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1.
Chemosphere ; 255: 126907, 2020 Apr 30.
Artigo em Inglês | MEDLINE | ID: mdl-32387906

RESUMO

The downward transport of ozone (O3) stemming from the stratosphere-to-troposphere exchange (STE) can be a significant contributor to background O3. Such enhancement of background O3 may also influence ground-level PM2.5, particularly in polluted regions which have abundant precursor emissions. In this study, we quantified the STE impact on tropospheric O3 and its subsequent influence on surface PM2.5 across the northern hemisphere. The sensitivity analyses was conducted by using a comprehensive hemispheric atmospheric modeling system. Results suggest the surface PM2.5 concentration can be considerably enhanced by the STE in polluted regions including East China, East US, and Europe, mostly in winter and spring. In winter, the PM2.5 concentrations in East China, East US, and Europe are estimated to be enhanced by 1.3%, 3.5% and 5.5% due to the STE. The STE-enhanced PM2.5 concentrations are typically higher on high pollution days suggesting likely increasing contributions in regions with the growing pollution levels. During the heavy polluted days, the PM2.5 concentrations in East China can be enhanced by 2.289 µg/m3 in winter and 2.034 µg/m3 in spring due to the STE. The STE-enhanced PM2.5 also exhibits strong diurnal variations following a pattern similar to the total PM2.5 concentration, with high increasing ratio in the morning and low at afternoon, suggesting that the enhancement is most pronounced during peak pollution events. The STE-enhanced PM2.5 is exclusively contributed by the increase of nitrate, ammonium, and secondary organic aerosol which in-turn are strongly influenced by the atmospheric oxidation capacity.

2.
Environ Sci Technol ; 2020 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-32379428

RESUMO

In this study, we investigated the emission characteristics of condensable particulate matter (CPM) and sulfur trioxide (SO3) simultaneously through ammonia-based/limestone-based wet flue gas desulfurization (WFGD) from four typical coal-fired power plants (CFPPs) by conducting field measurements. Stack emissions of filterable particulate matter (FPM) all meet the Chinese ultralow emission (ULE) standards, whereas CPM concentrations are prominent (even exceed 10 mg/Nm3 from two CFPPs). We find that NH4+ and Cl- increase markedly through the ammonia-based WFGD, and SO42- is generally the main ionic component, both in CPM and FPM. Notably, the occurrence of elemental Se in FPM and CPM is significantly affected by WFGD. Furthermore, the established chemical profiles in FPM and CPM show a distinct discrepancy. In CPM, the elemental S mainly exists as a sulfate, and the metallic elements of Na, K, Mg, and Ca mainly exist as ionic species. Our results may indicate that not all SO3 are included in CPM and they co-exist in stack plume. With the substantial reduction of sulfur dioxide (SO2), S distributed in SO3, CPM, and FPM becomes non-negligible. Finally, the emission factors of CPM and SO3 under typical ULE technical routes fall in the ranges of 74.33-167.83 and 48.76-86.30 g/(t of coal) accordingly.

3.
Sci Total Environ ; 721: 137700, 2020 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-32197281

RESUMO

SO2 concentration decreased rapidly in recent years in China due to the implementation of strict control policies by the government. Particulate sulfate (pSO42-) and gaseous H2SO4 (SA) are two major products of SO2 and they play important roles in the haze formation and new particle formation (NPF), respectively. We examined the change in pSO42- and SA concentrations in response to reduced SO2 concentration using long-term measurement data in Beijing. Simulations from the Community Multiscale Air Quality model with a 2-D Volatility Basis Set (CMAQ/2D-VBS) were used for comparison. From 2013 to 2018, SO2 concentration in Beijing decreased by ~81% (from 9.1 ppb to 1.7 ppb). pSO42- concentration in submicrometer particles decreased by ~60% from 2012-2013 (monthly average of ~10 µg·m-3) to 2018-2019 (monthly average of ~4 µg·m-3). Accordingly, the fraction of pSO42- in these particles decreased from 20-30% to <10%. Increased sulfur oxidation ratio was observed both in the measurements and the CMAQ/2D-VBS simulations. Despite the reduction in SO2 concentration, there was no obvious decrease in SA concentration based on data from several measuring periods from 2008 to 2019. This was supported by the increased SA:SO2 ratio with reduced SO2 concentration and condensation sink. NPF frequency in Beijing between 2004 and 2019 remains relatively constant. This constant NPF frequency is consistent with the relatively stable SA concentration in Beijing, while different from some other cities where NPF frequency was reported to decrease with decreased SO2 concentrations.

