Relationships of trace gases and aerosols and the emission characteristics at Lin'an, a rural site in eastern China, during spring 2001

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Abstract

[1] We present measurements of trace gases and fine aerosols obtained from a rural site in eastern China during 18 February to 30 April 2001. The field program aimed to characterize the variations in aerosol and gaseous pollutant concentrations and the emission signatures from the inland region of eastern China in the spring season. The data included O3, CO, NO, NOy*, SO2, methane, C2-C8 nonmethane hydrocarbons (NMHCs), C1-C2 halocarbons, and the chemical composition of PM2.5. The average hourly mixing ratios (±standard deviation) of CO, SO2, and NOy* were 677 (±315) ppbv, 15.9 (±14.6) ppbv, and 13.8 (±7.2) ppbv, respectively. The mean daytime ozone mixing ratio was 41 (±19) ppbv. The most abundant NMHC was ethane (3189 ± 717 pptv), followed by ethyne (2475 ± 1395 pptv), ethene (1679 ± 1455 pptv), and toluene (1529 ± 1608 pptv). Methyl chloride was the most abundant halocarbon (1108 ± 653 pptv). The average concentrations of particulate organic matter (POM, as organic carbon, OC, times 1.4) and elemental carbon (EC) in PM2.5 were 21.5 (±7) μg/m3 and 2.5 (±0.7) μg/m3, respectively, and sulfate and nitrate levels were 17.3 (±6.6) and 6.5 (±4) μg/m3, respectively. CO showed moderate to good correlation with NOy* (r2 = 0.59), OC (r2 = 0.65), CH3Cl (r2 = 0.59), soluble potassium (r2 = 0.53), and many NMHCs, indicating contributions from the burning of biofuel/biomass. CO also correlated with an industrial tracer, C2Cl4, indicative of some influence from industrial sources. SO2, on the other hand, correlated well with EC (r2 = 0.56), reflecting the contribution from the burning of coal. Ammonium was sufficiently abundant to fully neutralize sulfate and nitrate, indicating that there were strong emissions of ammonia from agricultural activities. Silicon and calcium had poor correlations with iron and aluminum, revealing the presence of source(s) for Si and Ca other than from soil. Examination of C2H2/CO, C3H8/C2H6, nitrate/(nitrate + NOy*), and sulfate/(SO2 + sulfate) suggested that relatively fresh air masses had been sampled at the study site in the spring season. Comparison of the observed ratios/slopes with those derived from emission inventories showed that while the observed SO2/NOy* ratio (1.29 ppbv/ppbv) in March was comparable (within 20%) to the inventory-derived ratio for the study region, the measured CO/NOy* slope (37 ppbv/ppbv) was about 200% larger. The observed slope of CO relative to NMHC (including ethane, propane, butanes, ethene, and ethyne) also indicated the presence of excess CO, compared to the ratios from the inventories. These results strongly suggest that emissions of CO in eastern China have been underrepresented. The findings of this study highlight the importance of characterizing trace gases and aerosols within source regions of the Asian continent. The springtime results were also compared with data previously collected at the site in 1999–2000 and with those obtained on the Transport and Chemical Evolution over the Pacific (TRACE-P) aircraft and from a coastal site in South China for the same study period.

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