Environ Monit Assess (2010) 166:529541 DOI 10.

1007/s10661-009-1021-7

Greenhouse gas emissions from Australian open-cut coal mines: contribution from spontaneous combustion and low-temperature oxidation
Stuart J. Day John N. Carras Robyn Fry David J. Williams

Received: 1 March 2009 / Accepted: 26 May 2009 / Published online: 27 June 2009 Springer Science + Business Media B.V. 2009

Abstract Spontaneous combustion and lowtemperature oxidation of waste coal and other carbonaceous material at open-cut coal mines are potentially signicant sources of greenhouse gas emissions. However, the magnitude of these emissions is largely unknown. In this study, emissions from spontaneous combustion and low-temperature oxidation were estimated for six Australian open-cut coal mines with annual coal production ranging from 1.7 to more than 16 Mt. Greenhouse emissions from all other sources at these mines were also estimated and compared to those from spontaneous combustion and low-temperature oxidation. In all cases, fugitive emission of methane was the largest source of greenhouse gas; however, in some mines, spontaneous combustion accounted for almost a third of all emissions. For one mine, it was estimated that emissions from spontaneous combustion were around 250,000 t CO2 -e per annum. The contribution from low-temperature oxidation was generally less than about 1% of the total for all six mines. Estimating areas of spoil affected by spontaneous combustion by ground-based surveys was prone to under-report the area.

Airborne infrared imaging appears to be a more reliable method. Keywords Coal mining Spontaneous combustion Greenhouse gas emissions Coal oxidation Infrared thermography

Introduction In Australia, coal mining is a signicant source of greenhouse gases. During 2006, emissions from the coal mining industry (both underground and open-cut) were estimated to contribute around 6% of the nations total emissions (Australian Dept of Climate Change 2008a). Slightly more than half of these emissions were attributed to fugitive emissions of methane, which is released as the coal is mined, while most of the remainder resulted from energy usage. Open-cut mining also produces large quantities of carbonaceous waste material, which, when exposed to air, is subject to low-temperature oxidation and, in some cases, spontaneous combustion. These processes produce CO2 and other gases, including methane, and therefore represent a potential additional source of greenhouse emissions. Worldwide, the signicance of emissions from coal res is well known (Stracher and Taylor 2004; Kuenzer et al. 2007), but quantitative data on the scale of these emissions are rare. In a study of

S. J. Day (B) J. N. Carras R. Fry D. J. Williams CSIRO Energy Technology, PO Box 330, Newcastle, NSW 2300, Australia e-mail: stuart.day@csiro.au

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greenhouse emissions from the Australian coal industry, Williams et al. (1998) suggested that up to 25% of the total greenhouse emissions from an open-cut mine may be derived from spontaneous combustion and low-temperature oxidation; however, this estimate was based on very limited data. The Intergovernmental Panel on Climate Change recognises the potential of lowtemperature oxidation and spontaneous combustion as a source of greenhouse gases, but at present, there is no recognised method for making reliable estimates. As a consequence, emissions from this source are not presently included in the Australian National Greenhouse Gas Inventory. However, with the likely introduction of an emissions trading scheme in Australia, it is becoming increasingly important to be able to account for all sources of emissions. Apart from the Williams et al. (1998) report, we are unaware of any other published estimates of greenhouse emissions from spontaneous combustion and low-temperature oxidation at the individual mine level. Hence, the scale of these emissions is largely unknown. Accordingly, research into developing a tractable methodology for estimating emissions has been conducted in Australia over the past decade. Carras et al. (2009), for instance, recently reported results of a study conducted at 11 Australian open-cut coal mines where emissions of CO2 and CH4 from low-temperature oxidation and spontaneous combustion in spoil and other waste were measured using ux chambers. In that study, emissions were categorised according to the intensity of spontaneous combustion, and despite considerable scatter in the data, three broad categories of spontaneous combustion were identied. Each category was assigned an emission factor ranging from about 12 to 8,200 kg CO2 -e year1 m2 . With appropriate classication of the affected ground, these emission factors provide the basis for estimating emissions from spontaneous combustion and low-temperature oxidation of coal wastes. Other work has investigated the use of airborne infrared thermography to measure the surface temperature of spoil piles (Carras et al. 2002). This, combined with the nding that the emission ux is roughly proportional to the surface temperature (Carras et al. 2009), also provides a potential

method for estimating emissions over relatively large areas. To date, however, these methods have not been applied to quantify emissions from individual mines. In the study reported in this paper, estimates of emissions from spontaneous combustion and low-temperature oxidation of waste material were made for a number of operating open-cut coal mines in Australia using the methods developed by Carras et al. (2002, 2009). To place these estimates into context, emission data from all other sources at each mine were also considered and compared with the estimates made for spontaneous combustion and low-temperature oxidation.

