Abstract
Energy supply utilities release significant amounts of greenhouse gases (GHGs) into the atmosphere. It is essential to accurately estimate GHG emissions with their uncertainties, for reducing GHG emissions and mitigating climate change. GHG emissions can be calculated by an activity-based method (i.e., fuel consumption) and continuous emission measurement (CEM). In this study, GHG emissions such as CO2, CH4, and N2O are estimated for a heat generation utility, which uses bituminous coal as fuel, by applying both the activity-based method and CEM. CO2 emissions by the activity-based method are 12–19% less than that by the CEM, while N2O and CH4 emissions by the activity-based method are two orders of magnitude and 60% less than those by the CEM, respectively. Comparing GHG emissions (as CO2 equivalent) from both methods, total GHG emissions by the activity-based methods are 12–27% lower than that by the CEM, as CO2 and N2O emissions are lower than those by the CEM. Results from uncertainty estimation show that uncertainties in the GHG emissions by the activity-based methods range from 3.4% to about 20%, from 67% to 900%, and from about 70% to about 200% for CO2, N2O, and CH4, respectively, while uncertainties in the GHG emissions by the CEM range from 4% to 4.5%. For the activity-based methods, an uncertainty in the Intergovernmental Panel on Climate Change (IPCC) default net calorific value (NCV) is the major uncertainty contributor to CO2 emissions, while an uncertainty in the IPCC default emission factor is the major uncertainty contributor to CH4 and N2O emissions. For the CEM, an uncertainty in volumetric flow measurement, especially for the distribution of the volumetric flow rate in a stack, is the major uncertainty contributor to all GHG emissions, while uncertainties in concentration measurements contribute a little to uncertainties in the GHG emissions.
Implications:
Energy supply utilities contribute a significant portion of the global greenhouse gas (GHG) emissions. It is important to accurately estimate GHG emissions with their uncertainties for reducing GHG emissions and mitigating climate change. GHG emissions can be estimated by an activity-based method and by continuous emission measurement (CEM), yet little study has been done to calculate GHG emissions with uncertainty analysis. This study estimates GHG emissions and their uncertainties, and also identifies major uncertainty contributors for each method.
Introduction
Human activities, such as fossil fuel combustion and land usage changes, increase greenhouse gas (GHG) concentrations in the atmosphere. The increased GHG concentrations result in increasing average global temperature by absorbing the surface radiation (Le Treut et al., Citation2007). In 1997, under the United Nations Framework Convention on Climate Change (UNFCCC), the Kyoto Protocol was established to set legally binding obligations for developed countries (Annex I countries) to reduce GHG emissions to 5% below the 1990 levels (Barker et al., Citation2007). In 2010, the Cancun Agreement, mainly based on the Copenhagen Accord, was reached to limit the increase in average global temperature not more than 2°C relative to the preindustrial temperature by reducing GHG emissions significantly (UNFCCC, Citation2011). Under the UNFCCC, the Annex I countries should submit annual national inventory reports for GHG emissions. The inventories are useful not only for policymakers to develop effective strategies to reduce GHG emissions, but also for scientists to understand the sources and trends in GHG emissions. To support the UNFCCC, the Intergovernmental Panel on Climate Change (IPCC) has developed methodologies and guidelines for preparing national inventories of GHG emissions (IPCC, Citation1997, 2006). The 2006 guidelines consists of five volumes that describe the general guidance for developing emission inventories and the more specific guidance for estimating GHG emissions in different sectors such as energy, industrial processes and product use, agriculture/forestry/other land use, and waste from economic activities. The energy supply (e.g., stationary combustion) in the energy sector is an important source of GHG emissions as it contributes 25.9% of the global GHG emissions (Barker et al., Citation2007). Therefore, it is essential to properly estimate GHG emissions from the energy supply for mitigating climate change.
GHG emissions can be estimated by an activity-based (fuel consumption-based) method and by continuous emission measurement (CEM). The activity-based method estimates GHG emissions by using fuel consumption and emission factors, while the CEM directly measures GHG emissions through monitoring GHG concentrations and volumetric flow rate at a stack. In addition to the emission estimates, proper uncertainty estimation for the GHG emissions is also important for policymakers to make decisions for mitigating GHG emissions and for scientists to understand climate change. The IPCC has developed good practical guidelines for estimating and reporting uncertainties in the GHG emissions (IPCC, Citation2000, 2006). There are previous studies that estimate CO2 emissions and their uncertainties for directly comparing those from both methods for coal-fired energy utilities (Ackerman and Sundquist, Citation2008; Evans et al., Citation2009; Quick, Citation2014).
In this study, GHG emissions (CO2, CH4, N2O) from an energy supply utility fueled by coal were estimated by both activity-based and CEM methods. In addition, associated uncertainties in the GHG emissions were calculated by propagating the uncertainties of input variables for both methods. Based on results, important uncertainty sources were suggested to reduce uncertainties in the GHG emissions from energy supply utilities for improving the quality of GHG emission inventories.
