Direct measurement of fugitive emissions of hydrocarbons from a refinery

Refineries are a source of emissions of volatile hydrocarbons that contribute to the formation of smog and ozone. Fugitive emissions of hydrocarbons are difficult to measure and quantify. Currently these emissions are estimated based on standard emission factors for the type and use of equipment installed. Differential absorption light detection and ranging (DIAL) can remotely measure concentration profiles of hydrocarbons in the atmosphere up to several hundred meters from the instrument. When combined with wind speed and direction, downwind vertical DIAL scans can be used to calculate mass fluxes of the measured gas leaving the site. Using a mobile DIAL unit, a survey was completed at a Canadian refinery to quantify fugitive emissions of methane, C2+ hydrocarbons, and benzene and to apportion the hydrocarbon emissions to the various areas of the refinery. Refinery fugitive emissions as measured with DIAL during this demonstration study were 1240 kg/hr of C2+ hydrocarbons, 300 kg/hr of methane, and 5 kg/hr of benzene. Storage tanks accounted for over 50% of the total emissions of C2+ hydrocarbons and benzene. The coker area and cooling towers were also significant sources. The C2+ hydrocarbons emissions measured during the demonstration amounted to 0.17% of the mass of the refinery hydrocarbon throughput for that period. If the same loss were repeated throughout the year, the lost product would represent a value of US$3.1 million/yr (assuming US$40/bbl). The DIAL-measured hourly emissions of C2+ hydrocarbons were 15 times higher than the emission factor estimates and gave a different perspective on which areas of the refinery were the main source of emissions. Methods, such as DIAL, that can directly measure fugitive emissions would improve the effectiveness of efforts to reduce emissions, quantify the reduction in emissions, and improve the accuracy of emissions data that are reported to regulators and the public.     

远距离多通道的无组织排放VOCs连续在线监测系统

研制了一套远距离多通道VOCs连续采样在线监测系统.监测系统主要由远距离多通道VOCs连续采样装置与真空紫外灯单光子电离源飞行时间质谱仪组成.通过PAMS与有机硫标准气体对该系统进行了性能表征测试.结果表明:各物质连续7次实验RSD≤7％;最优检测限为0.004 μmol?mol-1;在0.01～1.00 μmol?m...     

Characterization of the fugitive particulate emissions from construction mud/dirt carryout

Although the fugitive dust associated with construction mud/dirt carryout can represent a substantial portion of the particulate matter (PM) emissions inventory in nonattainment areas, it has not been well characterized by direct sampling methods. In this paper, a research program is described that directly determined both PM10 and PM2.5 (particles < or =10 and 2.5 microm in classical aerodynamic diameter, respectively) emission factors for mud/dirt carryout from a major construction project located in metropolitan Kansas City, MO. The program also assessed the contribution of automotive emissions to the total PM2.5 burden and determined the baseline emissions from the test road. As part of the study, both time-integrated and continuous exposure-profiling methods were used to assess the PM emissions, including particle size and elemental composition. This research resulted in overall PM10 and PM2.5 emission factors of 6 and 0.2 g/vehicle, respectively. Although PM10 is within the range of prior U.S. Environmental Protection Agency (EPA) guidance, the PM2.5 emission factor is far lower than previous estimates published by EPA. In addition, based on both the particle size and chemical data obtained in the study, a major portion of the PM2.5 emissions appears to be attributable to automotive exhaust from light-duty, gasoline-powered vehicles and not to the fugitive dust associated with reentrained mud/dirt carryout.     

Wind tunnel simulation of environmental controls on fugitive dust emissions from mine tailings

The development of techniques for determining fugitive dust emissions presents numerous challenges and remains the subject of much investigation. Past approaches have included field based monitoring stations and wind tunnel studies, while more recently, highly portable field units (e.g., PI-SWERL) have been added to our toolkit of instruments and methodologies. In the case of the investigation reported herein, a laboratory wind tunnel study was designed to systematically simulate PM₁₀ emissions from mine tailings for a range of surface treatments. Unique challenges were associated with the project in the sense that the proposed mine and tailings did not exist at the time of the investigation, so that it was impossible to work on-site. Only a small amount of slurry from a milled drill core was available to work with, and there were no established test protocols and few experimental precedents to work from. The slurry formed highly cohesive bricks when dried, similar to crusted playas investigated in field experiments. The PM₁₀ emissions demonstrated strong temporal variation with particle supply limitation. A small amount of vertical dust dispersion was observed, with PM₁₀ concentrations decaying exponentially away from the source. The emission rates obtained are similar in magnitude to those obtained in field analogues. The highly controlled experiment allowed for separation and analysis of several physical controls on PM₁₀ emissions from tailings; namely, the study addressed the degree of disturbance, shrinkage and cracking, and the effects of spigotting, particle settling and re-wetting.     

