Nigel
Gibson
,
Robert
Stewart
and
Erika
Rankin
AEA Group, The Gemini Building, Fermi Avenue, Harwell, Oxfordshire OX11 0QR, United Kingdom. E-mail: nigel.gibson@aeat.co.uk; Fax: +44 (0)870 190 6318; Tel: +44 (0)870 190 6478
First published on 24th November 2011
A study has been carried out to assess the contribution of Polycyclic Aromatic Hydrocarbons (PAHs) from asphalt plant operation, utilising Benzo(a)pyrene (BaP) as a marker for PAHs, to the background air concentration around asphalt plants in the UK. The purpose behind this assessment was to determine whether the use of published BaP emission factors based on the US Environmental Protection Agency (EPA) methodology is appropriate in the context of the UK, especially as the EPA methodology does not give BaP emission factors for all activities. The study also aimed to improve the overall understanding of BaP emissions from asphalt plants in the UK, and determine whether site location and operation is likely to influence the contribution of PAHs to ambient air quality. In order to establish whether the use of US EPA emissions factors is appropriate, the study has compared the BaP emissions measured and calculated emissions rates from two UK sites with those estimated using US EPA emission factors. A dispersion modelling exercise was carried out to show the BaP contribution to ambient air around each site. This study showed that, as the US EPA methodology does not provide factors for all emission sources on asphalt plants, their use may give rise to over- or under-estimations, particularly where sources of BaP are temperature dependent. However, the contribution of both the estimated and measured BaP concentrations to environmental concentration were low, averaging about 0.05 ng m−3 at the boundary of the sites, which is well below the UK BaP assessment threshold of 0.25 ng m−3. Therefore, BaP concentrations, and hence PAH concentrations, from similar asphalt plant operations are unlikely to contribute negatively to ambient air quality.
Impact statementThis study was carried out to assess the contribution of Polycyclic Aromatic Hydrocarbons (PAHs) from UK asphalt plant and to gain a better understanding of Benzo(a)pyrene (BaP) emissions in this context. The assessment determines whether the use of published BaP emission factors from the US Environmental Protection Agency (EPA) methodology is appropriate in the UK context to estimate BAP/PAH contribution to background air concentration. It also determines whether site location and operation is likely to influence the contribution. The study has shown that use of the US EPA methodology may give rise to over- and/or under-estimations, particularly where sources are temperature dependent. However, it also shows that the contribution of both estimated and measured BaP concentrations to ambient air were low. |
The study also aimed to improve overall understanding of BaP emissions from asphalt plants in the UK and determine whether plant design or siting is likely to impact on the contribution of PAHs to ambient air quality.
The chemical and physical properties of different PAHs vary, as do their carcinogenicity. Human exposure to PAH occurs through a number of environmental pathways and includes internal absorption (through eating and drinking) and inhalation of air both indoors and outdoors. A number of PAH have been classified by the International Agency for Research on Cancer (IARC) as either carcinogenic to humans (Group 1), a probable carcinogen (Group 2A) or a possible carcinogen (Group 2B) human carcinogens, with benzo(a)pyrene (BaP) being the only PAH to fall into the Group 1 category. It is usual for the carcinogenic potencies of PAH to be published relative to BaP.
The EU Working Group on Polycyclic Aromatic Hydrocarbons has proposed using BaP as a marker for PAHs. For this reason, as well as because of the harmful effect on human health, BaP has been utilised as a marker for PAHs during this air quality assessment study.
A lower assessment threshold for BaP of 0.4 ng m−3 and an upper assessment threshold of 0.6 ng m−3 are also set by the Fourth Daughter Directive primarily as a measure to set appropriate future assessment methods required to monitor the concentration of PAH. Below the upper assessment threshold the Directive allows for assessment by a combination of measurement and modelling. Below the lower threshold the use of modelling or objective estimation can be used.
The UK Expert Panel on Air Quality (EPAQS) air quality standard for BaP is 0.251 ng m−3. This concentration has been adopted as a provisional national air quality strategy objective for England, Wales and Scotland, to be achieved by 31 December 2010.
The Air Quality Strategy for England, Scotland, Wales and Northern Ireland projects that there will be exceedances of the 2010 objective for PAH in some major urban areas and alongside busy roads.2
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Fig. 1 Schematic overview of the asphalt process. |
In an asphalt or batch plant, mineral aggregates are heated in a rotary drum dryer to a temperature between 135 °C and 180 °C. Heated and dried mineral aggregate is placed into a pug mill mixer, where it is coated with bitumen and mineral filler. Bitumen is pumped into a pug mill mixer in discrete portions from bitumen storage tanks. Drum plants differ from batch plants in that the heating and drying of the mineral aggregate as well as the addition of bitumen and filler take place in the rotary drum.