Experiments and Methods
Fuel consumption estimation
A heat production plant that used bituminous coal as fuel was selected for this study. Monthly fuel consumption for August 2011 was estimated by using fuel mass that was carried into a plant storage tank and fuel mass that was left in the storage tank. The monthly fuel consumption was calculated as
Flow measurement
A flow velocity inside a stack was measured by a flow rate measurement system (FTV-05, Tech Korea Inc., Korea), every 3 sec from August 1 to August 31, 2011. A volumetric flow rate was estimated as
The flow rate measurement system was connected to the national tele-metering system (TMS) for monitoring stack emissions, reporting 5-minute accumulated volumetric flow to the national TMS. The 5-minute accumulated volumetric flow was estimated as
Gas concentration measurement
CO2, N2O, and CH4 were continuously measured by ULTRAMAT6 gas analyzers (Siemens, Munich, Germany) every 10 sec from August 1 to August 31, 2011. A sampling probe was installed at 0.5 m away from the center of an emission stack, and a sampling line was heated to prevent from condensing water vapor. Sampled emission gas was cooled at 4°C to remove water vapor prior to the gas analyzer. Prior to the continuous measurement, the distribution of CO2 concentrations inside the stack (2.5 m as diameter) was determined by measuring the concentrations at seven points across the stack (one point at the center, two points at 0.5 m away from the center, two points at 0.9 m away from the center, two points 1.1 m away from the center). The maximum deviation from the mean concentrations was 0.3%. The results indicated that the CO2 concentrations were not stratified across the stack, since the maximum deviation was less than 5% (U.S. Environmental Protection Agency [EPA], 1997). The sampling probe was installed at 0.5 m away from the center of the stack where the deviation from the mean CO2 concentrations was 0.09%. The gas analyzer was calibrated against the primary standard gas mixtures (PSMs), which are traceable to Korea Research Institute of Standards and Science (KRISS), before and during the measurement. The 5-min averaged concentrations were calculated and then used to estimate GHG emissions for the CEM.
Emission estimation based on activity data
GHG emissions during the study period (from August 1 to August 31, 2011) were estimated based on activity data (e.g., fuel consumption, net calorific value), emission factor, and carbon content of fuel according to the 2006 IPCC guidelines (IPCC, 2006). Emission estimates, by using emission factor (EF) and net calorific value (NCV), can be expressed as
By using carbon content (CC) and NCV, emission estimates can be expressed as
GHG emissions were estimated for four different cases: IPCC default EF (Tier 1) and NCV were used in case 1, IPCC default EF (Tier 1) and plant-specific NCV were used in case 2, plant-specific CC and NCV were used in case 3, and plant-specific CC for CO2, technology-specific IPCC default EF for N2O and CH4, and plant specific NCV were used in case 4. For case 4, the technology-specific EFs (default Tier 3 EFs) for N2O and CH4 were used since they may be more realistic values compared to the default Tier 1 EF based on only fuel.
Emission estimation based on continuous emission measurement (CEM)
Unlike the activity-based method, the concentrations and flow rate of gas emissions at a stack were measured continuously by CEM during the study period. GHG emissions were estimated as
Uncertainty Estimation
Uncertainty components of GHG emission estimation for each method were identified, calculated, and then combined according to the Guide to the Expression of Uncertainty in Measurement (BIPM et al., Citation1995). In a companion article, more statistical methods (e.g., bootstrap, Monte Carlo method, etc.) were discussed for combining uncertainties with different probability distributions. Therefore, the statistical methods were not discussed in this study.
