scholarly journals A statistical proxy for sulphuric acid concentration

2011 ◽  
Vol 11 (21) ◽  
pp. 11319-11334 ◽  
Author(s):  
S. Mikkonen ◽  
S. Romakkaniemi ◽  
J. N. Smith ◽  
H. Korhonen ◽  
T. Petäjä ◽  
...  

Abstract. Gaseous sulphuric acid is a key precursor for new particle formation in the atmosphere. Previous experimental studies have confirmed a strong correlation between the number concentrations of freshly formed particles and the ambient concentrations of sulphuric acid. This study evaluates a body of experimental gas phase sulphuric acid concentrations, as measured by Chemical Ionization Mass Spectrometry (CIMS) during six intensive measurement campaigns and one long-term observational period. The campaign datasets were measured in Hyytiälä, Finland, in 2003 and 2007, in San Pietro Capofiume, Italy, in 2009, in Melpitz, Germany, in 2008, in Atlanta, Georgia, USA, in 2002, and in Niwot Ridge, Colorado, USA, in 2007. The long term data were obtained in Hohenpeissenberg, Germany, during 1998 to 2000. The measured time series were used to construct proximity measures ("proxies") for sulphuric acid concentration by using statistical analysis methods. The objective of this study is to find a proxy for sulfuric acid that is valid in as many different atmospheric environments as possible. Our most accurate and universal formulation of the sulphuric acid concentration proxy uses global solar radiation, SO2 concentration, condensation sink and relative humidity as predictor variables, yielding a correlation measure (R) of 0.87 between observed concentration and the proxy predictions. Interestingly, the role of the condensation sink in the proxy was only minor, since similarly accurate proxies could be constructed with global solar radiation and SO2 concentration alone. This could be attributed to SO2 being an indicator for anthropogenic pollution, including particulate and gaseous emissions which represent sinks for the OH radical that, in turn, is needed for the formation of sulphuric acid.

2011 ◽  
Vol 11 (7) ◽  
pp. 20141-20179 ◽  
Author(s):  
S. Mikkonen ◽  
S. Romakkaniemi ◽  
J. N. Smith ◽  
H. Korhonen ◽  
T. Petäjä ◽  
...  

Abstract. Gaseous sulphuric acid is a key precursor for new particle formation in the atmosphere. Previous experimental studies have confirmed a strong correlation between the number concentrations of freshly formed particles and the ambient concentrations of sulphuric acid. This study evaluates a body of experimental gas phase sulphuric acid concentrations, as measured by Chemical Ionization Mass Spectrometry (CIMS) during six intensive measurement campaigns and one long-term observational period. The campaign datasets were measured in Hyytiälä, Finland, in 2003 and 2007, in San Pietro Capofiume, Italy, in 2009, in Melpitz, Germany, in 2008, in Atlanta, Georgia, USA, in 2002, and in Niwot Ridge, Colorado, USA, in 2007. The long term data were obtained in Hohenpeissenberg, Germany, during 1998 to 2000. The measured time series were used to construct proximity measures ("proxies") for sulphuric acid concentration by using statistical analysis methods. The objective of this study is to find a proxy for sulfuric acid that is valid in as many different atmospheric environments as possible. Our most accurate and universal formulation of the sulphuric acid concentration proxy uses global solar radiation, SO2 concentration, condensation sink and relative humidity as predictor variables, yielding a correlation measure (R) of 0.87 between observed concentration and the proxy predictions. Interestingly, the role of the condensation sink in the proxy was only minor, since similarly accurate proxies could be constructed with global solar radiation and SO2 concentration alone. This could be attributed to SO2 being an indicator for anthropogenic pollution, including particulate and gaseous emissions which represent sinks for the OH radical that, in turn, is needed for the formation of sulphuric acid.


2014 ◽  
Vol 7 (7) ◽  
pp. 6595-6624
Author(s):  
L. Rondo ◽  
A. Kürten ◽  
S. Ehrhart ◽  
S. Schobesberger ◽  
A. Franchin ◽  
...  

Abstract. Ternary aerosol nucleation experiments were conducted in the CLOUD chamber at CERN in order to investigate the influence of ions on new particle formation. Neutral and ion-induced nucleation experiments, i.e., with and without the presence of ions, were carried out under precisely controlled conditions. The sulphuric acid concentration was measured with a Chemical Ionization Mass Spectrometer (CIMS) during the new particle formation experiments. The added ternary trace gases were ammonia (NH3), dimethylamine (DMA, C2H7N) or oxidised products of pinanediol (PD, C10H18O2). When pinanediol was introduced into the chamber, an increase in the mass spectrometric signal used to determine the sulphuric acid concentration (m/z 97, i.e., HSO4−) was observed due to ions from the CLOUD chamber. The enhancement was only observed during ion-induced nucleation measurements by using either galactic cosmic rays (GCR) or the proton synchrotron (PS) pion beam for the ion generation, respectively. The ion effect typically involved an increase in the apparent sulphuric acid concentration by a factor of ~2 to 3 and was qualitatively verified by the ion measurements by an Atmospheric Pressure interface-Time Of Flight (APi-TOF) mass spectrometer. By applying a high voltage (HV) clearing field inside the CLOUD chamber the ion effect on the CIMS measurement was completely eliminated since, under these conditions, small ions are swept from the chamber in about one second. In order to exclude the ion effect and to provide corrected sulphuric acid concentrations during the GCR and PS beam nucleation experiments, a parameterisation was derived that utilizes the trace gas concentrations and the UV light intensity as input parameters. Atmospheric sulphuric acid measurements with a CIMS showed an insignificant ion effect.