Methodology Greenhouse gas emission data were analysed from six open-cut coal mines located in two of Australias major coal producing regions: four in the Hunter Valley in New South Wales (NSW) and two in the Bowen Basin in Queensland. Annual production of run-of-mine (ROM) coal from these mines ranged from approximately 1.7 Mt to more than 16 Mt. Mines were selected to include those with low, medium and severe occurrences of spontaneous combustion. Data on electricity, fuel and explosives consumption, land clearing, fugitive emissions and other sources of greenhouse gas sources were obtained from each mine. Information on the extent and severity of spontaneous combustion was also collected. For two of the mines selected, infrared data from the Carras et al. (2002) study were available, which were also used to estimate spontaneous combustion derived emissions from these mines. The data were collated to show the relative contribution from each source compared to the total greenhouse emissions from individual mines. Details on the data collection and analysis are discussed in the following sections. Electricity, fuel and explosives Open-cut coal mines operate a range of electrically powered equipment, which may include

Environ Monit Assess (2010) 166:529541 Table 1 Emission factors used for estimating greenhouse gas emissions from electricity, diesel, waste and explosives Source Electricity NSW Queensland Diesel Waste to landll Explosives ANFO Heavy ANFO Emulsion Emission factor 1.068 t CO2 -e MWh1 1.046 t CO2 -e MWh1 3.0 t CO2 -e kL1 0.9 t CO2 -e t1 0.17 CO2 -e t1 0.18 t CO2 -e t1 0.17 t CO2 -e t1

531

draglines, electric shovels and conveyors. Many mines also have coal preparation plants on site, which are large consumers of electricity. In addition to the electrical equipment, substantial eets of diesel-powered machinery, such as haul trucks, bulldozers and drilling rigs, are maintained. Emissions from electricity and diesel consumption were estimated by multiplying the activity (i.e. the megawatt hour of electricity or kiloliter of diesel used) by an appropriate emission factor. The emission factors used for electricity and diesel are shown in Table 1 (Australian Dept of Climate Change 2008b). Explosives based on ammonium nitrate and fuel oil (ANFO) mixtures are used universally throughout the Australian coal mining industry. These explosives contain approximately 6% fuel oil and produce about 170 kg of CO2 per tonne of explosive, depending on the formulation. The emission factors for the most commonly used explosives are shown in Table 1 (Australian Dept of Climate Change 2008b). Land clearing Land clearing is a necessary consequence of mining and therefore contributes to the greenhouse footprint of mines. To estimate emissions due to land clearing, it is necessary to know both the area of land cleared and an emission factor appropriate for the type of vegetation removed. The emission factor must take into account the amount of carbon in the biomass and the fate of the carbon released. The simplest case is to assume that all of the carbon is released as CO2 during the year of clearing.

Most mines were able to provide the area of land disturbed each year but usually did not have specic information relating to the type or amount of vegetation removed. Three of the mines surveyed (two in NSW and one in Queensland) did, however, make their own estimates of emissions due to land clearing using an emission factor supplied by their respective parent company. These emission factors were 165 t CO2 ha1 for NSW and 99 t CO2 ha1 for Queensland. There have been studies in central Queensland where the amount of biomass in eucalypt woodlands, typical of the Bowen Basin where the coal mines are located, has been measured, and it is interesting to compare the results with the emission factors used by the three mines. Burrows et al. (2000) found that the average biomass density of eucalypt woodland across 33 central Queensland sites was 5.86 t m2 of tree basal area. They also found that the average basal area over these sites was 12.0 m2 ha1 . Assuming a carbon fraction of 0.5 for the biomass (Burrows et al. 2002), this equates to an emission factor of about 129 t CO2 ha1 , which compares reasonably well with the factors used by the three mines. Thus, in the absence of mine-specic data, we applied the emission factors used by the mines to calculate the emissions due to land clearing from the other mines included in this study. General waste Most of the mines examined generate a certain amount of general waste material that is sent to landll. An emission factor of 0.9 t CO2 -e per tonne of waste was applied to estimate emissions from this source (Australian Dept of Climate Change 2008b). Fugitive emissions from seam gas Fugitive emissions of methane and, to a lesser extent, CO2 represent a large proportion of greenhouse gas emissions from the Australian coal mining industry. For open-cut mining, however, these emissions are not readily measured. Sagha et al. (2008) recently proposed a method for estimating fugitive emissions from individual mines; however, at present, there are insufcient data