Uncertainty for fuel consumption
The model equation for the fuel consumption estimation can be expressed as
Uncertainty for flow measurement
The model equation for the continuous flow measurement can be expressed as
Uncertainty for gas concentration measurement
The model equation for the continuous measurement of gaseous air pollutants can be expressed as
The estimate of xs was a certified concentration (e.g., concentration reported in certificates of PSMs) for the span gas. The standard uncertainty, u(xs), of the span gas was determined by dividing the reported expanded uncertainty of the span gas by a coverage factor, k:
For repeatability, a series of responses of the measuring instrument was observed by applying the span gas into the instrument. The arithmetic mean and experimental standard deviation was calculated for the n observations. The arithmetic mean was taken as the input estimate of Rs. The experimental standard deviation divided by a square root of the number (n = 20) of the observations, which was the experimental standard deviation of the mean of the observations, was the standard uncertainty for Rs:
The response (R) to an arbitrary concentration (x) varies as the measurand concentration changes. The standard uncertainty for R was assumed the same as the standard uncertainty of Rs:
The fractional calibration drift (fcal drift) and zero offset (Δx0) were determined through applying span and zero gas into the instrument, respectively. The standard uncertainty for the fractional calibration drift was equal to the experimental standard deviation of multiple estimates of the fraction calibration drift when the span gas was applied into the instrument:
The standard uncertainty of the zero offset correction was estimated as the experimental standard deviation of multiple observations of the zero offset when the zero gas was applied into the instrument:
The fractional linearity (flinearity) of the measuring instrument was determined by applying linearity gas (e.g., about a half concentration of the span gas) into the instrument. The standard uncertainty of the fractional linearity was estimated as the experimental standard deviation of multiple estimates of the fractional linearity:
The combined standard uncertainty was estimated by combining the standard uncertainties of all uncertainty components in the measurement. The combined standard uncertainty can be estimated as
The uncertainty budget for each gas measurement was summarized in and Figure S1 (Supplemental Materials). The standard uncertainty for each gas can be expressed as
The uncertainty equations indicate that the uncertainties in GHG concentration measurements vary as the measured GHG concentrations change. The contribution of each uncertainty component also changes as the measured GHG concentrations changes, shown in . The uncertainty contributions of the zero offsets are expressed as absolute values, while those of other uncertainty components are expressed as values relative to the measured GHG concentrations. As shown in Figure S1, the uncertainties in the zero offset corrections become the major uncertainty contributors for a lower measurement range of the gas analyzers (for less than 30% of a full range), whereas the uncertainties in the calibration drift and linearity become the major uncertainty contributors for a higher measurement range (for higher than 30% of a full measurement range). The relative uncertainties in GHG concentrations become larger, especially for the lower measurement range as the measured concentrations decrease. Therefore, for reducing the measurement uncertainty, it is a good practice to set the measurement range of gas analyzers properly so that measured GHG concentrations are not less than 30% of a full measurement range. As shown in Figure S1, typical concentration measurement uncertainties are from about 1% to 1.5%, while previous studies have reported less than 1% (Evans et al., Citation2009; Boze, Citation2010) and 7–12% (Quick, Citation2014).
Uncertainty for incomplete time coverage
Incomplete coverage of time period results in an additional uncertainty to the time average when there is a missing data for the time period in which the time average of a measurand (X) is calculated (ISO, Citation2002). The uncertainty due to the incomplete time coverage (or missing data) can be determined as
Uncertainty for emission estimates
The standard uncertainties of emission estimates based on the activity-based method were calculated as
The standard uncertainty of CO2 emission estimates based on fuel carbon content was calculated as
The standard uncertainties of emission estimates (for 5 min) based on CEM were calculated as
The standard uncertainties of emission estimates (for a month) based on the CEM were calculated as
Results and Discussion
Uncertainties of input parameters for GHG emission estimates are summarized in . The emission estimates with their uncertainties for all cases are summarized in . For case 1, all values with their uncertainties are default ones from the 2006 IPCC guidelines (IPCC, 2006) except the fuel mass consumed. The major uncertainty contributor for CO2 emission is the default NCV. For case 2, the same IPCC default EFs used in the case 1 are used for emission estimation while a plant-specific NCV, which is used to convert mass-based fuel consumption to energy-based fuel consumption, is determined from fuel analysis. The plant-specific NCV, 23.7 TJ/Gg, is within the uncertainty range of the IPCC default NCV (19.9–30.5 TJ/Gg). However, its uncertainty (±2.0%) is much lower than that of the IPCC default NCV, which results in a considerably reduced uncertainty (±6.0%) for the CO2 emission estimate compared to case 1. The major uncertainty contributor for the CO2 emission estimate is the IPCC default EF (±5.4%) due to the significantly reduced uncertainty in the plant specific NCV. For case 3 and case 4, CO2 emission is determined using a plant-specific CC (0.62 kg/kg) determined from fuel analysis. For a comparison, the mass-based CC (0.62 kg/kg) can be converted to an energy-based CC (26.3 kg/GJ) by using the plant-specific NCV. The energy-based plant specific CC agrees with the IPCC default CC (24.4–27.2 kg/GJ), and its uncertainty (±3.9%) is lower than that of the IPCC default (±5.4%). However, the uncertainty of the energy-based CC is larger than that of the mass-based CC (±2.9%), which is used to calculate CO2 emissions in this study, as the uncertainty in the plant specific NCV is combined with that of the mass-based CC for the energy-based CC. The smaller uncertainties of the plant specific NCV (case 2) and mass-based CC (case 3 and 4) results in significantly reduced uncertainties (±6.0% and ±3.4%, respectively) in CO2 emission estimates compared to the case 1 (larger than ±19%). For N2O and CH4 emissions, uncertainties in the EFs (larger than ± 67% and up to 900%) are the largest uncertainty contributors for all cases, as the uncertainties are much larger than those of fuel mass and NCVs. For the CEM, the volumetric flow with its uncertainty of ±3.9% is the major uncertainty contributor for all GHG emission estimates with uncertainties of ±4.0–4.5%.
