Atmospheric Measurements

2013
Xuan Wang, Yuxuan Wang, Jiming Hao, Yutaka Kondo, Martin Irwin, J. William Munger, and Yongjing Zhao. 2013. “Top-down estimate of China's black carbon emissions using surface observations: Sensitivity to observation representativeness and transport model error.” Journal of Geophysical Research, 118, 11, Pp. 5781-5795. Publisher's VersionAbstract

This study examines the sensitivity of “top-down” quantification of Chinese black carbon (BC) emissions to the temporal resolution of surface observations and to the transport model error associated with the grid resolution and wet deposition. At two rural sites (Miyun in North China Plain and Chongming in Yangtze River Delta), the model-inferred emission bias based on hourly BC observations can differ by up to 41% from that based on monthly mean observations. This difference relates to the intrinsic inability of the grid-based model in simulating high pollution plumes, which often exert a larger influence on the arithmetic mean of observations at monthly time steps. Adopting the variation of BC to carbon monoxide correlation slope with precipitation as a suitable measure to evaluate the model's wet deposition, we found that wet removal of BC in the model was too weak, due in part to the model's underestimation of large precipitation events. After filtering out the observations during high pollution plumes and large precipitation events for which the transport model error should not be translated into the emission error, the inferred emission bias changed from −11% (without filtering) to −2% (with filtering) at the Miyun site, and from −22% to +1% at the Chongming site. Using surface BC observations from three more rural sites (located in Northeast, Central, and Central South China, respectively) as constraints, our top-down estimate of total BC emissions over China was 1.80 ± 0.65 Tg/yr in 2006, 0.5% lower than the bottom-up inventory of Zhang et al. (2009) but with smaller uncertainty.