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4000 3500

available for most Australian mines to allow reliable estimates to be made. Consequently, estimates of fugitive emissions were made by multiplying the annual ROM coal production by an emission factor. This is the method currently used for compiling the Australian National Greenhouse Gas Inventory. For NSW, the emission factor is 2.17 kg t1 CH4 (45.5 kg t1 CO2 -e), while for Queensland, it is 0.81 kg t1 CH4 (17.1 kg t1 CO2 -e; Australian Dept of Climate Change 2008b). Although these emission factors have high uncertainties, we used this methodology to ensure consistency for all the mines studied. Emissions from spontaneous combustion and low-temperature oxidation Spontaneous combustionground measurements Emissions from spontaneous combustion were initially estimated by determining the area of ground affected by spontaneous combustion and applying an emission factor based on the work of Carras et al. (2009). Those authors observed a correlation between the surface temperature of a spoil pile and surface emission rate. While acknowledging that the surface temperature can at best be a crude measure of spontaneous combustion activity within a spoil pile and that the emissions are also governed by the nature of the topmost layers of spoil, the authors nevertheless found a useful relationship. This is shown in Fig. 1 (from Carras et al. 2009). Methane is often formed and emitted during spontaneous combustion, and the emission factors developed by Carras et al. (2009) took this into account. Linear regression of the data presented in Fig. 1 yielded the empirical expression shown in Eq. 1, where the emission rate, ER, in units of kg CO2 -e year1 m2 is related to the surface temperature, T ( C), by the expression: ER = 59.6T 496.4 (1)

CO2-e Emissions (kg y-1 m-2)

3000 2500 2000 1500 1000 500 0 0 10 20 30 40 50 60

Temparture (oC)

Fig. 1 Average emission rates from spoil affected by spontaneous combustion (as CO2 -equivalent) as a function of average surface temperature (from Carras et al. 2009)

which there are no emissions). Applying Eq. 1 to datasets measured when the threshold temperature is signicantly different, such as during summer months, may substantially over- or underestimate emissions. Hence, care was taken to ensure that ground temperature measurements were made in the early morning during winter months. Estimates of the area of ground (in square meter) affected by spontaneous combustion in each mine were made by visual inspection and the intensity categorised as either minor or major according to the following criteria: Minoractive spontaneous combustion with less obvious signs Surface discolouration No large cracks Little smoke or steam

Majoractive spontaneous combustion with marked surface signs Large cracks with obvious signs of gas venting Smoke and steam Hot gases Surface discolouration

Equation 1 is based on measurements made when the ambient temperature of unaffected ground was about 9 C (i.e., threshold temperature below

This information was gathered during site visits to mines and detailed discussions with mine personnel. Because of statutory environmental licensing obligations, a number of the mines already collect

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this information through regular ground surveys and prepare maps showing the area and intensity of heating within the mine. Where available, these data were used for estimating the area and severity of spontaneous combustion. During site visits, surface temperatures were measured at various locations showing signs of spontaneous combustion. In areas classied as minor, the ground temperature was less than about 10 C above unaffected ground so, from Fig. 1, an emission factor of 500 kg year1 m2 was applied. Major outbreaks typically had temperatures of 60 C or more, and this category was assigned an emission factor of 3,000 kg year1 m2 . There is, of course, a continuum between the categories, and it is recognised that this approach is only an approximation at best. Spontaneous combustionairborne measurements An alternative, potentially more accurate approach to determining the extent and intensity of heating across mines in the Hunter Valley has been investigated previously using airborne infrared thermography (Carras et al. 2002). Data from that study, which were collected during September 2000, were available for two of the mines included in the current study. These data were used in the present study to determine both the surface temperature and area of the ground undergoing heating at each of these mines. The infrared data were obtained with a Daedalus 1268 airborne thematic mapper system tted to a Cessna 414A aircraft. Measurements were made using bands 11 and 12 of the instrument covering a wavelength range of 814 m. To minimise the effects of solar radiation and maximise the thermal contrast, data were collected before dawn during winter months in cloudless, windless conditions. The ground temperature in areas unaffected by spontaneous combustion was below 10 C (i.e., comparable to the threshold temperature inferred by Eq. 1). Data were recorded by the scanner as pixels and assigned an integer value ranging from 0 to 255. The numerical value of each pixel was related to ground temperature according to a calibration function established by a series of ground-

