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Nitrogen oxide (NOx) emissions from heavy-duty diesel vehicles (HDDVs) have adverse effects on human health and the environment. On-board monitoring (OBM), which can continuously collect vehicle performance and NOx emissions throughout the operation lifespan, is recognized as the core technology for future vehicle in-use compliance, but its large-scale application has not been reported. Here, we utilized OBM data from 22,520 HDDVs in China to evaluate their real-world NOx emissions. Our findings showed that China VI HDDVs had a 73% NOx emission reduction compared with China V vehicles, but a considerable proportion still faced a significant risk of higher NOx emissions than the corresponding limits. The unsatisfactory efficiency of the emission treatment system under disadvantageous driving conditions (e.g., low speed or ambient temperature) resulted in the incompliance of NOx emissions, especially for utility vehicles (sanitation/garbage trucks). Furthermore, the observed intertrip and seasonal variability of NOx emissions demonstrated the need for a long-term continuous monitoring protocol instead of instantaneous evaluation for the OBM. With both functions of emission monitoring and malfunction diagnostics, OBM has the potential to accurately verify the in-use compliance status of large-scale HDDVs and discern the responsibility of high-emitting activities from manufacturers, vehicle operators, and driving conditions.
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Contaminantes Atmosféricos , Monitoreo del Ambiente , Óxidos de Nitrógeno , Emisiones de Vehículos , Emisiones de Vehículos/análisis , Monitoreo del Ambiente/métodos , Óxidos de Nitrógeno/análisis , Contaminantes Atmosféricos/análisis , ChinaRESUMEN
Secondary organic aerosol (SOA) formation from gasoline vehicles spanning a wide range of emission types was investigated using an oxidation flow reactor (OFR) by conducting chassis dynamometer tests. Aided by advanced mass spectrometric techniques, SOA precursors, including volatile organic compounds (VOCs) and intermediate/semivolatile organic compounds (I/SVOCs), were comprehensively characterized. The reconstructed SOA produced from the speciated VOCs and I/SVOCs can explain 69% of the SOA measured downstream of an OFR upon 0.5-3 days' OH exposure. While VOCs can only explain 10% of total SOA production, the contribution from I/SVOCs is 59%, with oxygenated I/SVOCs (O-I/SVOCs) taking up 20% of that contribution. O-I/SVOCs (e.g., benzylic or aliphatic aldehydes and ketones), as an obscured source, account for 16% of total nonmethane organic gas (NMOG) emission. More importantly, with the improvement in emission standards, the NMOG is effectively mitigated by 35% from China 4 to China 6, which is predominantly attributed to the decrease of VOCs. Real-time measurements of different NMOG components as well as SOA production further reveal that the current emission control measures, such as advances in engine and three-way catalytic converter (TWC) techniques, are effective in reducing the "light" SOA precursors (i.e., single-ring aromatics) but not for the I/SVOC emissions. Our results also highlight greater effects of O-I/SVOCs to SOA formation than previously observed and the urgent need for further investigation into their origins, i.e., incomplete combustion, lubricating oil, etc., which requires improvements in real-time molecular-level characterization of I/SVOC molecules and in turn will benefit the future design of control measures.
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Aerosoles , Gasolina , Emisiones de Vehículos , Compuestos Orgánicos Volátiles , Contaminantes Atmosféricos/química , Compuestos Orgánicos/químicaRESUMEN
Motor vehicle ammonia (NH3) emissions have attracted increasing attention for their potential to form secondary aerosols in urban atmospheres. However, vehicle NH3 emission factors (EFs) remain largely unknown due to a lack of measurements. Thus, we conducted detailed measurements of NH3 emissions from 18 Euro 2 to Euro 5 light-duty gasoline vehicles (LDGVs) in Shanghai, China. The distance- and fuel-based NH3 EFs average 29.2 ± 24.1 mg·km-1 and 0.49 ± 0.41 g·kg-1, respectively. The average NH3-to-CO2 ratio is 0.41 ± 0.34 ppbv·ppmv-1. The measurements reveal that NH3 emissions from LDGVs are strongly correlated with both vehicle specific power (VSP) and the modified combustion efficiency (MCE); these relationships were used to predict LDGV NH3 EFs via a newly developed model. The predicted LDGV NH3 EFs under urban and highway driving cycles are 23.3 mg·km-1 and 84.5 mg·km-1, respectively, which are consistent with field measurements. The NH3 EF has decreased by 32% in average since the implementation of vehicle emission control policies in China five years ago. The model presented herein more accurately predicts LDGV NH3 emissions, contributing substantially to the compilation of NH3 emission inventories and prediction of future motor vehicle emissions in China.
