Harvard T.H. Chan School of Public Health, C-CHANGE, Boston, Massachusetts 02215 United States.
PSE Healthy Energy, Oakland, California 94612, United States.
Environ Sci Technol. 2022 Jul 19;56(14):10258-10268. doi: 10.1021/acs.est.1c08298. Epub 2022 Jun 28.
The presence of volatile organic compounds (VOCs) in unprocessed natural gas (NG) is well documented; however, the degree to which VOCs are present in NG at the point of end use is largely uncharacterized. We collected 234 whole NG samples across 69 unique residential locations across the Greater Boston metropolitan area, Massachusetts. NG samples were measured for methane (CH), ethane (CH), and nonmethane VOC (NMVOC) content (including tentatively identified compounds) using commercially available USEPA analytical methods. Results revealed 296 unique NMVOC constituents in end use NG, of which 21 (or approximately 7%) were designated as hazardous air pollutants. Benzene (bootstrapped mean = 164 ppbv; SD = 16; 95% CI: 134-196) was detected in 95% of samples along with hexane (98% detection), toluene (94%), heptane (94%), and cyclohexane (89%), contributing to a mean total concentration of NMVOCs in distribution-grade NG of 6.0 ppmv (95% CI: 5.5-6.6). While total VOCs exhibited significant spatial variability, over twice as much temporal variability was observed, with a wintertime NG benzene concentration nearly eight-fold greater than summertime. By using previous NG leakage data, we estimated that 120-356 kg/yr of annual NG benzene emissions throughout Greater Boston are not currently accounted for in emissions inventories, along with an unaccounted-for indoor portion. NG-odorant content (-butyl mercaptan and isopropyl mercaptan) was used to estimate that a mean NG-CH concentration of 21.3 ppmv (95% CI: 16.7-25.9) could persist undetected in ambient air given known odor detection thresholds. This implies that indoor NG leakage may be an underappreciated source of both CH and associated VOCs.
未经处理的天然气(NG)中存在挥发性有机化合物(VOCs)已得到充分证实;然而,在最终用途点 NG 中存在的 VOC 程度在很大程度上尚未得到描述。我们在马萨诸塞州大波士顿大都市区的 69 个独特住宅地点收集了 234 个完整的 NG 样本。使用市售的美国环保署分析方法测量 NG 样本中的甲烷(CH)、乙烷(CH)和非甲烷 VOC(NMVOC)含量(包括暂定鉴定的化合物)。结果显示,最终用途 NG 中有 296 种独特的 NMVOC 成分,其中 21 种(约 7%)被指定为有害空气污染物。苯(自举均值=164ppbv;SD=16;95%CI:134-196)在 95%的样品中检测到,同时还检测到正己烷(98%检测)、甲苯(94%)、正庚烷(94%)和环己烷(89%),导致分配级 NG 中 NMVOC 的平均总浓度为 6.0ppmv(95%CI:5.5-6.6)。虽然总 VOC 表现出显著的空间变异性,但观察到的时间变异性高出两倍,冬季 NG 中苯的浓度比夏季高近 8 倍。通过使用之前的 NG 泄漏数据,我们估计在大波士顿地区,每年有 120-356kg 的 NG 苯排放量目前未计入排放清单,还有一部分未计入室内排放。NG 气味剂含量(正丁硫醇和异丙硫醇)用于估计,在已知的气味检测阈值下,环境空气中 21.3ppmv(95%CI:16.7-25.9)的 NG-CH 平均浓度可能会持续未被检测到。这意味着室内 NG 泄漏可能是 CH 和相关 VOC 的一个被低估的来源。