Vimont, IJ, et al. 2017 Carbon monoxide isotopic measurements in Indianapolis constrain urban source isotopic signatures and support mobile fossil fuel emissions as the dominant wintertime CO source. Elem Sci Anth, 5: 63. DOI: https://doi.org/10.1525/elementa.136
IntroductionUrban carbon monoxide (CO) is a regulated pollutant that impacts human health and influences atmospheric chemistry via its interaction with OH and its role in tropospheric ozone production. Urban emissions are also an important component of the global CO budget (Crutzen, 1973;Crutzen, 1979;Logan et al., 1981;Duncan et al., 2007). Within urban areas of the United States, CO emissions inventories may be inaccurate by as much as a factor of two (e.g. Turnbull et al., 2015;Parrish et al., 2006;Graven et al., 2009;LaFranchi et al., 2013; EPA NEI 2011). In addition to the atmospheric chemistry and health impacts, CO has been explored as a tracer for fossil fuel derived CO 2 (CO 2ff ) (Meijer et al., 1996;Levin and Karstens, 2007;Turnbull et al., 2006;Vogel et al., 2010;Turnbull et al., 2011; Turnbull et al., 2015). This method relies on an assumption that CO is produced entirely by combustion, which is not always true within urban regions (Turnbull et al., 2015). Turnbull et al. (2015) found that during winter at Indianapolis, using CO as a correlate tracer yielded CO 2ff enhancements that were in good agreement with those from 14 CO 2 measurements. This suggested that during the winter at Indianapolis, non-fossil fuel sources of CO do not contribute significantly. In contrast, during the summer, there is weaker correlation between CO and 14 C-derived CO 2ff , suggesting another summertime source of CO in Indianapolis (Turnbull et al., 2015) and in other locations (Turnbull et al., 2006;Miller et al., 2012). Stable isotopic measurements of urban CO can help quantify individual CO sources and sinks and provide an improved understanding of seasonal changes in the urban CO budget (e.g. Stevens et al., 1972;Brenninkmeijer, 1993;Conny, 1998).In order to quantify the sources and sinks of CO via isotopic analysis, the 13 CO and C 18 O isotopic signatures need to be known (Stevens et al., 1972;Brenninkmeijer, 1993;Rockmann and Brenninkmeijer, 1997; O) in air during the winters of 2013-14 and 2014-15 at tall tower sampling sites in and around Indianapolis, USA. A tower located upwind of the city was used to quantitatively remove the background CO signal, allowing for the first unambiguous isotopic characterization of the urban CO source and yielding
13CO of -27.7 ± 0.5‰ VPDB and C
18O of 17.7 ± 1.1‰ VSMOW for this source. We use the tower isotope measurements, results from a limited traffic study, as well as atmospheric reaction rates to examine contributions from different sources to the Indianapolis CO budget. Our results are consistent with earlier findings that traffic emissions are the dominant source, suggesting a contribution of 96% or more to the overall Indianapolis wintertime CO emissions. Our results are also consistent with the hypothesis ...