4.
Environ Res ; 184: 109368, 2020 May.
Artigo em Inglês | MEDLINE | ID: mdl-32192990

RESUMO

Large areas of mainland China have been suffering frequently from heavy haze pollution during the past years, which feature high concentrations of fine particulate matter (PM2.5, particulate matters with aerodynamic diameters less than 2.5 µm) and low visibility. Moreover, these areas manifested strong regional complex pollution characteristics, particularly in North China including Beijing and the five surrounding provinces (BSFP). In this study, by using the localized comprehensive emission inventory of BSFP region in 2012 as an input, the Comprehensive Air Quality Model with Extensions-Particulate Matter Source Apportionment Technology (CAMx/PSAT) was used to assess the seasonal variations and source apportionment of PM2.5 in the highly polluted BSFP region, with a specific focus on the sectoral and sub-regional contributions to PM2.5 in Beijing during winter and summer. Results showed that the PM2.5 concentrations of BSFP region was higher in winter than that in summer. And the heavily polluted area in BSFP region shrinked noticeably in summer, compared with winter. As for source apportionment of PM2.5, residential and remaining industrial sectors constituted the top two sources of PM2.5 mass concentrations in Beijing. In addition, agricultural source represented a major contributor to ammonium, whereas transportation and power sectors constituted major sources to nitrates. In terms of contributions from sub-regions, the local sources ranked as the dominant contributors to PM2.5 in Beijing, while the main external contributions originated from the surrounding areas, such as Hebei and Shandong. Results of daily source apportionment to PM2.5 in Beijing showed that sub-regional long-distance transport became stronger when haze pollution was severe, in which contribution from remaining industrial sector would be higher than that of other periods. The results will allow for an improved understanding of the causes and origins of heavy regional PM2.5 pollution, and thus will benefit the development of effective joint control policies and identification of key polluting emission categories in North China and ultimately serve as references for other highly polluted megacities in the world.

5.
Environ Sci Technol ; 54(5): 2772-2779, 2020 03 03.
Artigo em Inglês | MEDLINE | ID: mdl-32048839

RESUMO

Comprehensive mercury (Hg) budgets were constructed in two typical subtropical forests in southern China in 2014 to quantify Hg (gaseous elemental Hg, Hg0, and reactive Hg, HgII) input and output fluxes and Hg retention in forests, consequently exploring the roles of subtropical forests in the global Hg cycle. At site Qianyanzhou, representing a background region with an enhanced atmospheric Hg0 concentration, the total HgII deposition (67.7 µg·m-2·year-1, 73% as dry HgII deposition) was found to be slightly higher than the Hg0 emission above the canopy (58.5 µg·m-2·year-1), indicating that the forest is a minor Hg sink but a significant net Hg0 source on a yearly basis. In contrast, the forest in the moderately polluted region (site Huitong) acted as a significant Hg sink but a minor net Hg0 source with a higher HgII deposition (73.7 µg·m-2·year-1) and relatively negligible Hg0 emission (2.65 µg·m-2·year-1). The decreasing atmospheric Hg0 concentrations declined the total Hg sink based on the Hg budgets synthesized of this and previous studies and may promote forest Hg0 emissions. Consequently, it was expected that the re-emission of historically deposited Hg may be enhanced from subtropical forests by recent decreases in atmospheric Hg0 concentrations throughout China.