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Contaminantes Atmosféricos , Gasolina , Amoníaco , China , Vehículos a Motor , Emisiones de VehículosRESUMEN
Intermediate volatility organic compound (IVOC) emissions from a large cargo vessel were characterized under real-world operating conditions using an on-board measurement system. Test ship fuel-based emission factors (EFs) of total IVOCs were determined for two fuel types and seven operating conditions. The average total IVOC EF was 1003 ± 581 mg·kg-fuel-1, approximately 0.76 and 0.29 times the EFs of primary organic aerosol (POA) emissions from low-sulfur fuel (LSF, 0.38 wt % S) and high-sulfur fuel (HSF, 1.12 wt % S), respectively. The average total IVOC EF from LSF was 2.4 times that from HSF. The average IVOC EF under low engine load (15%) was 0.5-1.6 times higher than those under 36%-74% loads. An unresolved complex mixture (UCM) contributed 86.1 ± 1.9% of the total IVOC emissions. Ship secondary organic aerosol (SOA) production was estimated to be 546.5 ± 284.1 mg·kg-fuel-1; IVOCs contributed 98.9 ± 0.9% of the produced SOA on average. Fuel type was the dominant determinant of ship IVOC emissions, IVOC volatility distributions, and SOA production. The ship emitted more IVOC mass, produced higher proportions of volatile organic components, and produced more SOA mass when fueled with LSF than when fueled with HSF. When reducing ship POA emissions, more attention should be paid to commensurate control of ship SOA formation potential.
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Contaminantes Atmosféricos , Emisiones de Vehículos , Aerosoles , Compuestos Orgánicos , Navíos , VolatilizaciónRESUMEN
Some in-use China IV and China V heavy-duty diesel vehicles (HDDVs) with selective catalytic reduction (SCR) systems probably fail to mitigate nitrogen oxide (NOX) emissions as expected. Meanwhile, these SCR-equipped HDDVs might emit excessive ammonia (NH3). To better understand the NOX and NH3 emissions from typical HDDVs in China, seventeen in-use vehicles with various emission-control technologies were tested by using laboratory chassis dynamometers. The results indicated that individual NOX and NH3 emissions from HDDV fleets widely varied owing to differences in aftertreatment performance. China V and VI HDDVs with effectively functioning SCRs could substantially control their NOX emissions to be below the corresponding emission limits (i.e., 4.0 and 0.69 g/kWh for China V and China VI vehicles, respectively) but with a potential risk of high NH3 emissions caused by diesel exhaust fluid (DEF) overdosing. Furthermore, higher vehicle speed and payload resulted in lower NOX emissions and possibly higher NH3 emissions from HDDVs with effectively functioning SCRs, while higher NOX emissions from tampered- and non-SCR HDDVs. NOX emissions from China VI HDDVs were more sensitive to cold starts compared to China V and earlier vehicles, but there was no significant discrepancy in NH3 emissions between cold- and hot-start tests.
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Gas-phase dimethylamine (DMA) has recently been identified as one of the most important vapors to initiate new particle formation (NPF), even in China's polluted atmosphere. Nevertheless, there remains a fundamental need for understanding the atmospheric life cycle of DMA, particularly in urban areas. Here we pioneered large-scale mobile observations of the DMA concentrations within cities and across two pan-region transects of north-to-south (â¼700 km) and west-to-east (â¼2000 km) in China. Unexpectedly, DMA concentrations (mean ± 1σ) in South China with scattered croplands (0.018 ± 0.010 ppbv, 1 ppbv=10-9 L/L) were over three times higher than those in the north with contiguous croplands (0.005 ± 0.001 ppbv), suggesting that nonagricultural activities may be an important source of DMA. Particularly in non-rural regions, incidental pulsed industrial emissions led to some of the highest DMA concentration levels in the world (>2.3 ppbv). Besides, in highly urbanized areas of Shanghai, supported by direct source-emission measurements, the spatial pattern of DMA was generally correlated with population (R2 = 0.31) due to associated residential emissions rather than vehicular emissions. Chemical transport simulations further show that in the most populated regions of Shanghai, residential DMA emissions can contribute for up to 78% of particle number concentrations. Shanghai is a case study for populous megacities, and the impacts of nonagricultural emissions on local DMA concentration and nucleation are likely similar for other major urban regions globally.