2012
Yu Zhao, Chris P Nielsen, and Michael B. McElroy. 2012. “China's CO2 emissions estimated from the bottom up: Recent trends, spatial distributions, and quantification of uncertainties.” Atmospheric Environment, 59, Pp. 214-223. Publisher's VersionAbstract
China's emissions of anthropogenic CO2 are estimated using a bottom-up emission inventory framework based on a detailed categorization of economic sectors and provincial economic and energy data. It includes a newly compiled database of CO2 emission factors employing the latest field study results from China. Total annual emissions are estimated to have risen from 7126 to 9370 Mt CO2 from 2005 to 2009. Recent policies to conserve energy and reduce emissions have been effective in limiting CO2 emissions from power and iron & steel plants, but have had little effect on those from cement production. The uncertainties of China's CO2 emissions are quantified for the first time using Monte-Carlo simulation, producing a 95% confidence interval (CI) of −9% to +11% for total emissions in 2005. The largest contributors to sector-level emission uncertainty are emission factors for most industrial sources and activity levels for power plants, transportation, and residential & commercial sources. Application of province-level energy consumption and China-specific emission factors in some sectors results in higher annual emission estimates for 2005-2008 as compared with other studies, although most of those are within the 95% CIs of this study.
Yu Zhao, Chris P Nielsen, Michael B. McElroy, Lin Zhang, and Jie Zhang. 2012. “CO emissions in China: Uncertainties and implications of improved energy efficiency and emission control.” Atmospheric Environment, 49, Pp. 103-113. Publisher's VersionAbstract
A bottom-up methodology and an improved database of emission factors combining the latest domestic field measurements are developed to estimate the emissions of anthropogenic CO from China at national and provincial levels. The CO emission factors for major economic sectors declined to varying degrees from 2005 to 2009, attributed to improved energy efficiency and/or emission control regulations. Total national CO emissions are estimated at 173 Tg for 2005 and have been relatively stable for subsequent years, despite fast growth of energy consumption and industrial production. While industry and transportation sources dominated CO emissions in developed eastern and north-central China, residential combustion played a much greater role in the less developed western provinces. The uncertainties of national Chinese CO emissions are quantified using Monte Carlo simulation at −20% to +45% (95% confidence interval). Due to poor understanding of emission factors and activity levels for combustion of solid fuels, the largest uncertainties are found for emissions from the residential sector. The trends of bottom-up emissions compare reasonably to satellite observation of CO columns and to ground observations of CO2–CO correlation slopes. The increase in the ratio for emissions of CO2 relative to CO suggests that China has successfully improved combustion efficiencies across its economy in recent years, consistent with national policies to improve energy efficiency and to control criteria air pollutants.
2011
Yuxuan Wang, Xuan Wang, Yutaka Kondo, Mizuo Kajino, J. William Munger, and Jiming Hao. 2011. “Black carbon and its correlation with trace gases at a rural site in Beijing: implications for regional emissions.” Journal of Geophysical Research, 116, D24. Publisher's VersionAbstract
The mass concentrations of black carbon (BC) were measured continuously at Miyun, a rural site near Beijing, concurrently with some trace gases (CO, CO2, NOy, SO2) during the nonheating seasons of 2010 (April to October). The average concentration of BC was 2.26 ± 2.33 μg m−3. About 70%–100% of the air masses arriving at the site from June to September were from the source region of Beijing and the North China Plain (NCP), while in the spring, 40% were of continental background origin. BC had moderate to strong positive correlations with CO (R2 = 0.51), NOy (R2 = 0.58), and CO2 (nonsummer, R2 = 0.54), but not with SO2 (R2 < 0.1). The observed ΔBC/ΔCO ratio was 0.0050 ± 0.0001 μg m−3/ppbv for the regional air masses (excluding the influence of biomass burning). This ratio increased by 68% to 0.0084 ± 0.0004 μg m−3/ppbv after excluding the influence of wet deposition. Accounting further for the impact of atmospheric processes on the observation, we derived an average top‐down BC/CO emission ratio of 0.0095 ± 0.002 μg m−3/ppbv for the source region of Beijing and NCP that is 18%–21% lower than the average emission ratio from the bottom‐up inventory of Zhang et al. (2009), whereas the difference is substantially lower than the uncertainty of emissions for either species. The difference between the mean bottom‐up and top‐down emission ratios is most likely to be attributed to the residential sector, which needs to have a lower share in the total emissions of BC or a much lower BC/CO emission ratio. The industry and transportation sectors are found to be dominant sources of BC from Beijing and the NCP rather than from the residential sector as suggested by the bottom‐up inventory.
2010
Yuxuan Wang, J. William Munger, Shicheng Xu, Michael B. McElroy, Jiming Hao, Chris P Nielsen, and Hong Ma. 2010. “CO2 and its correlation with CO at a rural site near Beijing: Implications for combustion efficiency in China.” Atmospheric Chemistry and Physics, 10, Pp. 8881-8897. Publisher's VersionAbstract
Although China has surpassed the United States as the world’s largest carbon dioxide emitter, in situ measurements of atmospheric CO2 have been sparse in China.
This paper analyzes hourly CO2 and its correlation with CO at Miyun, a rural site near Beijing, over a period of 51 months (Dec 2004 through Feb 2009). The CO2-CO correlation analysis evaluated separately for each hour of the day provides useful information with statistical significance even in the growing season. We found that the intercept, representing the initial condition imposed by global distribution of CO2 with influence of photosynthesis and respiration, exhibits diurnal cycles differing by season. The background CO2 (CO2,b) derived from Miyun observations is comparable to CO2 observed at a Mongolian background station to the northwest.  Annual growth of overall mean CO2 at Miyun is estimated at 2.7 ppm yr−1 while that of CO2,b is only 1.7 ppm yr−1 similar to the mean growth rate at northern mid-latitude background stations. This suggests a relatively faster increase in the regional CO2 sources in China than the global average, consistent with bottom-up studies of CO2 emissions. For air masses with trajectories through the northern China boundary layer, mean winter CO2/CO correlation slopes (dCO2/dCO) increased by 2.8±0.9 ppmv/ppmv or 11% from 2005–2006 to 2007–2008, with CO2 increasing by 1.8 ppmv. The increase in dCO2/dCO indicates improvement in overall combustion efficiency over northern China after winter 2007, attributed to pollution reduction measures associated with the 2008 Beijing Olympics. The observed CO2/CO ratio at Miyun is
25% higher than the bottom-up CO2/CO emission ratio, suggesting a contribution of respired CO2 from urban residents as well as agricultural soils and livestock in the observations and uncertainty in the emission estimates. 
Yuxuan Wang, Michael B. McElroy, J. William Munger, Jiming Hao, Hong Ma, and Chris P Nielsen. 2010. “Year-round measurements of O3 and CO at a rural site near Beijing: Variations in their correlations.” Tellus B: Chemical and Physical Meteorology, 62, 4, Pp. 228-241. Publisher's VersionAbstract
 

ABSTRACT

We examine seasonal variations of carbon monoxide (CO), ozone (O3), and their relationships observed over the course of 3 yr (2005–2007) at Miyun, a rural site 100 km north of Beijing. Monthly mean afternoon mixing ratios of CO have broad maxima in winter and a secondary peak in June. Monthly mean afternoon O3 shows a clear seasonal pattern with a major peak in June (85 ppb), a secondary peak in September (65 ppb) and minimum in winter (50–55 ppb). The seasonal cycles of O3 and CO are associated with seasonal changes in dominant synoptic pattern. Substantial interannual variability is found for CO which is attributed to the interannual variability of meteorology and emissions from biomass burning. The seasonality and magnitude of background CO and O3 derived at Miyun are consistent with observations at upwind remote continental sites. The O3–CO correlation slope is about 0.07 ppb ppb−1 on average in summer, significantly lower than the typical slope of 0.3 ppb ppb−1 reported for developed countries. The O3–CO correlation slope shows large gradients for different types of air masses (0.133 ± 0.017 ppb ppb−1 in aged urban pollution plumes and 0.047 ± 0.008 ppb ppb−1 in biomass burning plumes), suggesting that the conventional method of direct scaling the mean O3–CO slope by CO emissions to deduce O3 production rate is subject to large uncertainties if applied for China.