Assuntos
Poluentes Atmosféricos , Mercúrio , China , Monitoramento Ambiental , Florestas
6.
Environ Pollut ; 259: 113918, 2020 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-32023794

RESUMO

Natural sources, such as soil and wind-erosion dust (SWD), biomass open burning (BOB), sea salt spray (SSAS) and biogenic source (BIO), are major contributors to atmospheric emissions of trace elements (TEs) globally. In this study, we used a comprehensive approach to account for area-, production- and biofuel consumption-based emission factor calculation methods, and thus developed an integrated high-resolution emission inventory for 15 types of TEs (As, B, Cd, Co, Cr, Cu, Hg, Mn, Mo, Ni, Pb, Sb, Se, V and Zn) originated from natural sources in China for the year 2015. The results show that national emissions of TEs in 2015 range from 7.45 tons (Hg) to 1, 400 tons (Zn) except for the extremely high emissions of Mn (10, 677 tons). SWD and BIO are identified as the top two source contributors, accounting for approximately 67.7% and 26.1% of the total emissions, respectively. Absolute emissions of TEs from natural sources are high in the Xinjiang, Inner Mongolia and Tibet autonomous regions with large areas of bare soil and desert. However, emission intensity of TEs per unit area in the Southern provinces of China is higher than those in Northern China and Southwestern China, with the Yunnan and Sichuan provinces displaying the highest emission intensity. Our results suggest that controlling SWD can play a significant role in reducing fugitive particulate matter and the associated emissions of TEs from natural sources in China; and desertification control is particularly critical in the Northwest provinces where the majority of deserts are located.

7.
J Environ Manage ; 260: 110069, 2020 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-32090813

RESUMO

Understanding the air pollution emission abatement potential and associated control cost is a prerequisite to design cost efficient control policies. In this study, a linear programming algorithm model, International Control Cost Estimate Tool, was updated with cost data for applications of 56 types of end-of-pipe technologies and five types of renewable energy in 10 major sectors namely power generation, industry combustion, cement production, iron and steel production, other industry processes, domestic combustion, transportation, solvent use, livestock rearing, and fertilizer use. The updated model was implemented to estimate the abatement potential and marginal cost of multiple pollutants in China. The total maximum abatement potentials of sulfur dioxide (SO2), nitrogen oxides (NOx), primary particulate matter (PM2.5), non-volatile organic compounds (NMVOCs), and ammonia (NH3) in China were estimated to be 19.2, 20.8, 9.1, 17.2 and 8.6 Mt, respectively, which accounted for 89.7%, 89.9%, 94.6%, 74.0%, and 80.2% of their total emissions in 2014, respectively. The associated control cost of such reductions was estimated as 92.5, 469.7, 75.7, 449.0, and 361.8 billion CNY in SO2, NOx, primary PM2.5, NMVOCs and NH3, respectively. Shandong, Jiangsu, Henan, Zhejiang, and Guangdong provinces exhibited large abatement potentials for all pollutants. Provincial disparity analysis shows that high GDP regions tend to have higher reduction potential and total abatement costs. End-of-pipe technologies tended be a cost-efficient way to control pollution in industries processes (i.e., cement plants, iron and steel plants, lime production, building ceramic production, glass and brick production), whereas such technologies were less cost-effective in fossil fuel-related sectors (i.e., power plants, industry combustion, domestic combustion, and transportation) compared with renewable energy. The abatement potentials and marginal abatement cost curves developed in this study can further be used as a crucial component in an integrated model to design optimized cost-efficient control policies.


Assuntos
Poluentes Atmosféricos , Poluição do Ar , China , Monitoramento Ambiental , Material Particulado , Dióxido de Enxofre
8.
Sci Total Environ ; 715: 136992, 2020 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-32023515