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Volatile organic compounds (VOCs) play important roles in the formation of ozone and fine particles in the troposphere. Industrial parks emit significant amounts of VOCs in China, while few studies have characterized them. In the present study, a mobile platform was employed to measure the levels and composition VOCs around industrial parks in the Yangzte River Delta region. The average concentration of VOCs ranged from 39 µg·m-3 (5% percentile) to 533 µg·m-3 (95% percentile) with an average of 183 µg·m-3, which was three times that of ambient concentrations. Maximum VOC concentrations ranged from 307 µg·m-3 (5% percentile) to 12006 µg·m-3 (95% percentile) with an average of 2812 µg·m-3. The frequency of abnormal peak values was as high as 64% across all the industrial parks, of which toluene (32%), xylene (18%), benzene (9%), and>C9 aromatics (19%) were the most common species. Differences in VOC characteristics were observed among the different types of industrial parks. Specifically, highest concentrations of VOCs were observed in textile industrial parks followed by chemical, painting, and petrochemical industrial parks, and VOC concentrations in electronics industrial parks were the lowest. Importantly, species measured using the mobile platform only contributed~50% of VOCs present in ambient samples, indicating that the concentrations of VOCs in the industrial parks were underestimated overall. These results can inform measures to control VOC pollution in industrial parks in China.
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Real-world vehicle emission factors (EFs) for the total intermediate volatile organic compounds (total-IVOCs) and volatile organic compounds (VOCs) from mixed fleets of vehicles were quantified in the Yangtze tunnel in Shanghai. Relationships of EFs of IVOCs with fleet compositions and vehicle speed as well as secondary organic formation potentials (SOAFPs) from IVOCs and VOCs were studied. Multiple linear regression (MLR) was used to estimate EFs of total-IVOCs for gasoline and diesel vehicles. IVOCs were classified into unresolved complex mixtures (unspeciated cyclic compounds and branched alkanes (b-alkanes)) and speciated targets (11 n-alkanes and ten polycyclic aromatic hydrocarbons (PAHs)). The results showed that the average EF of total-IVOCs was 24.9 ± 7.8 mg/(km·veh), which was comparable to that of VOCs. Unspeciated cyclic compounds and b-alkanes dominated the main composition (~77% and ~19%), followed by n-alkanes (~4%) and PAHs (~1%). EFs of IVOCs showed a significant, positive relationship with diesel vehicle fractions (p < 0.05). EFs of IVOCs dropped notably with the decrease of the diesel vehicle fractions. SOAFP produced by the total organic compounds (IVOCs + VOCs) was 8.9 ± 2.5 mg/(km·veh), in which up to 86% of SOAFP was from IVOCs. Estimated EFs of total-IVOCs for gasoline vehicles and diesel vehicles were 15.3 and 219.8 mg/(km·veh) respectively. Our results demonstrate that IVOCs emitted from diesel vehicles are the main emission sources under real world conditions and significant contributions of IVOCs emissions to SOA formation is evident, which indicates the necessity of making control policies to reduce IVOCs emissions from vehicles.
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The unintentional emission reductions caused by the COVID-19 pandemic provides an opportunity to investigate the impact of energy, industry, and transportation activities on air pollutants and CO2 emissions and their synergy. Here, we constructed an approach to estimate city-level high resolution dynamic emissions of both anthropogenic air pollutants and CO2 by introducing dynamic temporal allocation coefficients based on real-time multisource activity data. We first apply this approach to estimate the spatiotemporal evolution of sectoral emissions in eastern China, focusing on the period around the COVID-19 lockdown. Comparisons with observational data show that our approach can well capture the spatiotemporal changes of both short-lived precursors (NOx and NMVOCs) and CO2 emissions. Our results show that air pollutants (SO2, NOx, and NMVOCs) were reduced by up to 31%-53% during the lockdown period accompanied by simultaneous changes of 40% CO2 emissions. The declines in power and heavy industry sectors dominated regional SO2 and CO2 reductions. NOx reductions were mainly attributed to mobile sources, while NMVOCs emission reductions were mainly from light industry sectors. Our findings suggest that differentiated emission control strategies should be implemented for different source categories to achieve coordinated reduction goals.
