scholarly journals On the effects of organic matter and sulphur-containing compounds on the CCN activation of combustion particles

2005 ◽  
Vol 5 (12) ◽  
pp. 3187-3203 ◽  
Author(s):  
A. Petzold ◽  
M. Gysel ◽  
X. Vancassel ◽  
R. Hitzenberger ◽  
H. Puxbaum ◽  
...  

Abstract. The European PartEmis project (Measurement and prediction of emissions of aerosols and gaseous precursors from gas turbine engines) was focussed on the characterisation and quantification of exhaust emissions from a gas turbine engine. The combustion aerosol characterisation included on-line measurements of mass and number concentration, size distribution, mixing state, thermal stability of internally mixed particles, hygroscopicity, cloud condensation nuclei (CCN) activation potential, and off-line analysis of chemical composition. Based on this extensive data set, the role of sulphuric acid coating and of the organic fraction of the combustion particles for the CCN activation was investigated. Modelling of CCN activation was conducted using microphysical and chemical properties obtained from the measurements as input data. Coating the combustion particles with water-soluble sulphuric acid, increases the potential CCN activation, or lowers the activation diameter, respectively. The adaptation of a Köhler model to the experimental data yielded coatings from 0.1 to 3 vol-% of water-soluble matter, which corresponds to an increase in the fraction of CCN-activated combustion particles from ≤10−4 to ≌10−2 at a water vapour saturation ratio Sw=1.006. Additional particle coating by coagulation of combustion particles and aqueous sulphuric acid particles formed by nucleation further reduces the CCN activation diameter. In contrast, particles containing a large fraction of non-volatile organic compounds grow significantly less at high relative humidity than particles with a lower content of non-volatile OC. The resulting reduction in the potential CCN activation with an increasing fraction of non-volatile OC becomes visible as a trend in the experimental data. While a coating of water-soluble sulphuric acid increases the potential CCN activation, or lowers the activation diameter, respectively, the non-volatile organic compounds, mainly found at lower combustion temperatures, can partially compensate this sulphuric acid-related enhancement of CCN activation of carbonaceous combustion aerosol particles.

2005 ◽  
Vol 5 (3) ◽  
pp. 2599-2642 ◽  
Author(s):  
A. Petzold ◽  
M. Gysel ◽  
X. Vancassel ◽  
R. Hitzenberger ◽  
H. Puxbaum ◽  
...  

Abstract. The European PartEmis project (''Measurement and prediction of emissions of aerosols and gaseous precursors from gas turbine engines'') was focussed on the characterisation and quantification of exhaust emissions from a gas turbine engine. A comprehensive suite of aerosol, gas and chemi-ion measurements were conducted under different combustor operating conditions and fuel sulphur concentrations. Combustion aerosol characterisation included on-line measurements of mass and number concentration, size distribution, mixing state, thermal stability of internally mixed particles, hygroscopicity, cloud condensation nuclei (CCN) activation potential, and off-line analysis of chemical composition. Modelling of CCN activation of combustion particles was conducted using microphysical and chemical properties obtained from the measurements as input data. Based on this unique data set, the role of sulphuric acid coatings on the combustion particles, formed in the cooling exhaust plume through either direct condensation of gaseous sulphuric acid or coagulation with volatile condensation particles nucleating from gaseous sulphuric acid, and the role of the organic fraction for the CCN activation of combustion particles was investigated. It was found that particles containing a large fraction of non-volatile organic compounds grow significantly less at high relative humidity than particles with a lower content of non-volatile OC. Also the effect of the non-volatile OC fraction on the potential CCN activation is significant. While a coating of water-soluble sulphuric acid increases the potential CCN activation, or lowers the activation diameter, respectively, the non-volatile organic compounds, mainly found at lower combustion temperatures, can partially compensate this sulphuric acid-related enhancement of CCN activation of carbonaceous combustion aerosol particles.


2018 ◽  
Vol 18 (23) ◽  
pp. 17637-17654 ◽  
Author(s):  
Quanyang Lu ◽  
Yunliang Zhao ◽  
Allen L. Robinson