2009
Yuxuan Wang, Jiming Hao, Michael B. McElroy, J. William Munger, Hong Ma, Dan Chen, and Chris P Nielsen. 2009. “Ozone air quality during the 2008 Beijing Olympics: Effectiveness of emission restrictions.” Atmospheric Chemistry and Physics, 9, 14, Pp. 5237-5251. Publisher's VersionAbstract
A series of aggressive measures was launched by
the Chinese government to reduce pollutant emissions from
Beijing and surrounding areas during the Olympic Games.
Observations at Miyun, a rural site 100 km downwind of the
Beijing urban center, show significant decreases in concentrations
of O3, CO, NOy, and SO2 during August 2008, relative
to August 2006–2007. The mean daytime mixing ratio
of O3 was lower by about 15 ppbv, reduced to 50 ppbv, in
August 2008. The relative reductions in daytime SO2, CO,
and NOy were 61%, 25%, and 21%, respectively. Changes in
SO2 and in species correlations from 2007 to 2008 indicate
that emissions of SO2, CO, and NOx were reduced at least
by 60%, 32%, and 36%, respectively, during the Olympics.
Analysis of meteorological conditions and interpretation of
observations using a chemical transport model suggest that
although the day-to-day variability in ozone is driven mostly
by meteorology, the reduction in emissions of ozone precursors
associated with the Olympic Games had a significant
contribution to the observed decrease in O3 during August
2008, accounting for 80% of the O3 reduction for the
month as a whole and 45% during the Olympics Period (8–
24 August). The model predicts that emission restrictions
such as those implemented during the Olympics can affect
O3 far beyond the Beijing urban area, resulting in reductions
in boundary layer O3 of 2–10 ppbv over a large region of the
North China Plain and Northeastern China.
2008
Yuxuan Wang, Michael B. McElroy, J. William Munger, Jiming Hao, Hong Ma, Chris P Nielsen, and Yaosheng Chen. 2008. “Variations of O3 and CO in summertime at a rural site near Beijing.” Atmospheric Chemistry and Physics, 8, 21, Pp. 6355-6363. Publisher's VersionAbstract
Large intra-season differences in mixing ratios of
CO and O3 were detected at Miyun, a rural site north of Beijing,
in summer 2006. Despite an increase in mean daytime
mixing ratio of CO from 500 ppbv in June to 700 ppbv in
July, mean daytime O3 dropped from 67 ppbv in June to 50
ppbv in July and August. The observed changes in CO and
O3 are attributed to the influence of the summer monsoonal
circulation that develops over the North China Plain in July.
Photochemical production of O3 is reduced as a consequence
of increased cloudiness during July and August, as indicated
by the strong negative correlation observed between O3 and
satellite observations of cloud optical depth, with cloudiness
having little effect on CO. The analysis suggests a strategy
for emission controls that could be implemented in an economically
efficient manner to minimize the frequency of high
levels of O3 during summer in Beijing.
2003
P. Suntharalingam, C. M. Spivakovsky, J. A. Logan, and M.B. McElroy. 2003. “Estimating the distribution of terrestrial CO2 sources and sinks from atmospheric measurements: Sensitivity to configuration of the observation network.” Journal of Geophysical Research, 108, D15. Publisher's VersionAbstract
We explore the sensitivity of terrestrial CO2 flux estimates from a specific inversion methodology, based on the configuration of Fan et al. [1998], to different configurations of the global observation network. Using diagnostics derived from the inversion equations, we focus on quantifying the relative influence of individual stations on the flux estimates. We also examine the impact of different assumptions for the data uncertainty values by contrasting weighted and unweighted inversions and presenting related sensitivity analyses. For this particular methodology, unweighted estimates of continental scale fluxes prove very sensitive to network configuration. The inclusion or omission of a few important stations in and around the northern continents can result in shifts in continental‐scale flux estimates of up to 1.5 Gt C/year. The weighted estimates are less sensitive to network configuration. Diagnostics of relative station influence indicate that this results from the reduced roles of previously influential continental sites; i.e., those stations characterized by high levels of data uncertainty. In the weighted approach, stations on continental peripheries associated with lower levels of data uncertainty are the most important in determining terrestrial fluxes. Finally, using the diagnostics of relative station influence, we discuss potential sampling strategies for the determination of regional fluxes from surface measurements.

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