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In typical cities of East China, more than 900 non-road vehicles were tested for exhaust smoke. Based on the investigation of the properties of these non-road vehicles, exhaust smoke intensities for different kinds of non-road vehicles are recommended. We also quantitatively study the differences in smoke intensity among vehicle age, vehicle power, test conditions, and fuels. The results showed that smoke intensity of non-road vehicles was (1.02±0.57) m-1 and that Ringelmann smoke was 2.10±0.19. In comparison to Chinese national standard (GB 36886), approximately 12%-25% of tested non-road vehicles' smoke intensity exceeded the standard limit. The smoke intensity of 80% of tested non-road vehicles was higher during start-up than under free acceleration. In comparison to ordinary diesel, the smoke intensities of tested non-road vehicles that used automotive diesel were lower. The instantaneous increase in fuel injection during start-up, as well as poor fuel quality, can directly affect the exhaust smoke of non-road vehicles.
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The latest China VI emission standard has introduced a remote monitoring rule for regulating in-use emissions of heavy-duty diesel vehicles (HDDVs). Real-time data regarding engine and aftertreatment operating conditions and tailpipe nitrogen oxides (NOx) concentrations are required to be collected through electronic control unit and on-board NOx sensors by vehicle original equipment manufacturers (OEMs), and then transmitted to environmental authorities. Beijing has developed a local standard that requires OEMs to design China VI-like on-board monitoring (OBM) systems for new China V HDDVs since September 2018. Additionally, Beijing has been a pioneer in retrofitting in-use China IV and China V HDDVs with OBM systems since 2017. This paper contains a timely technical and policy assessment for the state-of-the-art OBM programs in China with a focus on the recent progress in Beijing. Both OEM-performed and retrofitted OBM data were collected from a fleet of OBM-instrumented vehicles. First, our assessment shows high data integrity and quality of OEM-performed OBM systems. In contrast, a considerable fraction of HDDVs equipped with retrofitted OBM systems did not completely report NOx concentrations, intake mass air flow and other parameters. Next, eight OBM-instrumented HDDVs were tested on road by portable emissions measurement systems (PEMSs) to examine the reliability of sensor-based NOx concentrations. The majority (6 of 8) shows a good agreement between OBM and PEMS results with an average relative error of approximately -15%. Furthermore, calculation of NOx mass emissions, inter-trip variability, and alternative methods of enforcing in-use emissions management (e.g., to develop concentration metric-based emission limits) are discussed. This early-stage assessment suggests the OBM approach has the potential to play a central role in in-use emission inspections for HDDVs in China. The regulatory agency should focus more attention to the data integrity and the reliability of NOx sensors by developing effective verification processes.
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Particle size distribution and emission factors from 9 State 3-5 light-duty gasoline vehicles (LDGVs) and 15 State 3-5 heavy-duty diesel vehicles (HDDVs) were tested in this study using a constant volume sampling (CVS) system on a dynamometer. The influences of driving cycles and emission control level on the PM emission factors and particle size distribution were analyzed. The results show that the PM emission factors of the tested LDGVs and HDDVs were (4.1±4.0)×1014 and (5.7±4.3)×1015 kg-1, respectively; the HDDV PM emission factor was (14±7) times less than that of LDGVs. Regarding LDGVs, the PM emission factor under the extra high speed condition was much more than that of the other speed conditions at (5.1±5.0)×1013 km-1, 11.7, 14.1, and 7.3 times more than that under the low, medium, and high speed conditions, respectively. Regarding HDDVs, the emission factor under the high speed condition was 2.5 and 1.4 times that under the low and medium speed conditions, respectively, and was mostly of nuclei-mode particles. At the emission control level of State 3-5, the PM emission factors of LDGVs were (2.7±1.7)×1013, (2.6±1.3)×1013, and (1.6±1.2)×1013 km-1, respectively, and those of HDDVs were (2.2±1.2)×1015, 2.0×1015, and (7.1±2.1)×1014 km-1, respectively. With improvement in emission control level, the particle number emission control of LDGVs and HDDVs generally showed a good downward trend. However, the emission of PM above 110 nm from LDGVs did not improve with the emission control level. Although the quantity emission factor of HDDVs with particle size above 110 nm is relatively low, its harm to the environment cannot be ignored, which should justify necessary attention.
