed of annually. The waste components that were taken into account and their average content of degradable carbon are given in Table 2. The patterns of municipal refuse generation and composition, also shown in Table 2, show pronounced variations among countries of different socioeconomic backgrounds. Industrialized countries have high waste generation rates, with paper and paperboard as the most significant contributors to degradable carbon. In low- and middle-income developing countries, vegetable wastes dominate the organic fraction. Worldwide waste carbon generation and landfill dumping rates are compiled in Table 3 from data available for 54 individual countries. For the industrialized countries of the west-

15 x 106 T C/yr generatedby 400 million people in these countries disposed at landfills,yieldinga flux of 13 x 106 is of
T C/yr. For the developing countries, MSW generation rates and compositions were available for major cities in all regions from Flintoff [1976], Holmes [1984], Thom-Kozmiensky [1982], Environmental Resources Ltd. [1983], Feachem et al. [1977], Bidhe and $undaresan [1981], and Bidhe et al. [1972]. Because of the sometimes wide scatter among data sets for

ern world, waste generation and composition data were mostly taken from the Organizationfor Economic Cooperation and Development (OECD) [1985] and for the United States also from Bowerman et al. [1977], American Chemical Society [1972], CEQ [1982], and Cointreau [1984]. The annual MSW carbon production derived for the OECD countries totals 66

individual countries,the data were averagedamong neighboring countries with similar economic backgrounds [United Nations, 1981]. For countries for which no data were available, we adopted data available for neighboring countries. Only the generation of organic wastes by the people living in urban environments, 22% of the total population, was considered, since in rural areas, organic wastes are largely used, e.g., vegetables are fed to animals, and wood residues are used as fuel.

x 106 T (1 T (ton)- 1000 kg). Information on the actual

fraction of the MSW that is finally disposed of on land (ex-

In some rural areas of Asia (China, India, Korea), fermentable

2184

BINGEMER AND CRUTZEN: METHANE FROM SOLID WASTES

TABLE 3. Degradable Organic Carbon (DOC) Generation Rates from MSW in the World, Including Estimatesof Quantities Dumped in Landfills
United States, Canada, and Australia USSR and Eastern Europe

Other OECD

Developing Countries

MSW generationrates, kg/cap/d

DOC in MSW

1.8
22 q- 2

0.8
19 q- 3

0.6
17.5

0.5
15 q- 5

% by weight DOC-generation rate, kg C/cap/yr Paper and paperboard generation rate, kg C/cap/yr Other DOC (e.g.,food, textiles, wood) generation rate, kg C/cap/yr Population considered
in millions

148 q- 30
107 q- 23

56 q- 21
32 +__ 16

38
14

27 + 17
11 + 13

41 q- !8

24 +__ 9

24

16 q- 8

272
40
91

47!
26
71

400
15
85

736
20
80

Waste C produced,

106T C/yr
Fraction of MSW

land filled, %

Waste C dumped,

37

19

13

16

106 T C/yr
Per capita rates are weightedaverages; uncertainties representstandarddeviations.Estimateduncertainty of MSW-carbon production is q-30%.

waste is also fed to anaerobic digesters to produce biogas for domestic use.Also, extreme poverty in urban regionsmay lead to extraction of organic waste constituents, which are used as fodder or fuel [Flintoff, 1976]. The urban population statistics
for the individual countries were taken from the United Na-

produce inert wasteslike scrap metal, grit, and sand or slowly biodegradable combustibles like oily sludges, organic chemicals, and solvents.Hazardous wastes are frequently separated from biodegradable wastes to avoid volatilization of toxic substancesor leaching of heavy metals.
For industrial waste, even more than was the case for

tions [1984] yearbook. We assume that in these countries, disposal on land occurs with 80% of the urban waste, although anaerobic conditions may not develop so readily because crude dumping and scavenging often occurs. This

implies that approximately16 x 106 T of the 20 x 106 T of

waste carbon generated in the urban areas in the developing world are dumped on land annually.