RESUMO

When addressing particulate matter (PM) emissions from residential solid fuel combustion, ultrafine particles are usually merged into PM2.5, while whose mass concentration is applied as the index in evaluating PM pollution as well as assessing PM-induced health risk. This may not effectively represent the risk from ultrafine particles. In this study, we explored ultrafine particle emissions during residential combustion under both laboratory-controlled and real-world rural household conditions. Significant ultrafine particle emissions (i.e. with emission factors between 2 × 1015 to 2 × 1016 particles per kg of fuel) are found for both coal and biomass. High emissions of particle mass concentration often occur at the beginning of the combustion (i.e. the first 30 min after fire start) while high emissions of particle number concentration occur in a later combustion period (60-150 min). Ultrafine particles account for over 90% of the emitted total particle number concentration from 3 nm to 10 µm. These emissions elevate ultrafine particle number concentration by more than a decade in indoor environment under which household residents are directly exposed. In addition, we show that there is notable inconsistency between reducing PM2.5 mass based emissions and reducing ultrafine particle number based emissions among various control strategies that were proposed for reducing pollution from residential combustion. Both "cleaner" fuels and stoves that are designed to reduce PM2.5 emissions are found to be not necessarily effective in reducing ultrafine particle emissions, even increase their emissions in some cases. These findings indicate that the overlook of ultrafine particle emissions from residential solid fuel combustion can lead to potential health risk to household residents, especially to those vulnerable ones (e.g., the elderly and children) who are more sensitive to indoor air pollution. More attentions are needed on ultrafine particle pollution and its potential health risk in comparison to using the PM mass concentration index alone.

9.
Environ Sci Technol ; 54(3): 1363-1371, 2020 02 04.
Artigo em Inglês | MEDLINE | ID: mdl-31904230

RESUMO

The dry impinger method, the indirect dilution method, and the direct dilution method can be used to measure the condensable particulate matter (CPM) emissions. We tested these methods in determining the CPM emissions from typical stationary sources in China and found that the CPM concentrations measured by the dry impinger method are much higher than those measured by the two dilution methods regardless of the type of stationary source. The soluble gases (e.g., SO2, HCl, and NH3) partially absorbed by the impinger solutions are the main reason for the overestimation of the CPM concentrations. This is supported by detecting more water-soluble ions (e.g., SO42-, Cl-, and NH4+) from the CPM collected using the dry impinger method. The positive biases of the CPM concentration and its water-soluble ions collected by the dry impinger method are larger under the conditions with high concentrations of soluble gases such as at the flue gas desulfurization inlet in coal-fired power plants. Comparing to the direct dilution method, the indirect dilution method can better capture the rapid dilution, cooling, and condensation of condensable gas precursors in the presence of filterable particulate matter and is recommended as the appropriate method for the CPM measurement in stationary sources.


Assuntos
Poluentes Atmosféricos , Material Particulado , China , Carvão Mineral , Monitoramento Ambiental , Íons , Centrais Elétricas
10.
Environ Pollut ; 259: 113886, 2020 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-31918144

RESUMO

The ultralow emission (ULE) retrofits for Chinese coal-fired power plants (CFPPs) are nearing completion. Large-scale and rapid retrofits have resulted in significant changes in the emission level and characteristics of particulate matter (PM). To investigate the variation characteristics of final three size fractions PM (PM2.5, PM10-2.5, PM>10) emissions, we conducted field tests at the outlets of wet flue gas desulfurization (WFGD) and wet electrostatic precipitator (WESP) by a pair of two-stage virtual impactors in eight representative ULE CFPPs. Our results indicate that, after WESP installations, the mass concentrations of final PM are significantly reduced and those of the final total ions and elements decrease as most individual chemical compositions are reduced. WESP presents an excellent removal performance for large particle sizes and high PM concentrations. SO42- is the major ionic component at both the outlets of WFGD and WESP, and its proportion in total ions is reduced to some extent through WESP. Furthermore, the average mass contents of SO42- and most elements in PM2.5 are significantly lower than those in PM10-2.5 and PM>10 whether at the WFGD-outlets or WESP-outlets. By comparison, chemical profiles of PM have substantially changed after ULE retrofits, and those after WFGD (e.g., sulfate, Zn, Pb, and Cu) have also changed relative to existing data. The end-tail emission factors (EFs) of PM2.5, PM10, and PMtotal under the typical ULE technical routes of WESP are calculated in time, and the corresponding EFs are in the range of 2.82-8.97, 15.7-27.6, and 38.6-61.7 g t-1, respectively. We believe the latest detailed PM EFs and the associated chemical profiles provided in this study are more representative of the current emission situations of Chinese CFPPs.


