Guorui Zhi

Measurements of emission factors for primary carbonaceous particles from residential raw‐coal combustion in China

The emission factors (EFs) of particles and their carbonaceous fractions, including black carbon (BC) and organic carbon (OC), are measured for residential burning of coal-chunks. Nine types of coals with wide-ranged thermal maturities were used. Particulate emissions from coal-stove are collected on quartz fiber filters through a dilution sampling system and analyzed for BC and OC by thermal-optical method. The EFs of particulate matter, OC, and BC from bituminous coal burning are 16.77, 8.29, and 3.32 g/kg, respectively, on the basis of burned dry and ash-free (daf) coal mass. They were much higher than those of anthracites, which are 0.78, 0.04, and 0.004 g/kg, respectively. Annual emission inventories of particles, OC, and BC from household coal burning are also estimated based on the EFs and coal consumption. The results of the calculations are 917.8, 477.7, and 128.4 gigagrams (Gg) for total particles, OC, and BC emitted in China during the year 2000.

Measurements of Black and Organic Carbon Emission Factors for Household Coal Combustion in China: Implication for Emission Reduction

Household coal combustion is considered as the greatest emission source for black carbon (BC) and an important source for organic carbon (OC) in China. However, measurements on BC and OC emission factors (EF(BC) and EF(OC)) are still scarce, which result in large uncertainties in emission estimates. In this study, a detailed data set of EF(BC) and EF(OC) for household coal burning was presented on the basis of 38 coal/stove combination experiments. These experiments included 13 coals with a wide coverage of geological maturity which were tested in honeycomb-coal-briquette and raw-coal-chunk forms in three typical coal stoves. Averaged values of EF(BC) are 0.004 and 0.007 g/kg for anthracite in briquette and chunk forms and 0.09 and 3.05 g/kg for bituminous coal, respectively; EF(OC) are 0.06 and 0.10 g/kg for anthracite and 3.74 and 5.50 g/kg for bituminous coal in both forms, respectively. Coal maturity was found to be the most important influencing factor relative to coals burning forms and the stoves burning efficiency, and when medium-volatile bituminous coals (MVB) are excluded from use, averaged EF(BC) and EF(OC) for bituminous coal decrease by 50% and 30%, respectively. According to these EFs, Chinas BC and OC emissions from the household sector in 2000 were 94 and 244 gigagrams (Gg), respectively. Compared with previous BC emission estimates for this sector (e.g., 465 Gg by Ohara et al., Atmos. Chem. Phys. 2007, 7, 4419-4444), a dramatic decrease was observed and was mainly attributed to the update of EFs. As suggested by this study, if MVB is prohibited as household fuel together with further promotion of briquettes, BC and OC emissions in this sector will be reduced by 80% and 34%, respectively, and then carbonaceous emissions can be controlled to a large extent in China.

Increase in polycyclic aromatic hydrocarbon (PAH) emissions due to briquetting: A challenge to the coal briquetting policy

Both China and UNEP recommend replacing raw coal chunks with coal briquettes in household sector as clean coal technology (CCT), which has been confirmed by the decreased emissions of particulate matter and black carbon. However, the clean effect has never been systematically checked by other pollutants like polycyclic aromatic hydrocarbons (PAHs). In this study, 5 coals with different geological maturities were processed as both chunks and briquettes and burned in 3 typical coal stoves for the measurement of emission factors (EFs) of particle-bound PAHs. It was found that the EFs of 16 parent PAHs, 26 nitrated PAHs, 6 oxygenated PAHs, and 8 alkylated PAHs for coal briquettes were 6.90 ± 7.89, 0.04 ± 0.03, 0.65 ± 0.40, and 72.78 ± 18.23 mg/kg, respectively, which were approximately 3.1, 3.7, 1.9, and 171 times those for coal chunks, respectively. Such significant increases in PAH emissions increased human health risk and challenged the policy of CCT.

Harmonizing Aerosol Carbon Measurements between Two Conventional Thermal/Optical Analysis Methods

Although total carbon (TC) can be consistently quantified by various aerosol carbon measurement methods, the demarcation of TC into organic carbon (OC) and elemental carbon (EC) has long been inconsistent. The NIOSH and IMPROVE protocols are most widely used for thermal/optical analysis (TOA), but current knowledge rests in the description that the NIOSH protocol usually gives lower EC values than does the IMPROVE protocol. This study seeks to explore the possibility of quantitatively linking the difference between the two TOA protocols. Residential coal-burning samples that had been collected and analyzed following the NIOSH protocol in previous studies were directly reanalyzed following the IMPROVE protocol for this study. A comparison of each pair of NIOSH and IMPROVE EC values reveals the dynamic relation between the two protocols, which can be expressed as a regression equation, y=(1-x)/(1+4.86x2) (R2=0.96), where the independent x is the EC/TC ratio R(EC/TC) for the IMPROVE protocol, and the dependent y is the difference between IMPROVE and NIOSH REC/TC relative to IMPROVE REC/TC. This regression equation may be the first effort in formulating the relationship between the two TOA protocols, and it is very helpful in harmonizing inconsistent TOA measurements, for example, source characterization, ambient monitoring, and atmospheric modeling.