Based on the analysisgiven above, 85 x 106 T of biodegradable carbon are depositedannually on landfills worldwide in MSW (Table 3). Based on the observed inconsistenciesbetween the reported statistics on waste C generation rates within and between countries, we roughly estimate the uncertainty of this figure to be about 30%. About 80% of the waste carbon is produced in the developed world, with about half of the waste carbon orginating from paper and paperboard (Table 3).
3.2. Industrial Solid Wastes

There are three types of industrial wastes: (1) wastes that are similar in nature to MSW and frequently collected and disposed of together with MSW, (2) specific production wastes,and (3) hazardous wastes. Most landfilled, biodegradable industrial and commercial waste carbon comesfrom category 1, mostly from offices,can-

MSW, the information on generation, composition, and method of disposal in various countries is sparse and conflicting. Not only do some of the data reported for individual countries disagree strongly among different compilations, but some of the industrial waste streams reported for different countries [Wilson, 1981; OECD, 1985] are inconsistent with the corresponding national industrial production data. These inconsistenciesseem to arise primarily from the fact that the various national inventories were conducted for different purposes (e.g., energy conversion, environmental safety considerations), and consequently, various types of waste materials have been assigned to different categories. Those industrial wastes that are similar to MSW are especially frequently masked in municipal inventories [Mantell, 1975]. In this study, estimates on the production and disposal of industrial biodegradable waste carbon were based on data from Umweltbundesamt [1984] for the Federal Republic of Germany (FRG). These data were extrapolated to other nations on the basis of economic data taken from the United

Nations [1981] and the Food and Atricultural Ortanization (FAO) [-19853. In a compilation of the waste streamsin the FRG, a total of

20.8 x 106 T of MSW is reportedto have been collecteddirectly by the municipalities for 1980 [Umweltbundesamt, 1984], including bulky and commerical wastes. In addition to this, another 11.8 x 106 T of industrial waste that is similar in nature to MSW is delivered directly to the same disposalsites by its producers.The degradablecomponentsin this industrial

teens, supermarkets, etc. For industrial waste in the United States an organic content of 40-76% is reported, with cellulosic material dominating [Mantell, 1975; Anderson, 1977]. In the wastes of category 2, only the food and the wood- and paper-processing industriesproduce putresciblewaste carbon, but due to the concentrated occurrence,a large fraction of the wood residuesis used for fuel. Many manufacturing industries

waste 1.7-3.1 10 T of paperandpaperboard, are x 6 0.9-1.9

x 106 T of food wastes,0.6-1.2 x 106 T of wood, and 0.2-0.6

BINGEMER AND CRUTZEN' METHANE FROM SOLID WASTES

2185

TABLE 4. Generation of Degradable Industrial and Commercial Waste Carbon in the FRG (1980) and Extrapolation to the Industrial
Nations of the World

Waste Category

Paper
Carbon content, % 40

Food
15

Textiles
40

Wood
30

Percentage by weight
in FRG industrial waste

14-26

8-16

2-5

5-10

equal to 480 million tons and that of animal wastes, 175 million tons (dry weight). With a carbon content of about 4045%, the total amount of agricultural waste for the United States alone is already 2.5 times larger than the 113 million tons of waste carbon that are generated worldwide and dumped in landfills (see Tables 3 and 4). Consequently, the anaerobic decay of only a few percent of the agricultural waste carbon worldwide could produce significant quantities of
methane.

FRG production of waste/category,

1.7-3.1

0.9-1.9

0.2-0.6

0.6-1.2

106T/yr
FRG production of waste C/category Consumption in all
industrial nations

In the developed nations, releasefrom concentrated animal wastesis the most likely candidatefor CH, production. Most
of the concentrated animal wastes is first collected in manure

0.7-1.2
14.7

0.1-0.3
18.6

0.1-0.24
35.4

0.18-0.36
37.8

compared with FRG Waste C produced

in all industrial

10-18

3-5

3-8

7-13

ponds and in feedlots,and much of it is later applied to agricultural lands. We do not know of field studies that give significant quantitative information on how much of the organic wastesmay decay anaerobically before application to produce CH,. Studiesare clearly required to addressthis issue.

nations,106 T C/yr
Waste C landfilled 8-15 2-4 3-7 6-11
in all industrial

4.

CONTRIBUTION LANDFILLS GLOBALCH, OF TO

nations,106 T C/yr
Method of extrapolation from FRG data to all industrial nations is based on paper, cotton, and plywood consumption statistics. For food the same per capita waste production (2.3-4.6 kg C/cap/yr) is
assumed.