Assuntos
Poluentes Atmosféricos , Monitoramento Ambiental , Material Particulado , Centrais Elétricas , Poluentes Atmosféricos/química , China , Carvão Mineral , Tamanho da Partícula , Material Particulado/química
11.
Sci Total Environ ; 706: 135735, 2020 Mar 01.
Artigo em Inglês | MEDLINE | ID: mdl-31806313

RESUMO

Chinese coal-fired power plants (CFPPs) are experiencing large-scale and rapid retrofitting of ultralow emission (ULE), causing significant changes in emission level of particulate matter (PM) from CFPPs. In this study, based on coal ash mass balance over the whole process, an integrated emission factors (EFs) database of three size-fractioned particulate matters (PM2.5, PM10, and PMtotal) for CFPPs is constructed, which covers almost all typical ULE technical routes installed in CFPPs. To verify the reliability of PM EFs established in this study, we compare those with related results based on field tests. Overall, the gaps in the EFs of PM2.5, PM10, and PMtotal obtained by the two methods are not outrageous within a reasonable range. By combined with the refined size-fractioned PM EFs and unit-based activity level database, a detailed high-resolution emission inventory of PM2.5, PM10, and PMtotal from Chinese CFPPs in 2017 is established, with the corresponding total emissions of 143, 207, and 267 kt, respectively. Our estimation of PMtotal emission is comparable to the official statistics announced by China Electricity Council (CEC), which further demonstrates the reliability of PM EFs constructed in this study. Moreover, potential reductions of PM from CFPPs at two stages before and after 2017 are assessed under three application scenarios of major ULE technical routes. We forecast the final annual emissions of PM2.5, PM10, and PMtotal until 2020 will be reduced further, which fall within the range of 86-111 kt, 120-157 kt, and 142-184 kt, respectively, if all CFPPs achieve ULE requirements under the three scenarios. We believe our integrated database of PM EFs of CFPPs has good universality, and the forecast results will be helpful for policy guidance of ULE technologies, emissions inventory compilation, and regional air quality simulation and management.

12.
Environ Int ; 134: 105323, 2020 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-31759275

RESUMO

Long-range transport of air pollutants may cause significant health impacts in the receptor regions. In this study, we calculated the transboundary health impact from different foreign regions using a state-of-the-art air quality model at hemispheric scale. Our results reveal that transboundary PM2.5 pollution from outside China was of great significance, causing 100 thousand (95% CI, 45 thousand-200 thousand) premature deaths in China in 2015, which accounted for 9.60% PM2.5 related premature death in China. The impact of transboundary pollution in China was most significant in winter, in which the average PM2.5 concentration increased by 3.7 µg/m3, and was least significant in summer, with the average PM2.5 concentration increasing by 0.5 µg/m3. Liaoning and Yunnan provinces were extremely susceptible to transboundary pollution, whose annual average PM2.5 concentrations were increased by 10.2 and 11.4 µg/m3 respectively. Among all foreign regions, the impact from South Asia was most significant, causing 30 thousand (95% CI, 12 thousand-62 thousand) premature deaths annually in China. This study only reveals the transboundary impact under the integrated exposure-response (IER) model and fixed meteorology field in 2015. Further studies are needed to investigate how different exposure-response functions and meteorology affect the transboundary PM2.5 pollution and its related death.

13.
Huan Jing Ke Xue ; 40(12): 5234-5239, 2019 Dec 08.
Artigo em Chinês | MEDLINE | ID: mdl-31854593

RESUMO

With the retrofitting of coal-fired power plants and steel plants for ultra-low-emission control, the concentration of filterable particles (FPM) from these sources is decreasing gradually. The condensable particle matter (CPM) draws more attention. The understanding of CPM emission concentration and chemical characteristics is still limited. There has been no standard determination method of CPM in China until now. In this study, three methods, including the dry impinger method (US EPA method 202), indirect dilution method, and direct dilution method, are discussed and compared in measuring CPM emissions from coal-fired power plants, coke-making plants and sintering plants. The results show that method 202 overestimates the emissions of CPM, due to the fact that the gaseous HCl or SO2 dissolves into condensable liquid and cannot be completely eliminated by N2 purging after sampling. Instead, CPM measured using the indirect dilution method better represents its real emission levels into the atmosphere.

