Search

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.

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 coal's burning forms and the stove's 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, China's 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.

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 (T(max)) 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 T(max ) ascends, i.e., EC results from T(max) of 650 degrees C, 750 degrees C and 850 degrees C are 0.89 +/- 0.06, 0.76 +/- 0.10, 0.62 +/- 0.13 times EC value from T( max) of 550 degrees C, respectively, and the magnitude of EC drop (EC(d), percent) is significantly correlated with OC abundance in total carbon (R(OC/TC)), expressed as EC(d) = 66.8R(OC/TC)-14.4 (r = 0.87); pyrolized OC(POC) values are also sensitive to T(max), 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 T(max), and reduces POC by 9%, much less than that by previous report.

China is thought to be the most important contributor to the global burden of carbonaceous aerosols, and residential coal combustion is the greatest emission source of black carbon (BC). In the present study, two high-efficiency household coal-stoves are tested together with honeycomb-coal-briquettes and raw-coal-chunks of nine different coals. Coal-burning emissions are collected onto quartz fiber filters (QFFs) and analyzed by a thermal-optical transmittance (TOT) method. Emission factors (EFs) of particulate matter (PM), organic carbon (OC), and elemental carbon (EC) are systematically measured, and the average EFs are calculated by taking into account our previous data. For bituminous coal-briquette and -chunk, EFs of PM, OC, and EC are 7.33, 4.16, and 0.08 g/kg and 14.8, 5.93, and 3.81 g/kg, respectively; and for anthracite-briquette and -chunk, they are 1.21, 0.06, and 0.004 g/kg and 1.08, 0.10, and 0.007 g/kg, respectively. Annual estimates for PM, OC, and EC emissions in China are calculated for the years of 2000 and 2005 according to the EFs and coal consumptions, and the results are consistent with our previous estimates. Bituminous coal-chunk contributes 68% and 99% of the total OC and EC emissions from household coal burning, respectively. Additionally, a new model of Aethalometer (AE90) is introduced into the sampling system to monitor the real-time BC concentrations. On one hand, AE90 provides a set of EFs for optical BC in parallel to thermal-optical EC, and these two data are generally comparable, although BC/EC ratios vary in different coal/stove combinations. On the other hand, AE90 offers a chance to observe the variation of BC concentrations during whole burning cycles, which demonstrates that almost all BC emits into the flue during the initial period of 15 min after coal addition into household stoves.

In recent years many households in northern China's rural areas tend to furnish their houses with water-circulating piping system for heating, which entails mini-boiler stoves to heat water via raw coal chunk or biomass pellets. In this study, consistent efforts were made to obtain first-hand emission factors of organic carbon (EF OC ) and elemental carbon (EF EC ) for residential solid fuel combustion. A total of 39 fuel/stove combinations, covering seven coals (with different geological maturities), eleven biomass fuels, and five different stoves, were tested. The mean EF OC and EF EC were (4.29 ± 2.33) and (4.43 ± 2.18) g/kg for residential coal combustion, (2.16 ± 4.47) and (0.42 ± 1.01) g/kg for indoor biomass burning. The EFs for tested coal combustion display a “bell shape” with the maximum EF value occurring at bitumite of middle maturity. Coal briquetting in this study led to a significant decrease in EF EC but a notable increase in EF OC , which contradicted with the result from some of previous studies that coal briquetting always leads to relatively low emissions of both OC and EC. The inside reason deserves further clarification. Averaging over the two mini-boiler stoves shows that the introduction of mini-boiler stoves can reduce 5% and 10% of OC from anthracite and bitumite, respectively, and 47% and 53% of EC from anthracite and bitumite, respectively, suggesting that transfer from pure heating stoves to mini-boiler stoves seems unlikely to increase carbonaceous particle emissions, particularly EC. The more significant decline in EF EC than in EF OC indicates that the access to mini-boiler stove for winter heating is very likely to be both a clean air measure and a warming mitigation approach. Updated emission inventories in China for the year of 2014 showed that the OC and EC emissions were 338 Gg and 529 Gg, respectively, from residential coal combustion, and 557 Gg and 79 Gg, respectively, from household biomass burning. [ABSTRACT FROM AUTHOR]

Abstract: Shanghai is the largest industrial and commercial city in China, and its air quality has been deteriorating for several decades. However, there are scarce researches on the level and seasonal variation of fine particle (PM2.5) as well as the carbonaceous fractions when compared with other cities in China and around the world. In the present paper, abundance and seasonal characteristics of PM2.5, organic carbon (OC) and elemental carbon (EC) were studied at urban and suburban sites in Shanghai during four season-representative months in 2005–2006 year. PM2.5 samples were collected with high-vol samplers and analyzed for OC and EC using thermal-optical transmittance (TOT) protocol. Results showed that the annual average PM2.5 concentrations were 90.3–95.5 μg/m3 at both sites, while OC and EC were 14.7–17.4 μg/m3 and 2.8–3.0 μg/m3, respectively, with the OC/EC ratios of 5.0–5.6. The carbonaceous levels ranked by the order of Beijing > Guangzhou > Shanghai > Hong Kong. The carbonaceous aerosol accounted for ∼30% of the PM2.5 mass. On seasonal average, the highest OC and EC levels occurred during fall, and they were higher than the values in summer by a factor of 2. Strong correlations (r =0.79–0.93) between OC and EC were found in the four seasons. Average level of secondary organic carbon (SOC) was 5.7–7.2 μg/m3, accounting for ∼30% of the total OC. Strong seasonal variation was observed for SOC with the highest value during fall, which was about two times the annual average. [Copyright &y& Elsevier]