To compare total GHG emission estimates for all cases, the estimated N2O and CH4 emissions are converted to CO2 equivalent emissions by multiplying with a gas-specific global warming potential (100-year time horizon), 298 and 25, respectively. The emission estimates by the CEM are larger than those by the activity-based method for all cases except N2O emission for the case 4 (). CO2 emission estimates by the activity-based method are 12–19% less than those by the CEM. The differences in the emission estimates by two different methods are similar with those reported in previous studies (Ackerman and Sundquist, Citation2008; Evans et al, Citation2009). N2O emission estimates by the activity-based method (cases 1–3) are two orders of magnitude less than that by the CEM. However, the N2O emission from case 4 (based on default technology-specific EF, Tier 3 default EF) is 40% higher than that by the CEM, though the estimate agrees with that by the CEM within the associated uncertainty. The Tier 3 default EF, which is a factor of about 41 higher EF than the Tier 1 default EF, results in the higher emission, but the associated uncertainty is the largest among all emission estimates (from –90% to +900%), indicating that more plant-specific EFs should be developed to reduce the uncertainty. Total GHG emissions based on the activity-based method are about 12–27% lower than that by the CEM, which is mainly due to the lower CO2 and N2O emissions by the activity-based method. The total GHG emissions by the activity-based method agree with each other within their associated uncertainty ranges, while that by the CEM agrees with only those from case 1 and case 4.
Summary
In this study, GHG emissions have been estimated for a heat generation utility, which uses bituminous coal as fuel, by applying both the activity-based and CEM method. In addition, associated uncertainties in the GHG emissions have been calculated by propagating the uncertainties of input variables for both methods. Based on results, important uncertainty sources have been identified to reduce uncertainties in the GHG emissions from energy supply utilities for improving the quality of GHG emission inventories. Results show that CO2 emissions by the activity-based method are 12–19% less than that by the CEM, while N2O and CH4 emissions by the activity-based method are two orders of magnitude and 60% less than those by the CEM, respectively. Comparing GHG emissions (as CO2 equivalent) from both methods, total GHG emissions by the activity-based methods are 12–27% lower than that by the CEM, as CO2 and N2O emissions are lower than those by the CEM. Results from the uncertainty estimation show that the major uncertainty contributors to the emission estimates are net calorific values (NCVs) and emission factors (EFs) for the activity-based method when the IPCC default values are used for the estimation. For the CEM, the major uncertainty contributor to the emission estimates is the volumetric flow, especially the distribution of flow rate in a stack. Although the uncertainties in GHG concentration measurements are minor uncertainty contributors for the GHG emission estimates in this study, it is important to properly calibrate gas analyzers and set an appropriate measurement range for the analyzers. To get more certain GHG emission estimates, it is a good practice to identify uncertainty contributors and quantify their uncertainties, whichever method is chosen for GHG emission estimation. Based on results from the uncertainty estimation, one can prioritize necessary work to improve the quality of input parameters in order to meet target (or required) uncertainties for GHG emission estimation.
Supplemental Material
Supplemental data for this article can be accessed at http://dx.doi.org/10.1080/10962247.2014.930078.
Funding
This work was supported by grants from the Korea Research Institute of Standards and Science (KRISS) under the Basic R&D Project of Establishment of National Gas Analysis Measurement Standards and Improvements of Calibration and Measurement Capabilities (Grant 13011020), and by grants from the Korea Research Council of Fundamental Science and Technology (KRCF) under the National Agenda Project of Development of Measurement Technology for Solving Climate Change (NAP-08-2).
Supplemental_Material.doc
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Notes on contributors
Sangil Lee
Sangil Lee and Jinchun Woo are principal scientists, and Jinsang Jung is a senior scientist with the Center for Gas Analysis in Korea Research Institute of Standards and Science.
Yongmoon Choi
Yongmoon Choi is a principal scientist and Woong Kang is a senior scientist with the Center for Fluid Flow and Acoustics in Korea Research Institute of Standards and Science, Daejeon, Republic of Korea.
Jinchun Woo
Sangil Lee and Jinchun Woo are principal scientists, and Jinsang Jung is a senior scientist with the Center for Gas Analysis in Korea Research Institute of Standards and Science.
Woong Kang
Yongmoon Choi is a principal scientist and Woong Kang is a senior scientist with the Center for Fluid Flow and Acoustics in Korea Research Institute of Standards and Science, Daejeon, Republic of Korea.
Jinsang Jung
Sangil Lee and Jinchun Woo are principal scientists, and Jinsang Jung is a senior scientist with the Center for Gas Analysis in Korea Research Institute of Standards and Science.
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