14.
Environ Sci Technol ; 2019 Dec 13.
Artigo em Inglês | MEDLINE | ID: mdl-31773945

RESUMO

To investigate the up-to-date migration and emission characteristics of NH3/NH4+ in coal-fired power plants (CFPPs) after implementing ultralow emission retrofitting, typical air pollution control devices (APCDs) in CFPPs, including flue gas denitrification, dust collectors, combined wet flue gas desulfurization (WFGD), and wet precipitators are involved in field measurements. The results show that most of the excessive injected and/or unreacted ammonia from the flue gas denitrification system, whether selective catalytic reduction (SCR) or selective noncatalytic reduction (SNCR), is converted into particle-bound NH4+ (>91%), and the rest (less than 9%) is carried by flue gas in the form of gaseous NH3, with a concentration value of 0.15-0.54 mg/(N m3) at the denitrification outlet. When passing through dust collectors, particle-bound NH4+ concentration decreases substantially along with the removal of particle matter. In WFGD, the dissolution and volatilization effects affect the gaseous ammonia concentration, which decreases when using limestone slurry and a 20% solution of ammonia as a desulfurization agent, while liquid ammonia solution with a high concentration (99.8%) may cause the flue gas NH3 concentration to increase considerably by 13 times. Particle-bound NH4+ concentration is mainly influenced by the relative strength of desulfurization slurry scouring and flue gas carrying effects and increases 2.84-116 times through ammonia-based WFGD. Furthermore, emission factors of NH3 for combinations of APCDs are discussed.

15.
Proc Natl Acad Sci U S A ; 116(49): 24463-24469, 2019 Dec 03.
Artigo em Inglês | MEDLINE | ID: mdl-31740599

RESUMO

From 2013 to 2017, with the implementation of the toughest-ever clean air policy in China, significant declines in fine particle (PM2.5) concentrations occurred nationwide. Here we estimate the drivers of the improved PM2.5 air quality and the associated health benefits in China from 2013 to 2017 based on a measure-specific integrated evaluation approach, which combines a bottom-up emission inventory, a chemical transport model, and epidemiological exposure-response functions. The estimated national population-weighted annual mean PM2.5 concentrations decreased from 61.8 (95%CI: 53.3-70.0) to 42.0 µg/m3 (95% CI: 35.7-48.6) in 5 y, with dominant contributions from anthropogenic emission abatements. Although interannual meteorological variations could significantly alter PM2.5 concentrations, the corresponding effects on the 5-y trends were relatively small. The measure-by-measure evaluation indicated that strengthening industrial emission standards (power plants and emission-intensive industrial sectors), upgrades on industrial boilers, phasing out outdated industrial capacities, and promoting clean fuels in the residential sector were major effective measures in reducing PM2.5 pollution and health burdens. These measures were estimated to contribute to 6.6- (95% CI: 5.9-7.1), 4.4- (95% CI: 3.8-4.9), 2.8- (95% CI: 2.5-3.0), and 2.2- (95% CI: 2.0-2.5) µg/m3 declines in the national PM2.5 concentration in 2017, respectively, and further reduced PM2.5-attributable excess deaths by 0.37 million (95% CI: 0.35-0.39), or 92% of the total avoided deaths. Our study confirms the effectiveness of China's recent clean air actions, and the measure-by-measure evaluation provides insights into future clean air policy making in China and in other developing and polluting countries.