Emissions of BaP will arise from incomplete combustion of fuel in the drier as well as from bitumen delivery and storage, the coating process, asphalt storage, loading and from vehicles before sheeting.
The use of published emissions factors is a recognised method for estimating the emissions from plants that are still in the development phase. The information that underpins the emission factor development tends to be the culmination of a significant number of separate studies that may not necessarily have been carried out for establishing detailed emission factors, especially across the full range of hazardous air pollutants. This is particularly true for the EPA emissions factors, as published in their AP-42 emission factor handbook.5 This handbook provides an interpretation of asphalt plant emissions based on the US design and operation of asphalt plants and may not necessarily transpose directly to the UK situation. As discussed, the purpose of this study has been to assess the suitability of the AP-42 data for the purpose of determining the impact of BaP in the vicinity of two asphalt plants in the UK and, through this determination, to identify whether any improvements can be made to the understanding of the significance of BaP from the various stages of the asphalt process and how this may impact on the siting of asphalt plants in future.
Study site 1 | |
Annual plant through put |
ca. 108![]() |
Operating hours | 24 h per day, with peak collection period between 0600–1000 and 1200–1400 |
Recycled materials used | Foundry sand which is dried alongside roadstone |
Main stack | 26 m serving emissions from drier and pug mixer |
Maximum operating temperature | 186 °C |
Bitumen storage | Four grades used and blended on site |
Bitumen delivery | Daily delivery of approximately 27 tonnes, 5 days per week |
Study site 2 | |
Annual plant throughput |
ca. 240![]() |
Operating hours | Permitted hours between 0530–2200 (Monday–Friday); 0600–1400 (Saturday) |
Recycled materials used | Various percentages of Reclaimed Asphalt Product (RAP) added which is dried alongside roadstone |
Main stack | 30 m serving emissions from drier |
Operating temperature | 160 °C |
Bitumen storage | 4 × 100 tonne tanks |
Bitumen delivery | 1–2 daily deliveries of approximately 27 tonnes each, 5 days per week |
The BaP emissions measured on each of these two sites were compared with the estimated emissions calculated using US EPA emission factors. This established whether the use of US EPA emissions factors in the context of a typical UK roadstone coating plant is an appropriate method for estimating emissions.
Following on from this, a dispersion modelling exercise, using ADMS v3.3, was carried out around both sites to show the BaP contribution to ambient air. This allowed an improved understanding of how site design contributes to BaP concentrations in ambient air, and may impact on the design and siting of asphalt plants in future.
The resin traps were not supplied at a temperature below −5 °C or kept in the dark.
The sampling volumetric flow rate was in the order of 0.9 m3 h−1, which was below the recommended rate of 1 m3 h−1.
Due to safety issues a sample was collected from only one port on the stack.
Gas velocities and temperatures were measured across the two sampling axes to enable the determination of isokinetic flow rates. Exhaust gas flow rates were measured using pitot probes at the stack, sampled gas volumes were recorded using calibrated gas meters.
In order to determine emissions rates, a number of other factors, including gas flow rates, measurement/sampling periods and production rates, were also measured where possible.
