Institute for Climate and Atmospheric Science, Department of Earth and Atmospheric Sciences, University of Houston , Houston, Texas 77004, United States.
Environ Sci Technol. 2015 Sep 1;49(17):10692-700. doi: 10.1021/acs.est.5b02287. Epub 2015 Aug 13.
Atmospheric mercury emissions in the Barnett Shale area were studied by employing both stationary measurements and mobile laboratory surveys. Stationary measurements near the Engle Mountain Lake showed that the median mixing ratio of total gaseous mercury (THg) was 138 ppqv (140 ± 29 ppqv for mean ± S.D.) during the June 2011 study period. A distinct diurnal variation pattern was observed in which the highest THg levels appeared near midnight, followed by a monotonic decrease until midafternoon. The influence of oil and gas (ONG) emissions was substantial in this area, as inferred from the i-pentane/n-pentane ratio (1.17). However, few THg plumes were captured by our mobile laboratory during a ∼3700 km survey with detailed downwind measurements from 50 ONG facilities. One compressor station and one natural gas condensate processing facility were found to have significant THg emissions, with maximum THg levels of 963 and 392 ppqv, respectively, and the emissions rates were estimated to be 7.9 kg/yr and 0.3 kg/yr, respectively. Our results suggest that the majority of ONG facilities in this area are not significant sources of THg; however, it is highly likely that a small number of these facilities contribute a relatively large amount of emissions in the ONG sector.
本研究采用固定站观测和车载移动观测相结合的方式,对 Barnett Shale 地区的大气汞排放进行了研究。Engle Mountain Lake 附近固定站观测结果表明,2011 年 6 月研究期间总气态汞(THg)的中值混合比为 138 ppqv(均值±标准偏差为 140 ± 29 ppqv)。观测结果呈现明显的日变化特征,THg 浓度在午夜附近最高,随后单调下降直至午后。该地区油气(ONG)排放对大气汞的影响较大,这可以从异戊烷/正戊烷的比值(1.17)推断得出。然而,在对 50 个 ONG 设施进行详细的下风测量、长达约 3700km 的车载移动观测中,我们仅捕获到少量的大气汞羽流。其中一个压缩机站和一个天然气凝析油处理设施被发现存在显著的 THg 排放,最大 THg 浓度分别为 963 和 392 ppqv,排放速率分别估计为 7.9 kg/yr 和 0.3 kg/yr。研究结果表明,该地区大多数 ONG 设施并非大气汞的重要排放源;但仍极有可能是少数设施在该地区的 ONG 排放中贡献了相对较大的排放量。