16.
Environ Sci Technol ; 53(18): 11013-11022, 2019 Sep 17.
Artigo em Inglês | MEDLINE | ID: mdl-31415163

RESUMO

Mass adoption of electric vehicles (EVs) is widely viewed as essential to address climate change and requires a compelling case for ownership worldwide. While the manufacturing costs and technical capabilities of EVs are similar across regions, customer needs and economic contexts vary widely. Assessments of the all-electric-range required to cover day-to-day driving demand, and the climate and economic benefits of EVs, need to account for differences in regional characteristics and individual travel patterns. To meet this need travel profiles for 1681 light-duty passenger vehicles in China, the U.S., and Germany were used to make the first consistent multiregional comparison of customer and greenhouse gas (GHG) emission benefits of EVs. We show that despite differences in fuel prices, driving patterns, and subsidies, the economic benefits/challenges of EVs are generally similar across regions. Individuals who are economically most likely to adopt EVs have GHG benefits that are substantially greater than for average drivers. Such "priority" EV customers have large (32%-63%) reductions in cradle-to-grave GHG emissions. It is shown that low battery costs (below approximately $100/kWh) and a portfolio of EV offerings are required for mass adoption of electric vehicles.


Assuntos
Gasolina , Emissões de Veículos , China , Alemanha , Efeito Estufa , Humanos , Veículos Automotores , Estados Unidos
17.
Sci Total Environ ; 693: 133580, 2019 Nov 25.
Artigo em Inglês | MEDLINE | ID: mdl-31376754

RESUMO

Heterogeneous reactions of N2O5, O3, OH, ClONO2, HOCl, ClNO2, and NO2, with chlorine-containing particles are incorporated in the Community Multiscale Air Quality (CMAQ) model to evaluate the impact of heterogeneous reactions of reactive chlorine species on ozone and free radicals. Changes of summertime ozone and free radical concentrations due to the additional heterogeneous reactions in north China were quantified. These heterogeneous reactions increased the O3, OH, HO2 and RO2 concentrations by up to 20%, 28%, 36% and 48% for some regions in the Beijing-Tianjin-Hebei (BTH) area. These areas typically have a larger amount of NOx emissions and a lower VOC/NOx ratio. The zero-out method evaluates that the photolysis of ClNO2 and Cl2 are the major contributors (42.4% and 57.6%, respectively) to atmospheric Cl in the early morning hours but the photolysis of Cl2 is the only significant contributor after 10:00 am. The results highlight that heterogeneous reactions of reactive chlorine species are important to atmospheric ozone and free-radical formation. Our study also suggests that the on-going NOx emission controls in the NCP region with a goal to reduce both O3 and secondary nitrate can also have the co-benefit of reducing the formation Cl from ClNO2 and Cl2, which may also lead to lower secondary organic aerosol formation and thus the control of summertime PM2.5 in the region.

18.
Sci Total Environ ; 689: 1293-1303, 2019 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-31466166

RESUMO

Water-soluble inorganic ions (WSI), a major component of PM2.5, often increased rapidly during the haze event in Beijing. Sulfate (SO42-), Nitrate (NO3-), and Ammonium (NH4+) are three main components of WSI. Since year 2015, sulfate concentrations in PM2.5 has gradually decreased owing to the effective control of SO2 emissions. However, the contribution of nitrate to PM2.5 has significantly increased during haze events in Beijing at the same time. In this study, a highly time-resolved online analyzer (Monitor for Aerosols and Gases, MARGA) was employed to measure the WSI in PM2.5 in Beijing from 5 February to 15 November 2017. Three typical haze events during this sampling period were investigated. During heavy pollution episodes in winter, nitrate concentrations increased from 7.5 µg/m3 to 45.6 µg/m3 (45.0% of WSI), while sulfate increased from 4.2 µg/m3 to 20.1 µg/m3 (19.8% of WSI). This indicated that nitrate is more important than sulfate as a driver for the growth of PM2.5 during the period of heavy air pollution in winter. Nitrate also dominates the increase of WSI in the pollution episodes in autumn, with an average concentration of 52.5 µg/m3, and contributed up to 67% of WSI. The average concentration ratio of NH4+ to SO42- was higher in autumn (1.02) than that in summer (0.74) and close to that in winter (1.00). This is mainly because the emission control of coal combustion in Beijing and surrounding areas results in an NH3-rich and SO2-lean atmosphere, which promoted the formation of ammonium nitrate. Our study indicates that nitrate has become the most important component of WSI in PM2.5 and is driving the rapid growth of PM2.5 concentrations during heavy pollution episodes in Beijing. Therefore, more efforts shall be made to reduce the nitrogen oxide and ammonia emissions in Beijing and surrounding areas.