BaP concentration (μg m−3) | Total PAH concentration (μg m−3)a | BaP as % of Total PAH | BaP Standard Deviation | |
---|---|---|---|---|
a PAH emissions measured on both sites included naphthalene, acenaphthylene, acenaphthene, fluorene, phenanthrene, anthracene, fluoranthene, pyrene, benzo(a)anthracene, chrysene, benzo(b/j)fluoranthene, benzo(k)fluoranthene, benzo(a)pyrene, indeno(123-cd)pyrene, dibenzo(ah)anthracene, benzo(ghi)perylene. | ||||
Stack Total | 0.001 | 61.9 | 0.002 | — |
Mixer 1–3 | 0.006 | 6.1 | 0.098 | |
Mixer 2–3 | 0.001 | 7.0 | 0.014 | |
Mixer 5–6 | 0.010 | 9.7 | 0.103 | |
Mixer Average | 0.006 | 7.6 | 0.075 | 0.0045 |
Unload 1 | 0.008 | 376.0 | 0.002 | |
Unload 2 | 0.007 | 327.5 | 0.002 | |
Bitumen Unload Average (Delivery) | 0.008 | 351.8 | 0.002 | 0.0007 |
Blow-out 1 | 0.245 | 413.0 | 0.059 | |
Blow-out 2 | 0.108 | 380.8 | 0.028 | |
Blow-out average | 0.177 | 396.9 | 0.044 | 0.0969 |
BaP concentration (μg/m3) | Total PAH concentration (μg m−3)a | BaP as % of Total PAH | BaP standard deviation | |
---|---|---|---|---|
a See footnote on Table 2. b The proportion of naphthalene determined in the bin samples was lower than for the other samples resulting in a comparatively high BaP as % of Total PAH. | ||||
Stack Vapour | 0.005 | 63.2 | 0.008 | |
Stack PM | 0.047 | 273.1 | 0.017 | |
Stack Total | 0.052 | 336.3 | 0.015 | — |
Bin 6/7 | 0.084 | 30.0 | 0.280b | |
Bin 4/5 | 0.026 | 9.0 | 0.289b | |
Bin Average | 0.055 | 19.5 | 0.282b | 0.0410 |
Bitumen Unload (Delivery) | 0.092 | 240.6 | 0.038 | — |
Blow-out | No data | No data | No data | — |
Vehicle test 1 | 1.2 | 596.5 | 0.201 | |
Vehicle test 2 | 0.5 | 710.6 | 0.070 | |
Vehicle test 3 | 0.3 | 662.8 | 0.045 | |
Vehicle test 4 | 0.2 | 781.1 | 0.026 | |
Vehicle test 5 | 0.4 | 952.4 | 0.042 | |
Vehicle average | 0.5 | 740.7 | 0.070 | 0.396 |
Following the completion of PAH monitoring for both sites, the measured BaP concentrations from each individual process on site were converted to emission factor estimates, in grams per tonne of asphalt (Table 5). The method used to carry out this conversion is discussed below. BaP contributions were also predicted using the US EPA AP-42 methodology, and results also displayed in grams per tonnes. This will allow a direct comparison between the two sets of results.
Unit Emission (g/tonne) = Total Emission (g)/total production during the sample period (tonnes) |
Total Emission (μg) = stack concentration (μg/m3) × gas flow rate (N m3/s) × sample period (seconds) |
Stack Concentration (μg m−3) = Stack vapour phase contribution (μg m−3) + PM phase contribution (μg m−3) |
Unit Emission (g/tonne) = Total Emission (g/yr)/production per year (tonnes/yr) |
Total Emission (g/yr) = USEPA organic PM emission estimate (kg/yr) × USEPA PAH % of total × % of BaP in average emission from bin/mixer |
Unit Emission (g/tonne) = Total Emission During Monitoring Period (g)/Production During Monitoring Period (tonnes) |
Total Emission During Monitoring Period (g) = Unload Emission (g) + Blow-out Emission (g) |
Unload/Blow-out Emission (μg) = Concentration (μg/m3) × Flow Rate (m3 s−1) × Unload Time (seconds) |
The figures used for the calculation and resulting emission estimates are show in Table 4.
Vehicle test 1 | Vehicle test 2 | Vehicle test 3 | Vehicle test 4 | Vehicle test 5 | |
---|---|---|---|---|---|
Measured BaP (μg m−3) | 1.2 | 0.5 | 0.3 | 0.2 | 0.4 |
Volume sampled (m3) | 1.617 | 1.617 | 1.557 | 1.111 | 0.515 |
Estimated tonnes per load | 19.5 | 19.5 | 19.5 | 19.5 | 19.5 |
Number of loads per test | 3 | 3 | 3 | 2 | 1 |
Total tonnes per test | 58.5 | 58.5 | 58.5 | 39 | 19.5 |
BaP emissions for measurement period (μg/tonne) | 0.03317 | 0.01382 | 0.00798 | 0.00570 | 0.01056 |
Total sample time per test (min) | 80 | 80 | 75 | 40 | 35 |
Unsheeted time per test (min) | 24 | 24 | 24 | 16 | 8 |
% time unsheeted | 30.0% | 30.0% | 32.0% | 40.0% | 22.9% |
BaP emissions for unsheeted period (μg/tonne) | 0.00995 | 0.00415 | 0.00256 | 0.00228 | 0.00241 |