From the estimates given above, the amount of biodegrad-

able carbon disposed on land in MSW (85 x 106 T C/yr) of and industrialwaste( 28 x 106T C/yr) addsup to approximately 113 x 106 T C/yr at the presenttime. Because imof
perfect statistics, this estimate is uncertain by about 30%. With a production efficiencyof 0.50 kg CH, per kg C, about

x 106 T of textiles.Extrapolationof theseFRG data to the

industrialized world (Table 4) was achieved by multiplying the FRG productions of waste carbon in each category (except for food waste)by the ratio of the total consumption of the specific material in all industrial nations to that in the FRG. This

40-75 x 106 T CH,/yr couldbe produced from landfillsand

waste dumps. As we have discussedbefore, this rate may be biased to the high side by at most 20% due to the relatively slow decomposition of a fraction of the waste carbon. The

global CH production rate may be in the range of 50 + 20

leads us to the following estimatesfor the various categories. 1. For food wastes, the same per capita amount of waste produced in the FRG (2.3-4.6 kg C/cap/yr) is also adopted for
all other industrialized nations. This leads to an industrial

106 T/yr. The uncertainty this estimate in can only be reduced by more detailed studieson CH releasefrom landfills and by better statisticsin different parts of the world. This range of estimates assumes furthermorethat little CH is oxidized in the top layers of the landfills, but that assimilated microbial organic matter and primary waste materials like lignin and plastics do indeed not produce methane. Some studies indicate that these materials may be degradable on very long time scales [Schobert, 1978; Boruff and Buswell,
1934]. It is known that, after a landfill is covered, methane production continuesfor severaldecades,due to slowly decaying waste constituents. Furthermore, we have also assumed that the fraction of CH that is flared off from controlled landfills or is used for energy conversion is negligible on a global scale. The figure for Germany, where controlled landfilling now is the exclusivemethod of disposalon land, may be regarded as an upper limit. Of the 350 large landfills in operation in this country, 30 flare off methane and 40 use it for energy recovery (V. Franzius, personal communication, 1986). The maximum yield of CH extraction for economic use is about 40% of the gas produced in the landfill if the fill is equipped with suitable gas collecting wells (V. Franzius, personal communication, 1986), but much less (,-20%) at those

foodwasteproductionof 3-5 x 106T C/yr.

2. For paper and paperboard, scaled up from the FRG data according to the total paper and paperboard consumption statistics [FAO, 1985], we arrive at a total annual waste

productionof 10-18 x 10 T C/yr in this categoryby the 6

industrialized nations. In a similar way, textile waste generation by the industrialized countries is estimated to be 3-8

x 106 T C/yr, basedon industrialcottonconsumption statistics [United Nations, 1981]. 3. For wood and wood products, the same extrapolation method as for paper and paperboard, based on the plywoodconsumption statistics [FAO, 1985], leads to a production of

7-13 x 106 T C/yr wood and wood product wastesby the

industrialized nations.

The data on industrial waste generation have been compiled in Table 4. We estimate a total generation of biodegradable

industrialand commercialwastesof 23-44 x 106 T C/yr by

the industrialized nations. Assuming the same disposal practices for industrial and commercial wastes as for MSW (i.e., 83-85% landfilled in the industrialized countries), a total of
wastes that are similar in nature to MSW.

fills that simplyflare off the gas.The fraction of CH, burnedis 19-37 x 106 T C/yr may go to landfillsannuallyin industrial thus 6% at best for Germany, but much smaller for other
countries.

The CH release rates derived in this work are much

3.3. Agricultural Wastes Very large amounts of organic matter are produced in agriculture. According to the Biomass Panel of the Energy Research Advisory Board (ERAB) [1983] the amount of crop residues presently generated in the United States is about

smallerthan the flux of 170 x 106 T/yr published Sheppard by

et al. [1982]. Becausethese authors extrapolated estimatesof Wilson [1977] for the United States to the world by total population ratios, it is clear that their estimate must be much too high.

2186

BINGEMER AND CRUTZEN.' METHANE FROM SOLID WASTES

MSW disposalhas been increasingrapidly in the industrial nations,especially the 1960'sby 5%/yr and in the 1970'sby in 2%/yr [CEQ, 1982], but is currently stagnating in many
countries [Urnweltbundesarnt, 1984; OECD, 1985]. Due to

time lags in the decay rates of a fraction of the organic matter,

the emission of methane from landfills in the industrialized

Pollution Control International Limited, Aylesbury, England; G. Rettenberger and K. S. Shin, Institute fiir Siedlungswasserbau, Wassergfite und Abfallwirtschaft, University of Stuttgart; and J. Darmstadter, Resources, Energy and Materials Division, Washington D.C. The contribution of two anonymous reviewers is gratefully acknowledged.
REFERENCES

nations is probably still growing. The projection for the developing countries suggests doua bling of MSW generation by the year 2000 due to increasing populations and urbanization [Kresse and Ringeltaube, 1982], This trend is likely to continue for the foreseeablefuture. With this trend, MSW generation may become one of the most important sourcesof methane in the next century.
5. CONCLUSIONS

American Chemical Society,Solid Waste II, Washington, D.C., 1972. Anderson, L. L., A wealth of waste, a shortage of energy, in Fuels From Waste, edited by L. L. Anderson and D. A. Tillmann, Academic, Orlando, Fla., 1977. Bidhe, A.D., and B. B. Sundaresan,Solid waste management in developing countries,210 pp., Natl. Environ. Eng. Res. Inst., Nagpur,
India, 1981. Bidhe, A.D., B. Z. Alone, S. K. Titus, R. C. Trivedi, and J. M. Dave,

Quality and quantity of refusefrom Calcutta City, Indian d. Environ. Health, 14, 80-87, 1972.