Abstract. Emissions from mobile sources are important contributors to both primary and secondary organic aerosols (POA and SOA) in urban environments. We compiled recently published data to create comprehensive model-ready organic emission profiles for on- and off-road gasoline, gas-turbine, and diesel engines. The profiles span the entire volatility range, including volatile organic compounds (VOCs, effective saturation concentration C*=107–1011 µg m−3), intermediate-volatile organic compounds (IVOCs, C*=103–106 µg m−3), semi-volatile organic compounds (SVOCs, C*=1–102 µg m−3), low-volatile organic compounds (LVOCs, C*≤0.1 µg m−3) and non-volatile organic compounds (NVOCs). Although our profiles are comprehensive, this paper focuses on the IVOC and SVOC fractions to improve predictions of SOA formation. Organic emissions from all three source categories feature tri-modal volatility distributions (“by-product” mode, “fuel” mode, and “lubricant oil” mode). Despite wide variations in emission factors for total organics, the mass fractions of IVOCs and SVOCs are relatively consistent across sources using the same fuel type, for example, contributing 4.5 % (2.4 %–9.6 % as 10th to 90th percentiles) and 1.1 % (0.4 %–3.6 %) for a diverse fleet of light duty gasoline vehicles tested over the cold-start unified cycle, respectively. This consistency indicates that a limited number of profiles are needed to construct emissions inventories. We define five distinct profiles: (i) cold-start and off-road gasoline, (ii) hot-operation gasoline, (iii) gas-turbine, (iv) traditional diesel and (v) diesel-particulate-filter equipped diesel. These profiles are designed to be directly implemented into chemical transport models and inventories. We compare emissions to unburned fuel; gasoline and gas-turbine emissions are enriched in IVOCs relative to unburned fuel. The new profiles predict that IVOCs and SVOC vapour will contribute significantly to SOA production. We compare our new profiles to traditional source profiles and various scaling approaches used previously to estimate IVOC emissions. These comparisons reveal large errors in these different approaches, ranging from failure to account for IVOC emissions (traditional source profiles) to assuming source-invariant scaling ratios (most IVOC scaling approaches).


2017 ◽  
Author(s):  
Ganlin Huang ◽  
Rosie Brook ◽  
Monica Crippa ◽  
Greet Janssens-Maenhout ◽  
Christian Schieberle ◽  
...  

Abstract. Non-methane volatile organic compounds (NMVOC) include a large number of chemical species which differ significantly in their chemical characteristics and thus in their impacts on ozone and secondary organic aerosols formation. It is important that chemical transport models (CTMs) simulate the chemical transformation of the different NMVOC species in the troposphere consistently. In most emission inventories, however, only total NMVOC emissions are reported, which need to be decomposed into classes to fit the requirements of CTMs. For instance, the Emissions Database for Global Atmospheric Research (EDGAR) provides spatially resolved global anthropogenic emissions of total NMVOC. In this study the EDGAR NMVOC inventory was revised and extended in time and in sectors. Moreover the new version of NMVOC emission data in the EDGAR database were disaggregated on a high sector resolution to individual species or species groups, thus enhancing the usability of the NMVOC emission data by the modelling community. Region- and source-specific speciation profiles of NMVOC species or species groups, are compiled and mapped to EDGAR processes (high resolution of sectors), with corresponding quality codes specifying the quality of the mapping. Individual NMVOC species in different profiles are aggregated to 25 species groups, in line with the common classification of the Global Emissions Initiative (GEIA). Global annual grid maps with a resolution of 0.1° × 0.1° for the period 1970–2012 are produced by sector and species. Furthermore, trends of NMVOC composition are analysed taking road transport and residential sources in Germany and the United Kingdom (UK) as examples.


Author(s):  
Michael T. Timko ◽  
Scott C. Herndon ◽  
Ezra C. Wood ◽  
Timothy B. Onasch ◽  
Megan J. Northway ◽  
...  

The potential human health and environmental impacts of aircraft gas turbine engine emissions during normal airport operation are issues of growing concern. During the JETS/Aircraft Particle Emissions eXperiment(APEX)-2 and APEX-3 field campaigns, we performed an extensive series of gas phase and particulate emissions measurements of on-wing gas turbine engines. In all, nine different CFM56 style engines (including both CFM56-3B1 and -7B22 models) and seven additional engines (two RB211-535E4-B engines, three AE3007 engines, one PW4158, and one CJ6108A) were studied to evaluate engine-to-engine variability. Specific gas-phase measurements include NO2, NO, and total NOx, HCHO, C2H4, CO, and a range of volatile organic compounds (e.g., benzene, styrene, toluene, naphthalene). A number of broad conclusions can be made based on the gas-phase data set: (1) field measurements of gas-phase emission indices (EIs) are generally consistent with ICAO certification values; (2) speciation of gas phase NOx between NO and NO2 is reproducible for different engine types and favors NO2 at low power (and low fuel flow rate) and NO at high power (high fuel flow rate); (3) emission indices of gas-phase organic compounds and CO decrease rapidly with increasing fuel flow rate; (4) plotting EI-CO or volatile organic compound EIs against fuel flow rate collapses much of the variability between the different engines, with one exception (AE3007); (5) HCHO, ethylene, acetaldehyde, and propene are the most abundant volatile organic compounds present in the exhaust gases that we can detect, independent of engine technology differences. Empirical correlations accurate to within 30% and based on the publicly available engine parameters are presented for estimating EI-NOx and EI-NO2. Engine-to-engine variability, unavailability of combustor input conditions, changing ambient temperatures, and complex reaction dynamics limit the accuracy of global correlations for CO or volatile organic compound EIs.


Sign in / Sign up

Export Citation Format

Share Document