truthing temperature measurements made at the time of the ight. The resolution of the thermal images was such that each pixel corresponded to an area on the ground of about 7 7 m. Data from the airborne scanner were analysed with Terrascan software (Resource Imaging Australia). Using the ground temperatures derived from the infrared data and Eq. 1, emissions from the two NSW mines covered by the airborne infrared survey were calculated and compared to the ground-based method described above. Low-temperature oxidation Low-temperature oxidation of waste coal in spoil piles was considered in detail by Carras et al. (2009). Using the results of laboratory measurements of oxidation rates of coal and carbonaceous material as well as numerical modelling, they calculated greenhouse gas emission rates from mining waste for a range of carbon contents and temperatures. They found that the emission rates from a variety of sources, including bare spoil, revegetated spoil, uncovered tailings, uncovered reject, natural forest oor and suburban lawn, were all similar. From this, they suggested that greenhouse emissions of CO2 from rehabilitated spoil, with no spontaneous combustion, could not be distinguished from other natural land surfaces, although they also indicated that further work would be required to disentangle the biogenic and coal-based contributions. For the purpose of the current study, we assumed that the average temperature and carbon content of the spoil were 27 C and 5%, respectively. According to the results of Carras et al. (2009), this yields an emission factor of 2.2 kg year1 m2 , which was applied to lowtemperature oxidation from uncovered spoil, tailings or reject with no spontaneous combustion. To estimate the contribution from lowtemperature oxidation, it is also necessary to know the surface area of exposed spoil. Aerial photographs of mines A, B, C, and D indicated that the spoil areas were roughly 4, 4, 0.5, and 2 km2 , respectively. Photographs for mines E and F were not available so the exposed spoil area was assumed to be 3 km2 in each case since they were about three quarters the size of mines A and B.

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Table 2 Summary of the greenhouse gas emission data for the six open-cut coal mines B 16.8 1.7 C

Mine

ROM Production (Mt pa)

16.8

Emissions Specic emissions Percent Emissions Specic emissions Percent Emissions Specic emissions Percent (t CO2 -e year1 ) (kg CO2 -e year1 t1 ) of total (t CO2 -e year1 ) (kg CO2 -e year1 t1 ) of total (t CO2 -e year1 ) (kg CO2 -e year1 t1 ) of total 10.2 6.7 0.4 45.5 0.0 0.6 0.0 0.5 63.9 E 12.2 100.0 1,097,802 65.4 100.0 129,459 F 13.1 16.0 10.4 0.6 71.2 0.0 0.9 0.1 0.8 130,910 164,412 6,390 763,663 661 22,935 0 8,830 7.8 9.8 0.4 45.5 0.0 1.4 0.0 0.5 11.9 15.0 0.6 69.6 0.1 2.1 0.0 0.8 3,886 16,142 584 76,518 Not assessed Not assessed 42,723 1,104 2.3 9.6 0.3 45.5 2.8 11.5 0.4 54.3

Electricity 171,820 Fuel 111,568 Explosives 6857 Fugitives 763,240 Waste 401 Land clearing 9,405 Spon Com 568 Low temp 8,830 oxidation Total 1,072,689

25.4 0.7 83.9

30.3 0.8 100.0

Mine

ROM Production (Mt pa)

7.3

Emissions Specic emissions Percent Emissions Specic emissions Percent Emissions Specic emissions Percent (t CO2 -e year1 ) (kg CO2 -e year1 t1 ) of total (t CO2 -e year1 ) (kg CO2 -e year1 t1 ) of total (t CO2 -e year1 ) (kg CO2 -e year1 t1 ) of total 7.7 16.2 0.4 45.5 4.4 34.5 0.6 109.4 100.0 4.0 31.5 0.6 7.0 14.8 0.4 41.7 47,271 30,115 1,790 209,133 550 7,227 78,750 6,623 381,458 3.9 2.5 0.1 17.1 0.0 0.6 6.4 0.5 31.2 12.4 7.9 0.5 54.8 0.1 1.9 20.6 1.7 100.0 205,083 140,773 6,368 223,350 371 27,423 3,000 6,623 612,990 15.7 10.8 0.5 17.1 0.0 2.1 0.2 0.5 46.9 33.5 23.0 1.0 36.4 0.1 4.5 0.5 1.1 100.0

Electricity Fuel Explosives Fugitives Waste Land clearing Spon Com Low temp oxidation Total

56,222 118,490 2,882 332,661 Not assessed 32,175 251,504 4,415

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798,350

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Results The results of the greenhouse gas emissions estimates for each of the six mines are shown in Table 2. Emissions from each source are expressed as t CO2 -e per year and also as a specic emission where the emissions have been normalised to the annual ROM coal production (expressed as kg CO2 -e year1 t1 ). The specic emissions for each mine are plotted in Fig. 2 (emissions from waste to land ll have been omitted since, in all cases, it contributed less than 0.1% of the total). The percentage contribution from the various sources relative to each mines total annual emissions are also listed in Table 2 and plotted in Fig. 3. The results for individual mines are discussed in more detail below. Mine A is a large Hunter Valley mine with an annual production of around 16 Mt of ROM coal. Spontaneous combustion is comparatively rare at this mine, with only a few small outbreaks occurring from time to time in reject dumps and disused tailings emplacements. The total area that was thought to have had occurrences of heating in the past was estimated to be about 20,000 m2 .