Comparison of modeling with empirical calculation of diffuse and fugitive methane emissions in a Spanish landfill

One of the most significant environmental problems arising from landfills is the emission of methane into the atmosphere. In this study, methane emissions from a currently in-use Spanish landfill were modeled as well as being experimentally measured using a two-step method. The first step involved a qualitative walkover survey to detect where gases were being emitted on the surface of the landfill. The second stage comprised a quantitative analysis of these surface methane emissions at a selected number of points on the landfill surface using a specially designed flux chamber. The statistical analysis of the data obtained was based on the Sichel function and resulted in an average emission rate of 74.9 g·m^?2·day^?1, with 27.8 and 202.1 g·m^?2·day^?1 as the lower and upper limits of the 95% confidence interval, respectively. The total emission for the landfill, with an emitting surface of 335,000 m², is 9.16 × 10³ ton/yr. These values have been compared with those from three different models, with the model results being above the calculated mean emissions measured at the landfill, but below the upper confidence limit at 95%.

Implications: One of the main environmental problems arising from the presence of landfills is the emission of biogas (which mainly contains methane and carbon dioxide) into the atmosphere. Several experimental methods as well as models have been developed to quantify these emissions. In this work, the authors have compared the results obtained using experimental measurements with those provided by some local and international models using the default parameters proposed. The results obtained from the experimental method are in accordance with those provided by the models, although the models could be slightly overestimating these emissions.     

Localizing gaseous fugitive emission sources by combining real-time optical remote sensing and wind data

This paper presents a new approach to localize point emissions from ground-level fugitive gaseous air pollution sources. We estimate the crosswind plume's ground-level peak location downwind from the source by combining smooth basis functions minimization (SBFM) with pathintegrated optical remote sensing concentration data acquired along the crosswind direction in alternating beam path lengths. Peak location estimates, in conjunction with real-time measured wind direction data, are used to reconstruct the fugitive source location. We conducted a synthetic data study to evaluate the proposed peak location SBFM reconstruction. Furthermore, the methodology was validated with open-path Fourier transform infrared concentration data collected with wind direction data downwind from a controlled point source. This approach was found to provide reasonable estimates of point source location. The field study reconstructed source location was within several meters of the real source location.     

Derivation of new emission factors for quantification of mass emissions when using optical gas imaging for detecting leaks

This paper describes the development of new "leak/no-leak" emission factors that are suitable for estimating facilities' fugitive emissions when using an alternative work practice (AWP) that is based on optical gas imaging technology for detecting leaking piping system components. These emission factors were derived for valves, pumps, and connectors/flanges for instrument leak detection thresholds ranging from 3 to 60 g/hr using a combination of field data and Monte Carlo statistical simulation techniques. These newly derived leak/no-leak emission factors are designed to replace the U.S. Environment Protection Agency (EPA) 1995 Protocol factors, which were based on Method 21 monitoring of leaks at "uncontrolled" facilities. The emission factors published in the 1995 Protocol have not been updated since the 1970s. This derivation is based on results where the authors document the use of a Monte Carlo simulation technique to quantify the required leak detection thresholds that provide equal--or better--environmental benefits for an AWP. The use of these newly derived emission factors is demonstrated for different methods of computing fugitive emissions from a hypothetical model refinery. The resulting facility emissions calculated by using these new emission factors is compared with the existing emission estimation methods provided in the EPA 1995 Protocol. The results demonstrate that the new emission factors provide an emission estimate that is the closest to that obtained from the direct determination of total emissions by Monte Carlo simulations.     

Innovative approach for estimating fugitive gaseous fluxes using computed tomography and remote optical sensing techniques.

This paper presents a new approach to quantify emissions from fugitive gaseous air pollution sources. The authors combine Computed Tomography (CT) with Path-Integrated Optical Remote Sensing (PI-ORS) concentration data in a new field beam geometry. Path-integrated concentrations are sampled in a vertical plane downwind from the source along several radial beam paths. An innovative CT technique, which applies the Smooth Basis Function Minimization method to the beam data in conjunction with measured wind data, is used to estimate the total flux from the fugitive source. The authors conducted a synthetic data study to evaluate the proposed methodology under different meteorological conditions, beam geometry configurations, and simulated measurement errors. The measurement errors were simulated based on data collected with an Open-Path Fourier Transform Infra-Red system. This approach was found to be robust for the simulated errors and for a wide range of fluctuating wind directions. In the very sparse beam geometry examined (eight beam paths), successful emission rates were retrieved over a 70 degrees range of wind directions under extremely large measurement error conditions.     