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During the COVID-19 lockdown period (from January 23 to February 29, 2020), ambient PM2.5 concentrations in the Yangtze River Delta (YRD) region were observed to be much lower, while the maximum daily 8 h average (MDA8) O3 concentrations became much higher compared to those before the lockdown (from January 1 to 22, 2020). Here, we show that emission reduction is the major driving force for the PM2.5 change, contributing to a PM2.5 decrease by 37% to 55% in the four YRD major cities (i.e., Shanghai, Hangzhou, Nanjing, and Hefei), but the MDA8 O3 increase is driven by both emission reduction (29%-52%) and variation in meteorological conditions (17%- 49%). Among all pollutants, reduction in emissions mainly of primary PM contributes to a PM2.5 decrease by 28% to 46%, and NOx emission reduction contributes 7% to 10%. Although NOx emission reduction dominates the MDA8 O3 increase (38%-59%), volatile organic compounds (VOCs) emission reduction lead to a 5% to 9% MDA8 O3 decrease. Increased O3 promotes secondary aerosol formation and partially offsets the decrease of PM2.5 caused by the primary PM emission reductions. The results demonstrate that more coordinated air pollution control strategies are needed in YRD.
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Organic carbon (OC) and elemental carbon (EC) emission factors from 27 State 3-5 light-duty gasoline vehicles (LDGVs) were tested in this study using a CVS (Constant Volume Sampling) system on a dynamometer. The influences of start conditions, driving cycles, and fuel injection technologies on the OC and EC emissions were analyzed. The results show that the OC emission factors of the tested State 3 to 5 LDGVs were (2.09±1.03), (1.59±0.78), and (0.75±0.31) mg·km-1, respectively, and the EC emission factors were (1.98±1.42), (1.57±1.80), and (0.65±0.49) mg·km-1. Both OC and EC emissions significantly decreased with the promotion of emission standards. The OC/EC ratios were 1.54±0.92, 1.53±0.91, and 1.47±0.66, respectively. OC1, OC2, EC1, and EC2 were the most important carbonaceous components from LDGVs, accounting for 15%, 20.6%, 22.2%, and 21.7%, respectively. OC and EC emission factors under cold-start conditions were 1.4 and 1.8 times those under hot-start conditions. OC and EC emission factors for highway cycles were 2 and 4 times those for urban cycles. OC emission factors from GDI (Gasoline Direct Injection) engines were close to those from PFI (Port Fuel Injection) engines. However, their EC emission factors were 1.7 times those from PFI engines. With the increasing popularity of GDI engines in LDGV fleets in China, the EC emissions from these engines should be paid more attention in the future.
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The selective catalytic reduction system (SCR) is an essential method to reduce NOx emissions from heavy-duty diesel engine-powered vehicles, which include conventional diesel buses and diesel-electric hybrid buses. Using wireless remote communication technology, the SCR system status and NOx emissions were reviewed for ten fully-operational hybrid buses from Hangzhou China in this research. Under the internal combustion engine mode, the main factors studied were vehicle speed, engine operation conditions and environment temperature, impact on the SCR catalyst outlet temperature and NOx concentration and dosing rate of the urea injector of the SCR system. The research result shows that (32.4±4)% of the operational time of the hybrid buses with SCR system was spent in internal combustion engine mode, and under (26.9±11)% of the operation time of this mode, the SCR system did not dose urea. The average NOx emission reduction rate of the SCR system, when operating normally with hybrid buses, is about 59%. The main reasons for the high NOx emission of the diesel-electric hybrid buses in operation condition are poor satisfaction of the requirements of the SCR system control strategy and the SCR catalyst's low temperature conversion efficiency. Whenever the speed of the hybrid buses was above 40 km·h-1, the SCR catalyst outlet temperatures were higher than the 230â, and the NOx emission concentrations were significantly reduced, as the urea injector working proportion and urea quantity increased. In the winter, the SCR catalyst outlet temperature and urea injection quantity dropped with the reduced environment temperature, which led to increased NOx emissions.