Average (μg/tonne) | 4.27 × 10−3 | ||||
Emission rate (g/tonne) | 4.27 × 10−9 |
Unit Emission (g/tonne) = Average[Unit Emission (g/tonne) of vehicle loads] |
Unit Emission (g/tonne) of vehicle loads = Total Emission During Exposed Period (g)/Total Vehicle Load per Test (tonnes) |
Total Emission During Exposed Period (g) = BaP emission for measurement period (g/tonne) × % load unsheeted time |
BaP emission for measurement period (g/tonne) = measured BaP (g m−3) × volume sampled (m3)/load weight (tonnes) |
Emission calculation | Site 1 | Site 2 |
---|---|---|
a The yard contributions for site 1 were incomplete. b At site 2, the level of detail around the bitumen unloading activity was lower, as the blow off activity, where bitumen is cleared from the transfer pipe, was carried out too quickly for any samples to be collected. c See Table 4. | ||
Main stack | ||
Total Stack Contribution (μg m−3) | 0.001 | 0.052 |
Gas Flow Rate (N m3 s−1) | 8.2 | 3.39 |
Sample period (seconds) | 14![]() |
14![]() |
Total Emission (g) | 1.18 × 10−04 | 0.0025 |
Sample Period Production (tonnes) | 179 | 152 |
Emission (g/tonne) | 6.6 × 10−07 | 1.67 × 10−05 |
Silo emission | ||
USEPA organic PM emission estimate (kg/yr) | 39.15 | 22.06 |
USEPA PAH % of Organic PM | 11.40 | 11.40 |
% of BaP in average emission from bin/mixer | 0.075 | 0.28 |
Total Annual Emission (kg/yr) | 0.0033 | 0.0071 |
Production (tonnes/yr) | 108![]() |
240![]() |
Emission (g/tonne) | 3.08 × 10−05 | 2.96 × 10−05 |
Load out | ||
USEPA organic PM emission estimate (kg/yr) | 52.57 | 29.62 |
USEPA PAH % of Organic PM | 5.93 | 5.93 |
% of BaP in average emission from bin/mixer | 0.075 | 0.28 |
Total Annual Emission (kg/yr) | 0.0023 | 0.0050 |
Production (tonnes/yr) | 108![]() |
240![]() |
Emission (g/tonne) | 2.15 × 10−05 | 2.06 × 10−05 |
Bitumen Delivery | ||
Unloading Concentration (μg m−3) | 0.0075 | 0.0920 |
Unloading Flow Rate (m3 s−1) | 0.0157 | 0.0118 |
Unload Time (seconds) | 2,400 | 3120 |
Total Unloading Emission (μg) | 0.2827 | 3.3816 |
Blow-out Concentration (μg m−3) | 0.1765 | Not determined/measuredb |
Blow-out Flow Rate (m3 s−1) | 0.0471 | |
Blow-out Time (seconds) | 120 | |
Total Blow-out Emission (μg) | 0.9981 | |
Total Emission During Monitoring Period (g) | 1.28 × 10−06 | |
Production During Monitoring Period | 415 | 758 |
Emission (g/tonne) | 3.09 × 10−09 | >4.46 × 10−09 |
Yard Emissions | ||
Emission (g/tonne)c | Not determineda (assumed to be 1.27 × 10−05 g/t using the USEPA methodology) | 4.27 × 10−09 |
Total Emission Factor (g/tonne) | 6.57 × 10 −05 | >6.69 × 10 −05 |
Emission Rate Calculation | Site 1 | Site 2 |
---|---|---|
a V is the asphalt volatility as determined by ASTM Method D2872-88, set at default value of −0.5. b T is operating temperature in °F. c EF is the organic particulate matter emission factor (g or kg per tonne asphalt). d AF is the proportion of the organic particulate matter fraction that is BaP (in %). | ||
T/°C | 186 | 160 |
Temperature (°F) | 366.8 | 320 |
Main Stack | ||
ERBaP (g/t) | 1.55 × 10−07 | 1.55 × 10−07 |
Silo Emission | ||
EFPM = 0.00105(−V)e((0.0251)(T + 460)−20.43) (kg/t) | 0.00036 | 0.00011 |
AFBaP (%) | No data | No data |
EFBaP (g/t) = EFPM × AFBaP | No value | No value |
Load Out | ||
EFPM = 0.0141(−V)e((0.0251)(T + 460)−20.43) (kg/t) | 0.00049 | 0.00015 |
AFBaP (%) | 0.0023% | 0.0023% |
EFBaP (g/t) = EFPM × AFBaP | 1.12 × 10−05 | 3.46 × 10−06 |
Bitumen Storage /Delivery | ||
EFPM determined using US EPA ‘TANKS’ programme (kg/t) | Not possible for bitumen PM | Not possible for bitumen PM |
AFBaP (%) | No data | No data |
EFBaP (g/t) = EFPM × AFBaP | No value | No value |
Yard Emissions | ||
EFPM (kg/t) | 0.00055 | 0.00055 |
AFBaP (%) | 0.0023% | 0.0023% |
EFBaP (g/t) = EFPM × AFBaP | 1.27 × 10−05 | 1.27 × 10−05 |
Total Emission Factor (g/tonne) | >2.40 × 10 −05 | >1.63 × 10 −05 |
Parameter - stack parameters | Site 1 | Site 2 |
Assumed operation hours | 24 per day | 24 per day |
