Phillips 66 Research Center , Highway 60 and 123, Bartlesville , Oklahoma 74003 , United States.
Environ Sci Technol. 2018 Mar 6;52(5):3285-3294. doi: 10.1021/acs.est.7b05726. Epub 2018 Feb 21.
A total of three ground-based ambient air studies were conducted in February through March of 2015, 2016, and 2017 at the Phillips 66 Research Center in northeastern Oklahoma. C-C nonmethane hydrocarbons (NMHCs) were measured using whole-air sampling and gas chromatography-mass spectrometry. In 2016 and 2017, online methane and ethane measurements were also conducted. Strong methane-ethane correlation identified oil and gas (O&G) upstream and midstream operations to be the primary methane source. C-C alkanes were the dominant NMHCs whose average mixing ratio peaked in 2016 before dropping in 2017. This observation is attributed to regional O&G upstream operations, which peaked in 2015. Mean mixing ratios of C-C alkanes ranged from 0.99 to 16.99 ppb. Measured ratios of i-C/ n-C were 0.97 ± 0.03, 1.18 ± 0.04, and 1.06 ± 0.02 in 2015, 2016, and 2017, respectively, indicating that O&G upstream and midstream operations were their primary source. Photochemical age was estimated using observed ratio between hexane and propane. Emission ratios of NMHCs at zero photochemical age were calculated, which resembled the composition reported in the literature for natural gas field condensate tank flashing. Back-trajectory analysis showed that hydrocarbon-rich plumes came from the south and west directions, where O&G upstream and midstream operations are abundant. High OH reactivity values were calculated from C-C alkanes mixing ratios, with the average reactivity for the 3 years being 1.55, 1.88, and 1.16 s. This indicates that VOC emissions from O & G operations may contribute to ozone production.
在 2015 年 2 月至 3 月、2016 年和 2017 年,总共在俄克拉荷马州东北部的菲利普斯 66 研究中心进行了三项基于地面的环境空气研究。使用全空气采样和气相色谱-质谱法测量 C-C 非甲烷碳氢化合物 (NMHC)。在 2016 年和 2017 年,还进行了在线甲烷和乙烷测量。强甲烷-乙烷相关性表明,上游和中游的石油和天然气 (O&G) 作业是主要的甲烷源。C-C 烷烃是主要的 NMHC,其平均混合比在 2016 年达到峰值,然后在 2017 年下降。这一观察结果归因于 2015 年达到峰值的区域 O&G 上游作业。C-C 烷烃的平均混合比范围为 0.99 至 16.99 ppb。2015 年、2016 年和 2017 年测量的 i-C/n-C 比值分别为 0.97±0.03、1.18±0.04 和 1.06±0.02,表明 O&G 上游和中游作业是其主要来源。使用观测到的己烷和丙烷之间的比值估算光化学年龄。计算了零光化学年龄下 NMHC 的排放比,其组成与文献中报道的天然气田凝析油闪蒸罐的组成相似。后向轨迹分析表明,富含碳氢化合物的羽流来自南方和西方,那里 O&G 上游和中游作业丰富。根据 C-C 烷烃混合比计算得到高 OH 反应性值,3 年的平均反应性分别为 1.55、1.88 和 1.16 s。这表明 O&G 作业的 VOC 排放可能有助于臭氧生成。