垂直HDPE膜安装过程的电学破损检测方法

针对柔性垂直防渗帷幕的结构特点和场地条件,参考水平防渗系统破损检测的偶极子方法,提出了适用于柔性垂直防渗帷幕HDPE铺设过程破损检测的改进的方法和装置——缆式电法。结果表明,当HDPE垂直膜两侧施加高压直流电时,漏洞附近介质电势有明显异常,可以通过检测电势定位漏点位置。基于现场实验数据对模拟漏洞检测结果进行验证,最后基于验证后的数据讨论了缆式电法在柔性垂直防渗帷幕渗漏检测方面的可行性和影响因素,得出以下主要结论:缆式电法通过检测HDPE膜表面电势的异常点(极小值点)对漏洞位置进行定位,它能够对漏洞进行准确定位,定位精度在0.1 m以内,有效检测距离大于1 m;供电电极和检测传感器到膜的距离越近,漏洞信号越明显,越容易判断漏洞及其所在位置;检测传感器间距越小,漏洞信号越明显,越容易判断漏洞及其所在位置,检测漏点处偏离实际漏点位置的距离越小。     

Using satellite imagery to locate innovative forest management practices in Nepal

There is a critical need to locate innovative forest management institutions that significantly impact forest cover change. This research presents an initial "proof of concept" methodology which combines deforestation theory with satellite image change analysis to identify forested areas that, theoretically, should probably not be there. Ten such "forest anomalies" are identified using temporal analysis of Landsat TM imagery of the Chitwan district in Nepal, linked with a GIS database on roads and a visual estimation of topography. A rapid field reconnaissance is undertaken to determine which of these anomalies exhibit interesting forest management innovations. Based on this information, one case is selected for detailed field study: this turns out to be a major case of community forestry and a premier ecotourism initiative that we were not aware of until we undertook this analysis. The utility and limitations of the method are described for monitoring trends in forest cover change.     

Chemical composition of fugitive dust emitters in Mexico City

The gravimetric and chemical composition of fugitive dust emitters of Mexico City were analyzed to determine the particulate matter source profiles. Samples of geological material, unpaved and paved roads, agricultural soil, dried lake, asphalt, cement plants, landfill, gravel, and tezontle soil, were collected directly from the ground using a broom and a dustpan. These were dried, sieved and taken through a laboratory resuspension chamber to emulate the natural wind-blown processes of bulk soils and also to provide a uniform deposit on Teflon membrane and quartz fiber filters for further gravimetric and chemical analyses of PM_2.5 and PM₁₀ size fractions. Chemical analyses of the filters included X-ray fluorescence for elemental composition, ion chromatography for water soluble anions, atomic absorption for water soluble metals, automated colorimetric analysis for ammonium and thermal/optical reflectance analysis for carbon species. The data show that most fugitive emitters are composed of 20–30% PM_2.5, which is relatively less than the reported contribution by fossil fuels and biomass (40–60%).     

Field evaluation of digital optical method to quantify the visual opacity of plumes

Visual Determination of the Opacity of Emissions from Stationary Sources (Method 9) is a reference method established by U.S. Environmental Protection Agency (EPA) to quantify plume opacity. However, Method 9 relies on observations from humans, which introduces subjectivity. In addition, it is expensive to teach and certify personnel to evaluate plume opacity on a semiannual basis. In this study, field tests were completed during a "smoke school" and a 4-month monitoring program of plumes emitted from stationary sources with a Method 9 qualified observer to evaluate the use of digital photography and two computer algorithms as an alternative to Method 9. This Digital Optical Method (DOM) improves objectivity, costs less to implement than Method 9, and provides archival photographic records of the plumes. Results from "smoke school" tests indicate that DOM passed six of eight tests when the sun was located in the 140 degrees sector behind one of the three cameras, with the individual opacity errors of 15% or less and average opacity errors of 7.5% or less. DOM also passed seven of the eight tests when the sun was located in the 216 degrees sector behind another camera. However, DOM passed only one of the eight tests when the sun was located in the 116 degrees sector in front of the third camera. Certification to read plume opacity by a "smoke reader" for 6 months requires that the "smoke reader" pass one of the smoke school tests during smoke school. The average opacity errors and percentage of observations with individual opacity errors above 15% for the results obtained with DOM were lower than those obtained by the smoke school trainees with the sun was located behind the camera, whereas they were higher than the smoke school trainee results with the sun located in front of the camera. In addition, the difference between plume opacity values obtained by DOM and a Method 9 qualified observer, as measured in the field for two industrial sources, were 2.2%. These encouraging results demonstrate that DOM is able to meet Method 9 requirements under a wide variety of field conditions and, therefore, has potential to be used as an alternative to Method 9.     