Efflux velocity | 14.9 m s−1 | 11.9 m s−1 |
Exit temperature | 111 °C | 103 °C |
Exit diameter | 1.02 m | 1.18 m |
Stack height | 26 m | 30 m |
Flow rate (actual) (m3 h−1) | 43,920 | 47,700 |
Parameters - Other sources | Site 1 | Site 2 |
Discharge Heights | ||
Load out | 1 m | 1 m |
Silo filling | 5 m | 5 m |
Yard emissions | 1 m | 1 m |
Bitumen tanks | 0.5 m | 0.5 m |
Discharge velocity | ||
Load out | ||
Silo filling | 0 m s−1 | 0 m s−1 |
Yard emissions | ||
Bitumen tanks |
Fig. 2 and 3 show the BaP contribution superimposed on the site plans. In each case the emission rates applied were those calculated from the measured BaP concentrations, as shown in Table 2. In each case the dispersion modelling shows that the contribution of BaP to the ambient concentration is focused around the main processing building, where both the silos and load out activity are located. In addition to this, in Fig. 2 (site 1), a small area where the where the BaP contribution may exceeds 0.25 ng m−3, i.e. within the 0.1 ng m−3 contour, lies very close to the eastern side of the plant boundary. This feature coincides with the yard activities, which were assigned the predicted US EPA emission factor, which was much higher than the emission factor determined at site 2. It is important to note that the findings of this dispersion modelling exercise are site specific. Other building/discharge configurations may result in significantly different impact profiles.
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Fig. 2 Annual mean BaP concentration (ng m−3) around site 1. Contours shown are 0.25, 0.05 and 0.01 ng m−3. |
![]() | ||
Fig. 3 Annual mean BaP concentration (ng m−3) around site 2. Contours shown are 0.25, 0.05 and 0.01 ng m−3. |
However, notwithstanding the omissions in the US EPA methodology, this study has shown that the estimated BaP emissions measured on the two sites (6.57 × 10−05 g/t and 6.69 × 10−05 g/t) is broadly similar to that determined using the US EPA method: >2.40 × 10−05 g/t and >1.63 × 10−05 g/t for sites 1 and 2, respectively.
The annual average BaP concentration in large urban centres such as London and Glasgow in 2005 was found to be 0.08 ng m−3 and 0.10 ng m−3 respectively6 and in industrial areas, that contain major BaP emission sources, the BaP concentrations are likely to be higher. Based on the findings of this study, it is highly unlikely that the BaP assessment threshold of 0.25 ng m−3 will be exceeded when siting asphalt plants. In locations where there is already an existing and significant source of BaP the implications of additional activities that might generate further emissions should be considered.
•Careful control of the process temperatures to minimise the generation of organic particulate matter.
•Containment of fugitive emissions, especially close to the site boundary.
•Ensuring that any new plant is not sited in close proximity to potentially sensitive receptors who may be affected over the exposure period of a year.
•Ensuring that BaP producing activities, where located near to site boundary, are located on sides away from potentially sensitive receptors.
Footnotes |
† 1 ng m−3 is equal to 1 × 10−9 g m−3. |
‡ The consequence of operating temperature on organic particulate matter can be seen from the US EPA equations reproduced in Table 6 and the estimates for organic PM emission in Table 5. It can be seen that the generation of organic particulate matter is a temperature dependent function. For example, comparing the BaP contributions at 160 °C and 180 °C against 140 °C will result in a 3 and 9 fold increase in BaP emission. It is therefore critical for this type of operation to maintain the drier temperature as low as practicable whilst maintaining the required asphalt temperature at the point of use. Clearly, the same effects will be found for the silo and probably the yard emissions. |
This journal is © The Royal Society of Chemistry 2012 |