However, because there was no sign of active spontaneous combustion anywhere on the mine, an emission factor of 500 kg CO2 -e year1 m2 was considered to be too large for the intensity of heating present. Instead, an estimate of emissions due to spontaneous combustion was made by assuming that all of this area corresponded to the lowest category for rejects and tailings as dened by Carras et al. (2009), i.e. 28.4 kg CO2 -e year1 m2 . Fugitive emissions from mine A represent nearly three quarters of the mines total greenhouse gas emissions, but, as noted previously, this estimate is subject to a large uncertainty. Most of the remaining emissions originate from electricity and fuel usage, which together comprise about 27% of the total. Not surprisingly, spontaneous combustion contributes only about 0.1% to the total. Low-temperature oxidation of waste coal in the spoil contributes about 1% of the total greenhouse emissions from the mine. Similar results were obtained for mine B, which is also in the Hunter Valley and has around the same annual output as mine A. There are no known outbreaks of spontaneous combustion at mine B. Again, fugitive emissions comprise

Specific Emission (kg CO2-e y t )

Fig. 2 Specic greenhouse gas emissions (i.e., emissions normalised to the annual ROM coal production) attributed to the main sources for the six mines. Note that waste to landll has been omitted for the sake of clarity

50 Mine A Mine B Mine C Mine D Mine E Mine F

-1 -1

40

30

20

10

0
ity g El ec tri c Sp on O xi da tio n p Te m Lo w Fu el Fu gi tiv es ive s C le ar in pl os C om

Ex

La nd

536 Fig. 3 Greenhouse gas emissions expressed as a percentage of the total emissions from individual mines

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Greenhouse Emissions (% of Mine's Total)

100

80

60

40

20

0 Mine A Mine B Mine C Mine D Mine E Mine F

Mine
Electricty Fuel Explosives Fugitives Land Clearing Spon Com Low Temp Ox

the bulk of greenhouse emissions, while energyrelated emissions make up slightly more than a quarter of the total. Compared to the other mines studied, mine C, which is located in the Hunter Valley, is relatively small and produces around 1.7 Mt of ROM coal annually. The contribution from land clearing was not assessed for mine C, but since this mine disturbs little fresh ground, it is unlikely to contribute signicantly to the mines total greenhouse emissions. Mine C has, for many years, been affected by moderate spontaneous combustion throughout the site. It is apparent from Figs. 2 and 3 that the proportion of energy-related emissions derived from electricity is relatively low in mine C compared to other mines. This is because mine C uses mostly diesel powered equipment in their mining operations; the other mines use large electrically powered draglines and shovels. Fugitive emissions accounted about 76,000 t CO2 -e, about 55% of the total greenhouse gas emission from the mine. Ground-based assessments of the spontaneous combustion at Mine C yielded areas of 9,950 m2 for the minor and 8,750 m2 for the major categories. On this basis, emissions from spontaneous

combustion were calculated to be approximately 31,000 t CO2 -e. As well as the ground-based survey of spontaneous combustion, an infrared image of mine C (Carras et al. 2002) was used to estimate emissions. Figure 4 shows the infrared image of mine C; areas with elevated surface temperatures are shown in lighter shades. Data from the infrared image were used to measure the area and temperature of ground showing signs of heating, from which CO2 -e emissions for the mine were calculated (Table 3). The area of heat-affected ground estimated from the thermography data was approximately 41,000 m2 , more than twice that estimated by a ground survey. Spontaneous combustion-related greenhouse gas emissions based on this value and Eq. 1 were around 43,000 t CO2 -e y1 , about 50% higher than the value determined from the ground survey data. This is equivalent to a specic emission of 25.4 kg CO2 t1 year1 or around 30% of the total greenhouse gas emission. The difference between the two methods is the result of ground surveys tending to underestimate the area because they rely on some form of surface expression to identify that spontaneous

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Fig. 4 Infrared image of mine C. The surface resolution of the image is about 7 m

combustion is present. Thermography, on the other hand, is more sensitive to detecting even small changes in surface temperature that may not be associated with visible manifestations. Mine D regularly surveys the area of the mine that is affected by spontaneous combustion. During 2003, the area of spontaneous combustion was monitored each month and found to range from about 650 to 2,500 m2 , with an average value for the year of 1,326 m2 . Information on the severity was not available so a 50:50 minor/major split was assumed. On this basis, the emissions attributed to spontaneous combustion were very low, representing only about 0.4% of the total from the mine.