Methane formation from the anaerobic decay of municipal and industrial organic matter that is collectedand dumped in

Blake, D. R., and F. S. Rowland, World-wide increasein tropospheric

methane, J. Atmos. Chem., 4, 43-62, 1986.

landfillsmay add 30-70 x 106 T CH, per year to the atmosphere and therefore constitutesa significant fraction (6-18%)
of the estimated total emission of methane at the earth's sur-

Boruff, C. S., and A.M. Buswell, The anaerobic fermentation of lignin, J. Am. Chem.,56, 886-888, 1934. Bowerman, F. B., N. K. Rohatgi, K. Y. Chen, and R. A. Lockwood, A

case study of the Los AngelesCounty sanitation districts Palos Verdes landfill gas development project, EPA-600/3-77-047, U.S. face. By far the largest contribution currently comes from Environ. Prot. Agency,Cincinnati, Ohio, 1977. landfills in the industrialized world. This source of atmospher- Braun, R., Biogas-MethangiirungorganischerAbfallstoffe, 204 pp., Springer,Wien, 1982. ic methane has been increasingstrongly over the past decades. However, becausewaste dumping rates in the industrialized Chameides, W. L., and J. C. G. Walker, A photochemical theory of troposphericozone,J. Geophys. Res., 78, 8751-8760, 1973.

world are now almost stagnating, we expect this growth to stop in the next decade.On the other hand, becauseof strong population growths and increasing urbanization, very large increases in methane production from waste dumps are expected in the coming decades from the developing world. Consequently,methaneproduction from municipal and industrial wastes could become one of the main contributors to the

Cicerone, R. J., J. D. Shetter, and C. C. Delwiche, Seasonal variation of methane flux from a Californian rice paddy, J. Geophys.Res.,
88,11,022-11,024, 1983.

global atmospheric methane budget. Increased recovery of methane gas in landfills and in biggas generators may not only provide an economic energy source,but will also reduce global air pollution significantly. Table 1 shows a compilation of what is currently estimated
about the sourcesand sinks of atmospheric methane. We note

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that CH, production in landfills may be larger than the release from coal mining and natural gas leaks. It may approach methane production by domestic animals (especially cows), various NO x sourceson troposphericozone, J. Geophys. Res., which is about 70-80 x 106 T/yr. The contribution from 88(Cll), 6641-6661, 1983. biomas burning in the tropics is uncertain becauseof insuffiCrutzen, P. J., and U. Schmailzl, Chemical budgets of the stratocient knowledge about the amounts of biomass that are sphere,Planet. SpaceSci.,31, 1009-1032, 1983. burned annually and the efficiency of methane production. Crutzen, P. J., I. Aselmann, and W. Seiler, Methane production by

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Bestcurrentestimates in the rangeof 30-100 x 106T/yr. are

Although natural wetlands at high latitudes may releasesubstantial quantities of methane to the atmosphere [Harriss et al., 1985; Sebacheret al., 1986], model calculations by Crutzen and Gidel [1983] suggest that the largest contributions of methane to the atmosphere must come from the wet tropics. The production of methane from rice fields and tropical wetlands may yield the largest contributions [Cicerone et al., 1983; Holzapfel-Pschornand Seiler, 1986]. Field observations in the tropics are required to addressthis important and interesting question.
Acknowledgments. We are very grateful to K. H. Friederichs, chairman of the Working Group "Environmental Engineering" of the German Engineers Association (VDI) in Miinster, West Germany, who first drew our attention to the potential significanceof landfill emissionsfor the atmospheric budget of methane. We further would like to thank the following scientistsfor providing us with valuable information, which was used in the preparation of this article: M. Betts, Environmental Resources Limited, London; V. Franzius, G. Goosmann, and H. Lie, Umweltbundesamt, Berlin; J. R. Holmes,

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H. G. Bingemerand P. J. Crutzen, Max Planck Institute for Chemistry, P.O. Box 3060, D-6500 Mainz, Federal Republicof Germany.
(Received August 1, 1986;
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accepted November 12, 1986.)