Air pollutant emission from the underestimated households' coal consumption source in China.

In order to improve the regional air quality, many control strategies have been developed by Chinese government for reducing air pollutant emission from power plants, industrial and transport sources during the past decade. However, little attention has been paid to residential combustion sources. To fill the knowledge gap, a series of surveys were carried out to investigate the residential energy use in Beijing-Tianjin-Hebei (BTH) region during the period of 2013-2014. Study shows that the actual average amount of residential coal consumption is over 0.7tyr-1 per capita in 2013, which is much higher than that of 0.15tyr-1 per capita reported in the 2014 China Energy Statistical Yearbook (CESY). Combining the investigated activities data with the best available emission factors (EFs), bottom-up method was used to evaluate the potential air pollutant emissions from residential coal combustion in BTH region in 2013. The results indicate that Baoding is the top contributor to the whole BTH region and accounts for approximately 15% of the regional residential emissions in 2013. The spatial pattern of air pollutants shows that high emissions locate in the southeast, along the Yanshan and Taihang Mountains, where much more rural people live and coal combustion is prevalent in winter. The future emission scenario at the end of the 13th Five Year Plan (in 2020) was also predicted based on the policy guidance for the residential coal consumptions in the BTH region. The scenario analysis indicates that air pollutant emissions will drop substantially around 90% because more strict rules will be made for reducing the residential coal consumption. With combined survey information and statistical data, the uncertainty of the emission inventory which was established in this study for the residential sector in the BTH region is reduced and the emission inventory is more reliable for air quality decision making.

Effects of temperature parameters on thermal-optical analysis of organic and elemental carbon in aerosol

Thermal–optical analysis (TOA) is a popular method to determine aerosol elemental carbon (EC) and organic carbon (OC) collected on quartz fiber filter. However, temperature protocol adopted in TOA has great effects on OC and EC results. The purpose of this study is to investigate and quantify the effects of maximum temperature (Tmax) and residence time (RT) for each step in helium stage on ECOC measurements. Fourteen typical source samples and 20 ambient samples were collected and six temperature programs were designed for this study. It was found that EC value decreases regularly as Tmax ascends, i.e., EC results from Tmax of 650°C, 750°C and 850°C are 0.89 ± 0.06, 0.76 ± 0.10, 0.62 ± 0.13 times EC value from Tmax of 550°C, respectively, and the magnitude of EC drop (ECd, percent) is significantly correlated with OC abundance in total carbon (ROC/TC), expressed as ECd = 66.8ROC/TC − 14.4 (r = 0.87); pyrolized OC (POC) values are also sensitive to Tmax, but there are various trends for samples with different OC constituents. On average of the samples studied here, prolonged RT reduces EC values by only 3%, almost negligible compared to the effect of Tmax, and reduces POC by 9%, much less than that by previous report.

Assessment of the Evolution of Nitrate Deposition Using Remote Sensing Data Over the Yangtze River Delta, China

Along with the increasing concentration of nitrogenous pollutants emitted from the combustion and fertilizers, atmospheric nitrogen (N) deposition has become a great concern due to its significant ecological effect, especially in severe N emission regions such as the Yangtze River Delta (YRD) in east China. The spatial and temporal nitrate deposition fluxes were conducted using satellite data in YRD from 1996 to 2011. Our study reveals significant spatial variations of nitrate deposition in YRD region. In general, the fluxes of total (dry plus wet) nitrate deposition in YRD were up to 22.03 kg·N·ha-1·yr-1 with large loading received in winter. Most high fluxes appeared over urban (37.72 kg·N·ha-1·yr-1) and cropland (30.29 kg·N·ha-1·yr-1) areas. During the study period (1996-2011), a significant increasing trend of nitrate deposition was clearly observed in YRD with an annual rate of 1.33 kg·N·ha-1·yr-1. The spatial patterns of estimated nitrate deposition also showed that there were much higher fluxes and annual increasing trend in the middle region of YRD, i.e., the metropolitan areas contained Shanghai-Nanjing-Hangzhou cities, than in other areas. Our results also reveal that dry nitrate deposition contributed more than 50% of the total nitrate deposition over all provinces and land covers except coastal sea (14.27%), which indicates the relative importance of dry deposition to the total nitrate deposition in the YRD region. Therefore, it is necessary to consider both dry and wet deposition when evaluating the influences of nitrate deposition on environment and ecosystem health.