Infrared data from the study of Carras et al. (2002) were also available for mine D, so emissions were estimated using the same technique applied to mine C. The area affected by spontaneous combustion and associated emissions determined by airborne thermography for mine D are listed in Table 3. Using the infrared data yielded an area of about 22 ha of heat affected ground, which is more than a factor of 160 higher than that determined by the ground survey. Accordingly, the greenhouse gas emissions determined by this method were much higher, totalling more than 250,000 t CO2 -e. This represents approximately 30% of the mines total annual greenhouse emissions. Although the infrared survey of mine D was made several years before the ground-based estimate, it is unlikely that the large discrepancy between the two methods can be accounted for by improved spontaneous combustion management at the mine (such as covering active areas with inert material). Results of ground measurements made at the time of the airborne survey indicated that the area of affected ground was even less than the 1,326 m2 used in these calculations. It seems that most of the spoil undergoing heating at mine D is not readily detected by visible inspection. The estimate for Mine D based on the infrared data compares well to measurements made during the late 1990s by CSIRO (unpublished data). In that instance, plumes of CO2 originating from mine D (and an adjacent mine which also has spontaneous combustion) were traversed in an instrumented vehicle, which measured the CO2 concentration in the plumes. Local meteorological data and a plume model were then used to infer the ux of CO2 emitted from the

Table 3 Surface temperature and area of ground affected by spontaneous combustion and associated emissions in mines C and D determined by airborne thermography

Average temperature ( C) 17.5 22.5 27.5 32.5 37.5 42.5 Total

Mine C Area (m2 ) 16,660 8,869 3,969 2,793 1,617 7,252 41,160 Emissions (t CO2 -e year1 ) 9,103 7,488 4,534 4,022 2,811 14,765 42,723

Mine D Area (m2 ) 73,500 45,080 27,293 21,266 14,259 42,581 223,979 Emissions (t CO2 -e year1 ) 40,160 38,062 31,175 30,627 24,784 86,696 251,504

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mine site. This technique yielded an emission estimate of up to 260,000 t CO2 -e year1 . This value, however, may be an overestimation since it also included emissions from vehicles and other equipment operating on the mine site at the time of the measurements. Overall specic emissions for mine D were the highest of the six mines at 109.4 kg CO2 -e t1 y1 . Mine E, located in the Bowen Basin, is a large mine producing about 12 Mt of thermal coal per annum. The coal is subject to spontaneous combustion, and there are numerous outbreaks in waste material throughout the mine. There are also old underground workings on the mine lease, which are prone to spontaneously combust as the open-cut operations uncover the old shafts. Table 2 shows that the electricity and diesel usage in this mine were the lowest of all six mines; the combined electricity and diesel contribution to greenhouse gas emissions amounted to 6.4 kg CO2 -e t1 year1 . This compares to the next lowest mine (mine C) with nearly twice that emission and the highest, mine F, at 26.5 kg CO2 -e t1 year1 . The reason for the large differences is that the amount of material moved to produce the coal varies considerably from mine to mine. In the case of mine E, which has a very low stripping ratio (i.e. the ratio of the volume of overburden to the volume of coal), the total amount of material moved is only about a third of that at mines A and B. The amount of energy required to extract the coal is therefore correspondingly lower. The total area of the mine affected by spontaneous combustion was estimated to be between about 30,000 and 40,000 m2 with about 30% classed as minor (500 kg CO2 -e y1 m2 ) and 70% major (3,000 kg CO2 -e year1 m2 ). Infrared imagery of this mine was not available, but based on the experience of mines C and D, it is possible that this is less than the actual area of spoil with elevated surface temperatures. Assuming an average area of 35,000 m2 of active spontaneous combustion, the total annual emission equates to around 79,000 t CO2 -e (6.4 kg CO2 -e year1 t1 ). This represents around 20% of the mines total emissions. Due to the relatively low energy requirements and the lower emission factor for fugitive emissions of seam gas from Queensland mines, specic

emissions (from all sources) at mine E were the lowest (31 kg CO2 -e year1 t1 ) of all the mines surveyed. Mine F is located in the Bowen Basin and produces about 13 Mt of ROM coal annually. In this mine, the amount of material moved to produce a tonne of coal is high, and this is reected in the higher energy usage compared to the other mines. The combined CO2 emissions for electricity and fuel of 26.5 kg CO2 -e year1 t1 was the highest of the six mines and accounted for more than half of the mines total emissions. Mine F has relatively few occurrences of spontaneous combustion, all of which can be classied as minor. The total area of affected ground was estimated to be around 6,000 m2 . Using this information (but bearing in mind the problems associated with estimating the area of spoil undergoing spontaneous combustion by ground surveys), emissions from spontaneous combustion at mine F were estimated to be 3,000 t CO2 -e per year or about 0.5% of the mines total greenhouse gas emissions.