冶金企业无组织排放颗粒物影响评价

以上海市某冶金企业为例,该厂有正常运行的冶炼炉13座,每年向大气中排放大量颗粒污染物.基于高斯倾斜烟羽模式,整理了2003年上海市全年的气象资料,运用气象概率矩阵法计算了该厂直排点源及无组织面源排放颗粒物的影响,得出了厂区内无组织排放颗粒物落地浓度等值线图.计算结果表明,厂区内颗粒物污染主要来自无组织面源,污染集中在厂区中心的污染源附近;直排点源对环境的影响较小,污染主要集中在下风向.     

Characterization of fugitive material within a primary lead smelter.

The primary production of Pb via the sinter plant-blast furnace method resulted in a large number of Pb and other phases, reflecting the complex reactions occurring within each of the processes. Optical microscopy and X-ray diffraction (XRD) techniques have been used to characterize fugitive emissions and dusts generated during sintering, smelting, Cu drossing, refining, and slag fuming at a primary Pb-Zn smelter. The results displayed a complex array of phases, with the mineralogy of the dusts and fume reflecting conditions of the particular metallurgical operation. The principal Pb species followed a transformation from PbS through PbSO4 and PbO to Pb(o) (metal) from raw materials to the refinery. The fugitive emissions generated by the blast furnace were of a finer size with more complex chemistry than fugitive material from other source areas. XRD identified a mixture of PbS, ZnO, and ZnS, associated with one or more of the Cl-bearing phases Pb(OH)Cl, PbCl2, Pb4O3Cl2, Na3Pb2(SO4)3Cl, Pb10(SO4)Cl2O8, Pb4SCl6, and Pb7S2Cl10. The presence of Cl-bearing phases in the fume has possible health implications.     

Geologic emissions of methane to the atmosphere

The atmospheric methane budget is commonly defined assuming that major sources derive from the biosphere (wetlands, rice paddies, animals, termites) and that fossil, radiocarbon-free CH4 emission is due to and mediated by anthropogenic activity (natural gas production and distribution, and coal mining). However, the amount of radiocarbon-free CH4 in the atmosphere, estimated at approximately 20% of atmospheric CH4, is higher than the estimates from statistical data of CH4 emission from fossil fuel related anthropogenic sources. This work documents that significant amounts of "old" methane, produced within the Earth crust, can be released naturally into the atmosphere through gas permeable faults and fractured rocks. Major geologic emissions of methane are related to hydrocarbon production in sedimentary basins (biogenic and thermogenic methane) and, subordinately, to inorganic reactions (Fischer-Tropsch type) in geothermal systems. Geologic CH4 emissions include diffuse fluxes over wide areas, or microseepage, on the order of 10(0)-10(2) mg m(-2) day(-1), and localised flows and gas vents, on the order of 10(2) t y(-1), both on land and on the seafloor. Mud volcanoes producing flows of up to 10(3) t y(-1) represent the largest visible expression of geologic methane emission. Several studies have indicated that methanotrophic consumption in soil may be insufficient to consume all leaking geologic CH4 and positive fluxes into the atmosphere can take place in dry or seasonally cold environments. Unsaturated soils have generally been considered a major sink for atmospheric methane, and never a continuous, intermittent, or localised source to the atmosphere. Although geologic CH4 sources need to be quantified more accurately, a preliminary global estimate indicates that there are likely more than enough sources to provide the amount of methane required to account for the suspected missing source of fossil CH4.     

印刷环节挥发性有机物无组织排放特征测定研究

对使用溶剂型油墨的凹版印刷设备和使用水性油墨的柔版印刷设备无组织排放的挥发性有机物(VOCs)浓度进行了实际监测,并采用计算流体动力学模拟无组织排放VOCs的收集效率。结果表明：(1)使用溶剂型油墨的凹版连续印刷过程非甲烷总烃(NMHC)最高均值达到5 975.67 mg/m³,约为使用水性油墨的柔版印刷(191.67 mg/m³)的31.2倍。虽然使用水性油墨可明显降低NMHC的排放,但其操作空间的浓度依然存在超过《工作场所有害因素职业接触限值第1部分：化学有害因素》(GBZ 2.1—2019)的现象。(2)印刷车间应该设置专门的调墨室,能缓解印刷车间内挥发性污染气体浓度的波动。(3)计算流体动力学模拟显示,设置合理的集气罩可有效降低VOCs的无组织排放,收集效率为70%～75%。     