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On-board emissions measurements were performed on a Handysize-class bulk carrier operating under real-world conditions. Emission factors (EFs) were determined for criteria pollutants such as NOx, CO, total hydrocarbons (THC), and PM; PM composition, including organic and elemental carbon (OC and EC), inorganic species, and a variety of organic compounds and VOC species (including alkanes, alkenes, single-ring aromatics, and oxygenated VOCs) were also analyzed. To investigate the impacts of engine type, fuel, and operating conditions on emissions, measurements were conducted on one main and one auxiliary engines using low- and high-sulfur fuels (LSF and HSF) under actual operating conditions, including at-berth, maneuvering, and cruising at different engine loads. OC was the most abundant PM component (contributing 45-65%), followed by sulfate (2-15%) and EC (1-20%). Compounds with 3 or 4 aromatic rings, including phenanthrene, fluoranthene, pyrene, and benzo[b+k]fluoranthene, dominated the particulate polycyclic aromatic hydrocarbons (PAHs) emitted from the ship, accounting for 69-89% of the total PAHs. Single-ring aromatics constituted 50-78% of the emitted VOCs and were dominated by toluene. In this study, switching from HSF (1.12% S) to LSF (0.38% S) reduced emitted PM by 12%, OC by 20%, sulfate by 71%, and particulate PAHs by 94%, but caused an increase in single-ring aromatics. The power-based EFs generally decreased with increasing engine loads. However, decreasing the ship engine load also reduced the vessel speed and, thus, decreased emissions over a given voyage distance. Herein, a Vessel Speed Reduction (VSR) from 11 to 8-9 knots decreased NOx and PM emissions by approximately 33% and 36%, respectively, and OC, EC, sulfate, and particulate PAHs in PM emissions by 34%, 83%, 29%, and 11%. These data can be used to minimize uncertainty in the emission factors used in ship emissions calculations.
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Contaminantes Atmosféricos/análisis , Monitoreo del Ambiente , Material Particulado/análisis , Navíos , Emisiones de Vehículos/análisis , Aeronaves , Carbono/análisis , Polvo , Gases , Hidrocarburos/análisis , Compuestos Orgánicos , Hidrocarburos Policíclicos Aromáticos/análisisRESUMEN
Gaseous emissions from 25 State 2-5 light-duty gasoline vehicles were tested by Vehicle Mass Analysis System (VMAS) and CVS (Constant Volume Sampling) system, respectively. The correlations of emission factors of tested vehicles measured by these 2 methods were analyzed. The results showed that emission factors of light-duty gasoline vehicle had a decreasing trend with the promotion of emission standard. There were some high-emitting vehicles in the fleet of tested State 2 and State 3 vehicles, but fewer in State 4 or Stated 5 vehicle fleet. The correlations of the emission factors measured by the 2 methods deteriorated with the promotion of emission standard. The relative bias of CO and HC+NOx emission factors measured by the 2 methods reached 197% and 177%, respectively. The correlation coefficient of emission factors of higher-emitting vehicles was 0.75-0.85, while that of lower-emitting vehicles was only 0.46. If tighter emission standard of in-use light-duty gasoline vehicle was adopted, the false positive rate of measurement results by VMAS would rise significantly. In summary, VMAS method is hard to be applied in the emission measurements of light-duty gasoline vehicles with stricter emissions standard. It is necessary to conduct more studies on sophisticated in-use vehicle measurement system.
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Based on site investigation of non-road vehicles in Shanghai and Hangzhou located in east China, non-road vehicle emission inventory in 2014 was established in these cities as well as its emission inventory technology. Characteristics of non-road vehicle were also analyzed, including classification, type of fuel, power and emission standard. The results showed that diesel consumed by non-road vehicles was 6.1×105 t in Shanghai and 3.2×105 t in Hangzhou; NOx emission was 3.09×104 t in Shanghai and 1.72×104 t in Hangzhou; PM2.5 emission was 1.41×103 t in Shanghai and 8.1×102 t in Hangzhou, 2014. Emissions from excavators and other construction equipment contributed the most in non-road vehicle emission inventory. Non-road vehicle has become one of the important sources of urban air pollution, whose NOx emissions accounted for 11.1% of all urban sources in Shanghai and 16.1% in Hangzhou, and accounted for 18.5% of mobile sources in Shanghai and 32.2% in Hangzhou.