Discussion The eight sources of greenhouse gases examined in this study account for the bulk of the greenhouse emissions from open-cut mining; however, before considering the magnitude of these estimates, it is worthwhile discussing the associated uncertainties. The most reliable estimates are those for electricity and fuel usage since the activities are measured accurately for billing purposes and the emission factors are well established. Emissions from explosives are also reasonably accurate because consumption is closely monitored and robust emission factors, determined by assuming that the fuel oil in the ANFO mixture is burnt to produce CO2 , are used. Although other gases may be produced during blasting, most of the carbon in the fuel oil is converted to CO2 with only relatively small quantities of CO and hydrocarbons formed under some conditions (Attalla et al. 2008). The uncertainty for energy-derived emission estimates (which includes explosives) is probably less than 5% (Leung 2002).

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Emissions from waste sent to landll are poorly dened, but since they comprise only a very small proportion of each mines total emission, even large errors in the waste component have very little effect on the overall estimate. Similarly, land clearing is subject to moderate uncertainty, but the overall effect of these errors is low because the contribution accounts for no more than a few per cent of the total. Fugitive emissions of seam gas, on the other hand, represent the largest source of greenhouse gas emissions from open-cut coal mining, but the uncertainty associated with fugitive emissions estimates is very high. Leung (2002) suggested that the uncertainty on open-cut fugitives was 50%, while Williams et al. (1998) considered that it may be as high as a factor of two. Consequently, estimates of total greenhouse gas emissions from individual mines have a relatively high uncertainty because of the strong contribution from fugitive emissions. Recent work by Sagha et al. (2008) has resulted in the development of a method to directly measure fugitive emissions from individual open-cut coal mines and with sufcient data, this methodology may substantially reduce the uncertainty of these estimates. Spontaneous combustion emission estimates are also subject to high uncertainty. The emission factors and the emission/temperature relationship developed by Carras et al. (2009) have, in themselves, signicant uncertainty as evidenced by the scatter in measurements on which they are based (Fig. 1). In addition, there are a number of practical problems that compound this uncertainty. In the methodology used in this study, it is necessary to know the area of the spoil affected by spontaneous combustion, which is difcult to measure accurately, especially at ground level. The results of this study suggest that ground-based surveys underestimate the area, in some cases

by very large margins. This is probably because ground surveys rely on detecting visible surface expressions of spontaneous combustion; less obvious signs may be overlooked. As well, physical access to parts of spoil piles is often very difcult or impossible due to operational and safety factors. Airborne infrared thermography appears to be capable of providing better area estimates and also has the advantage of being able to measure the surface temperature of the spoil piles. However, care must be taken when interpreting the results of the infrared surveys to infer ground temperatures. The radiation measured by the infrared sensor is dependent on both the thermodynamic temperature of the surface and its emissivity. Emissivity is wavelength-dependent but also depends on the nature of the emitter. Since different substances have different emissivities, for a given thermodynamic temperature, the apparent temperatures inferred from the infrared data will vary accordingly. Accurate temperature values therefore depend on accurate knowledge of the emissivities of the materials. Carras et al. (2002) suggested that the uncertainty of the emissivity meant that surface temperatures could only be determined to about 3 C. This has implications when using ground temperatures derived from infrared data to estimate greenhouse gas emissions. Carras et al. (2002) showed that the method is very sensitive to the temperature below which emissions are assumed to be zero. Since a large proportion of the emissions are associated with relatively low temperatures, variations of even a few degrees in this threshold temperature can make a substantial difference to the emission estimate. Notwithstanding the uncertainties discussed above, the emission estimates are based on actual mine data and provide some indication of

Table 4 Equivalent amount of ROM coal that would have to be burnt to produce the spontaneous combustion estimates for each mine Mine A Annual spontaneous combustion emission (t CO2 -e) ROM coal equivalent (t) Per cent of annual production 568 221 0 Mine B 0 0 0 Mine C 31,225 12,166 0.72 Mine D 251,504 97,989 1.34 Mine E 78,750 30,682 0.25 Mine F 3,000 1,169 0.01