19.
Environ Sci Technol ; 53(15): 9269-9278, 2019 Aug 06.
Artigo em Inglês | MEDLINE | ID: mdl-31288521

RESUMO

Coal combustion in low-efficiency household stoves results in the emission of large amounts of nonmethane organic compounds (NMOCs), including intermediate-volatility compounds (IVOCs) and semivolatile organic compounds (SVOCs). This conceptual picture is reasonably well established, however, quantitative assessment of I/SVOC emissions from household stoves is rare. We used a proton-transfer-reaction time-of-flight mass spectrometer (PTR-ToF-MS) to quantify the emissions of organic gases from a typical Chinese household coal stove operated with anthracite and bituminous coals. Most NMOCs (approximately 64-88%) were dominated by hydrocarbons and emitted during the ignition and flaming phases. The ratio of oxidized hydrocarbons increased during the flaming and smoldering stages due to the elevated combustion efficiency. The average emission factors of NMOCs were 121 ± 25.7 and 3690 ± 930 mg/kg for anthracite and bituminous coals, respectively. I/SVOCs contributed to approximately 30% of the total emitted NMOC mass during bituminous coal combustion, much higher than the contribution of biomass burning (approximately 1.5%). Furthermore, I/SVOCs may contribute over 70% of the secondary organic aerosol (SOA) mass formed from gaseous organic species emitted as a result of bituminous coal combustion. This study highlights the importance of inventorying coal-originated I/SVOCs when conducting SOA formation simulation studies.


Assuntos
Poluentes Atmosféricos , Carvão Mineral , China , Compostos Orgânicos , Volatilização
20.
J Environ Manage ; 245: 95-104, 2019 Sep 01.
Artigo em Inglês | MEDLINE | ID: mdl-31150914

RESUMO

Control strategies can be optimized to attain air quality standards at minimal cost through selecting optimal combinations of controls on various pollutants and regional sources. In this study, we developed a module for least-cost control strategy optimization based on a real-time prediction system of the responses of pollution concentrations to emissions changes and marginal cost curves of pollutant controls. Different from other method, in this study the relationship between pollution concentrations to and precursor emissions was derived from multiple air quality simulations in which the nonlinear interactions among different precursor emissions can be well addressed. Hypothetical control pathways were designed to attain certain air quality goals for particulate matter (PM2.5) and ozone (O3) in the Beijing-Tianjin-Hebei region under the 2014 baseline emission level. Results suggest that reducing local primary PM emissions was the most cost-efficient method to attain the ambient PM2.5 standard, whereas for O3 attainment, reducing regional emission sources of gaseous pollutants (i.e., SO2, NOx, and volatile organic compounds (VOCs)) exhibited greater effectiveness. NH3 controls may be cost-efficient in achieving strengthened PM2.5 targets; however, they might not help in reducing O3. To achieve both PM2.5 (<35 µg m-3) and O3 (daily 1-h maxima concentration < 100 ppb) targets in Beijing, the reduced rates in BTH regions of NOx, SO2, NH3, VOCs and primary PM are 75%, 75%, 5%, 55%, and 85%, respectively from the emission levels in the year of 2014. Local reduction is the most effective method of attaining moderate PM2.5 and O3 targets; however, to achieve more aggressive air quality goals, the same level of reductions must be conducted across the whole Beijing-Tianjin-Hebei region.


Assuntos
Poluentes Atmosféricos , Poluição do Ar , Pequim , China , Controle de Custos , Monitoramento Ambiental , Material Particulado
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