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Long-term variability and source signature of gases emitted from oil & natural gas and cattle feedlot operations in the Colorado front range
Atmospheric Environment ( IF 5 ) Pub Date : 2021-08-14 , DOI: 10.1016/j.atmosenv.2021.118663
I. Ortega 1 , J.W. Hannigan 1 , R.R. Buchholz 1 , G. Pfister 1
Affiliation  

Multiple tropospheric gases are analyzed in ten years of observations (2010–2019) using a high-resolution ground-based solar absorption Fourier Transform InfraRed (FTIR) instrument in the Colorado Northern Front Range (CNFR). The first year of measurements in 2010 coincides with the start of the remarkable increase of oil and natural (O&NG) extraction in the region. We show seasonal variations and trends of atmospheric gases related to O&NG (C2H6), cattle feedlot activities (NH3), urban emissions (CO, C2H2), biomass burning (HCN), and volatile organic compounds related to photochemistry and ozone production (H2CO, HCOOH). The long-term time series of C2H6 shows clear episodic peak-enhancements related to local O&NG emissions that contribute to a positive trend of 0.9 ± 0.3% ⋅yr−1. NH3 also shows episodic enhancements and has the greatest rate of change for the gases studied here (2.7 ± 0.7% ⋅yr−1). Simulations of all gases are presented using the Community Atmosphere Model with chemistry (CAM-chem) within the Community Earth System Model (CESM) framework. Modeled gases are compared to the observations using different combinations of global emissions in order to determine the best combination for the CNFR. For most gases, using best emissions, the annual rate of change obtained with CAM-chem agrees with the FTIR observations, except for NH3, which is underestimated by a factor of 6. Nevertheless, simulations of NH3 show that the positive trend in NH3 is due to a decrease in its removal via reaction with H2SO4 from a reduction in coal power plant emissions. The seasonal variations of all gases are generally well represented in the model, although magnitudes are often underestimated. The anthropogenic emissions of CO, C2H2, and C2H6 are underestimated by about 20%, 40%, and 65%, respectively, independent of emission inventories. While NH3 summer values are underestimated significantly, other months show low relative mean difference between FTIR observations and CAM-chem simulations. Excellent agreement is found for H2CO, but for HCOOH a factor of 2–3 is needed in the simulations to match observations, pointing to a significant missing source. HCN, a tracer for biomass burning emissions, is well reproduced by the NCAR Fire Inventory (FINN). Furthermore, we show here a simple approach to identify local enhancements of gases related to nearby O&NG and concentrated animal feeding operations. These enhancements above ambient levels are used to estimate emission ratios (ER) of C2H6, H2CO, and HCOOH relative to CO from O&NG air masses. A median ER (and standard deviation) of 0.48 ± 0.41, 0.26 ± 0.15, and 0.13 ± 0.09 [ppb/ppb] are estimated for C2H6, H2CO, and HCOOH, respectively and are representative of the ten years of observations. ER can be used to estimate emission factors (EF), although CO emissions from O&NG need to be well-known. To complement the FTIR observations, we show results derived with airborne observations during The Front Range Air Pollution and Photochemical Experiment (FRAPPE) in 2014. Even though FTIR and FRAPPE observations can not be compared easily they both yield similar median ER. Finally, plumes of fires originated in the western United States in August 2015 were identified and EF are estimated.



中文翻译:

科罗拉多前沿范围内石油和天然气以及牛饲养场作业排放的气体的长期可变性和来源特征

使用高分辨率地基太阳能吸收傅里叶变换红外 (FTIR) 仪器在科罗拉多北锋范围 (CNFR) 的十年观测中(2010-2019 年)分析了多种对流层气体。2010 年测量的第一年恰逢该地区石油和天然(O NG)开采量显着增加的开始。我们展示了与 O & NG (C 2 H 6 )、牛饲养场活动 (NH 3 )、城市排放 (CO, C 2 H 2 )、生物质燃烧 (HCN) 和挥发性有机化合物相关的大气气体的季节性变化和趋势与光化学和臭氧生产有关(H 2CO,HCOOH)。C 2 H 6的长期时间序列显示出与本地 ONG 排放相关的明显间歇性峰值增强,这有助于 0.9 ± 0.3 % ⋅yr -1的积极趋势。NH 3也显示出偶发增强,并且对于此处研究的气体具有最大的变化率 (2.7 ± 0.7 % ⋅yr -1)。所有气体的模拟都使用社区地球系统模型 (CESM) 框架内的社区大气模型和化学 (CAM-chem) 呈现。使用全球排放的不同组合将模拟气体与观测值进行比较,以确定 CNFR 的最佳组合。对于大多数气体,使用最佳排放,使用 CAM-chem 获得的年变化率与 FTIR 观测结果一致,除了 NH 3被低估了 6 倍。然而,NH 3 的模拟表明NH 3是由于通过与 H 2 SO 4反应而去除的减少来自煤电厂排放的减少。所有气体的季节性变化通常在模型中得到很好的体现,尽管幅度经常被低估。CO、C 2 H 2和C 2 H 6的人为排放分别被低估了约20 %、40 %和65 %,与排放清单无关。虽然 NH 3夏季值被显着低估,但其他月份的 FTIR 观测值和 CAM 化学模拟之间的相对平均差异较低。H 2 具有极好的一致性CO,但对于 HCOOH,模拟中需要 2-3 的因子来匹配观察结果,指出一个重要的缺失源。NCAR 火灾清单 (FINN) 很好地再现了 HCN 是生物质燃烧排放的示踪剂。此外,我们在这里展示了一种简单的方法来识别与附近 O & NG 和集中动物饲养操作相关的气体的局部增强。这些高于环境水平的增强用于估计 C 2 H 6、H 2 CO 和 HCOOH 相对于来自 O & NG 气团的CO 的排放比 (ER) 。估计 C 2 H 6、H 2 的中值 ER(和标准偏差)为 0.48 ± 0.41、0.26 ± 0.15 和 0.13 ± 0.09 [ppb/ppb]CO 和 HCOOH 分别代表十年的观察结果。ER 可用于估算排放因子 (EF),但 ONG 的CO 排放需要众所周知。为了补充 FTIR 观测,我们展示了 2014 年前沿空气污染和光化学实验 (FRAPPE) 期间通过机载观测得出的结果。尽管 FTIR 和 FRAPPE 观测无法轻易比较,但它们都产生了相似的中值 ER。最后,确定了 2015 年 8 月起源于美国西部的火羽,并估算了 EF。

更新日期:2021-08-21
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