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the relative contribution to greenhouse gas emissions from the major sources. Total specic emissions from the six mines varied from about 31 kg CO2 -e year1 t1 up to almost 110 kg CO2 -e y1 t1 . Fugitive emissions of methane from seam gas were the dominant source of greenhouse gases, ranging from slightly more than a third to almost three quarters of individual mines total greenhouse emissions. For some mines, emissions from spontaneous combustion are substantial and are of the same order as all of their energy-related emissions, in some cases representing up to about a third of all emissions. For one of the mines (mine D), spontaneous combustion is estimated to produce more than 250,000 t CO2 per year. Table 4 summarises the emissions from spontaneous combustion and also shows the amount of ROM coal that would need to be burnt to produce an equivalent amount of CO2 (assuming 70% carbon in the ROM coal). Table 4 shows that the annual emissions from spontaneous combustion can be equivalent to burning as much as 100,000 tonnes of coal. For mine D, this represents about 1.3% of its annual production. Given that spoil piles may contain millions of tonnes of carbonaceous waste, it is clear that a mine with uncontrolled spontaneous combustion is likely to release very large quantities of greenhouse gases over its lifetime and beyond. While the contribution of spontaneous combustion is clearly signicant for some individual mines, it is, however, unclear at present how important this source is for the industry as a whole, since many of the 60 or so open-cut coal mines currently operating in Queensland and NSW are not affected by spontaneous combustion. Low-temperature oxidation contributed only around 1% of the total greenhouse emissions for all six mines. Estimates were made by assuming that the average carbon content of the spoil was 5%, but this is likely to be highly variable both between individual mines and also within the spoil. However, even if the emissions from lowtemperature oxidation were a factor of two higher, they would still be relatively minor compared to spontaneous combustion and fugitives.

Conclusions Estimates of greenhouse gas emissions were made at six Australian open-cut coal mines. Fugitive emissions of methane from seam gas were in all cases estimated to be the largest source of greenhouse gas, but for some mines, up to a third of the total emissions originated from spontaneous combustion. In one mine, annual emissions attributed to spontaneous combustion amounted to about 250,000 t CO2 -e. There is, however, considerable uncertainty surrounding estimates from spontaneous combustion. The emission factors and the emission/ temperature relationship established by Carras et al. (2009) are subject to considerable inherent uncertainty, but compounding this are errors in measuring the area of spoil affected by spontaneous combustion. The area is generally estimated by ground surveys; however, these appear to substantially underestimate the true area because ground without visible signs of heating may not be included. Airborne infrared thermography is a more reliable method for measuring the area of spontaneous combustion, since it is capable of detecting even slightly elevated surface temperatures where other visual signs of heating are not apparent. Infrared data also provides a method for measuring the surface temperature, which can in turn be used to infer greenhouse emissions. Although emissions from spontaneous combustion represent a large proportion of the total in some mines, the contribution to greenhouse gas emissions from the coal mining industry as a whole is probably substantially less since spontaneous combustion is not present in all mines. Lowtemperature oxidation, on the other hand, is likely to be present at most mines but is a relatively minor source of greenhouse gas, contributing up to about 1% of a mines total emissions.

Acknowledgements We are grateful to the many mine personnel who provided the data for this project and their helpful discussions. This project was partially supported by the Australian Coal Association Research Program.

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541 combustion and greenhouse gas emissions. ACARP Project C9062 Final Report (41 pp.). Brisbane: Australian Coal Association. Carras, J. N., Day, S. J., Sagha, A., & Williams, D. J. (2009). Greenhouse gas emissions from low temperature oxidation and spontaneous combustion at opencut coal mines in Australia. International Journal of Coal Geology. doi:10.1016/j.coal.2008.12.001. Kuenzer, C., Zhang, J., Tetzlaff, A., van Dijk, P., Voight, S., Mehl, H., et al. (2007). Uncontrolled coal res and their environmental impacts: Investigating two arid mining regions in north-central China. Applied Geography (Sevenoaks, England), 27, 4262. doi:10.1016/j.apgeog.2006.09.007. Leung, L. (2002). Coal mine greenhouse gas emissions measurement accuracy. ACARP Project 11003 Final Report (32 pp.). Brisbane: Australian Coal Association. Sagha, A., Roberts, D., Fry, R., Quintanar, A., Day, S., Lange, T., et al. (2008). Evaluating a Tier 3 method for estimating fugitive emissions from open cut coal mining. ACARP Project 15076 Final Report (104 pp.). Australian Coal Association, Brisbane. Stracher, G. B., & Taylor, T. P. (2004). Coal res burning out of control around the world: thermodynamic recipe for environmental catastrophe. International Journal of Coal Geology, 59, 717. doi:10.1016/j. coal.2003.03.002. Williams, D. J., Carras, J. N., Mallett, C., Mark, M., Cooke, D., & Randall, C. (1998). Scoping study on the management and abatement of greenhouse gas emissions. ACARP Project C7050 Final Report (84 pp.). Brisbane: Australian Coal Association.

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