A combined approach for the evaluation of a volatile organic compound emissions inventory

Emissions inventories significantly affect photochemical air quality model performance and the development of effective control strategies. However, there have been very few studies to evaluate their accuracy. Here, to evaluate a volatile organic compound (VOC) emissions inventory, we implemented a combined approach: comparing the ratios of carbon bond (CB)-IV VOC groups to nitrogen oxides (NOx) or carbon monoxide (CO) using an emission preprocessing model, comparing the ratios of VOC source contributions from a source apportionment technique to NOx or CO, and comparing ratios of CB-IV VOC groups to NOx or CO and the absolute concentrations of CB-IV VOC groups using an air quality model, with the corresponding ratios and concentrations observed at three sites (Maryland, Washington, DC, and New Jersey). The comparisons of the ethene/NOx ratio, the xylene group (XYL)/NOx ratio, and ethene and XYL concentrations between estimates and measurements showed some differences, depending on the comparison approach, at the Maryland and Washington, DC sites. On the other hand, consistent results at the New Jersey site were observed, implying a possible overestimation of vehicle exhaust. However, in the case of the toluene group (TOL), which is emitted mainly from surface coating and printing sources in the solvent utilization category, the ratios of TOL/ NOx or CO, as well as the absolute concentrations revealed an overestimate of these solvent sources by a factor of 1.5 to 3 at all three sites. In addition, the overestimate of these solvent sources agreed with the comparisons of surface coating and printing source contributions relative to NOx from a source apportionment technique to the corresponding value of estimates at the Maryland site. Other studies have also suggested an overestimate of solvent sources, implying a possibility of inaccurate emission factors in estimating VOC emissions from surface coating and printing sources. We tested the impact of these overestimates with a chemical transport model and found little change in ozone but substantial changes in calculated secondary organic aerosol concentrations.     

2010—2019年成都市机动车排污特征分析及防控措施减排效果评估

为评估2010—2019年成都市机动车防控措施的减排效果,以2010年为基准年,采用排放清单法计算了各减排措施下2019年的减排量,对比分析了4种控制措施的减排效益。结果表明：成都市机动车排污总量逐年下降,2019年PM_2.5、NO_x、VOCs、CO、SO₂和NH₃的排放量分别为0.27×10⁴、4.63×10⁴、1.70×10⁴、28.99×10⁴、0.21×10⁴和0.45×10⁴ t,主要分布在中心城区,其中重型货车对PM_2.5和NO_x贡献最大,小型客车对VOCs、CO、SO₂和NH₃贡献最大;措施中加严标准的综合减排量最大,重点减排车型为小型客车、轻型货车、公交车等,2019年6种污染物减排量分别为0.14×10⁴、2.27×10⁴、1.29×10⁴、6.77×10⁴、0.07×10⁴和0.38×10⁴ t;优化城市交通管理对小型客车和摩托车的减排效果显著,2019年6种污染物减排量分别为0.04×10⁴、0.81×10⁴、0.38×10⁴、2.55×10⁴、0.05×10⁴和0.04×10⁴ t;淘汰高排放车辆对小型客车、轻型货车等的减排较明显,2019年6种污染物减排放量分别为0.13×10⁴、0.98×10⁴、0.34×10⁴、2.62×10⁴、0.01×10⁴和0.007×10⁴ t;推广清洁能源汽车的重点减排车型为出租车和公交车,虽然可有效减少PM_2.5、NO_x的排放,但VOCs却有小幅增加,2019年6种污染物减排放量分别为0.12×10⁴、0.62×10⁴、−0.13×10⁴、0.30×10⁴、0.004×10⁴和0.000 5×10⁴ t。     

An automatic sampler for measurement of dust-deposition rates around fugitive sources

A wind-directional sampler for determination of dust-deposition rates has been developed, enabling the measurement of dust-deposition caused by a specific source and, at the same time, providing information on the dust-deposition rate for the background area. The sampler is called METDUST. This paper describes the results of a field evaluation of the METDUST sampler. The field evaluation was performed in a village in Southern Jutland, Denmark, where complaints of dust-deposition had occurred close to a power plant with large stockpiles of coal. The results showed that, out of a 9-month period, increased dust-deposition occurred downwind from the stockpiles during 4 months. Episodes were identified by comparison with the background deposition rate. The METDUST sampler offers an opportunity to measure the dust-deposition rate contributed by the source and the background simultaneously. It can, therefore, be used by environmental authorities to identify the "likelihood of complaint" and to define a suitable guideline for the case in question.