2006 ◽  
Vol 6 (12) ◽  
pp. 4079-4091 ◽  
Author(s):  
S.-L. Sihto ◽  
M. Kulmala ◽  
V.-M. Kerminen ◽  
M. Dal Maso ◽  
T. Petäjä ◽  
...  

Abstract. We have investigated the formation and early growth of atmospheric secondary aerosol particles building on atmospheric measurements. The measurements were part of the QUEST 2 campaign which took place in spring 2003 in Hyytiälä (Finland). During the campaign numerous aerosol particle formation events occurred of which 15 were accompanied by gaseous sulphuric acid measurements. Our detailed analysis of these 15 events is focussed on nucleation and early growth (to a diameter of 3 nm) of fresh particles. It revealed that new particle formation seems to be a function of the gaseous sulphuric acid concentration to the power from one to two when the time delay between the sulphuric acid and particle number concentration is taken into account. From the time delay the growth rates of freshly nucleated particles from 1 nm to 3 nm were determined. The mean growth rate was 1.2 nm/h and it was clearly correlated with the gaseous sulphuric acid concentration. We tested two nucleation mechanisms – recently proposed cluster activation and kinetic type nucleation – as possible candidates to explain the observed dependences, and determined experimental nucleation coefficients. We found that some events are dominated by the activation mechanism and some by the kinetic mechanism. Inferred coefficients for the two nucleation mechanisms are the same order of magnitude as chemical reaction coefficients in the gas phase and they correlate with the product of gaseous sulphuric acid and ammonia concentrations. This indicates that besides gaseous sulphuric acid also ammonia has a role in nucleation.


2016 ◽  
Author(s):  
Rosa Delia García ◽  
Emilio Cuevas ◽  
Omaira Elena García ◽  
Ramon Ramón ◽  
Pedro Miguel Romero-Campos ◽  
...  

Abstract. A 1-year intercomparison of classical and modern radiation and sunshine duration instruments has been performed at Izaña Atmospheric Observatory (IZO) located in Tenerife (Canary Islands, Spain) starting on July 17, 2014. We compare global solar radiation (GSR) records measured with a CM-21 pyranometer Kipp & Zonen, taken in the framework of the Baseline Surface Radiation Network, with those measured with a Multifilter Rotating Shadowband Radiometer (MFRSR), and a bimetallic pyranometer (PYR), and GSR estimated from sunshine duration performed by a Campbell-Stokes sunshine recorder (CS) and a Kipp & Zonen sunshine duration sensor (CSD). Given the GSR BSRN records are subject of strict quality controls (based on principles of physical limits and comparison with the LibRadtran model), they have been used as reference in the intercomparison study. We obtain an overall root mean square error (RMSE) of ~0.9 MJm2 (4 %) for GSR PYR and GSR MFRSR, 1.9 MJm2 (7 %) and 1.2 MJm2 (5 %) for GSR CS and GSR CSD, respectively. Factors such as temperature, fraction of the clear sky, relative humidity and the solar zenith angle have shown to moderately affect the GSR observations. As application of the methodology developed in this work, we have re-evaluated the GSR time series between 1977 and 1991 obtained with two PYRs at IZO. By comparing with coincident GSR estimates from SD observations, we probe the high consistency of those measurements and their temporal stability. These results demonstrate that 1) the continuous-basis intercomparison of different GSR techniques offers important diagnostics for identifying inconsistencies between GSR data records, and 2) the GSR measurements performed with classical and more simple instruments are consistent with more modern techniques and, thus, valid to recover GSR time series and complete worldwide distributed GSR data. The intercomparison and quality assessment of these different techniques have allowed to obtain a complete and consistent long-term global solar radiation series (1977–2015) at Izaña.


2012 ◽  
Vol 2012 ◽  
pp. 1-9 ◽  
Author(s):  
Haixiang Zang ◽  
Qingshan Xu ◽  
Pengwei Du ◽  
Katsuhiro Ichiyanagi

A modified typical meteorological year (TMY) method is proposed for generating TMY from practical measured weather data. A total of eleven weather indices and novel assigned weighting factors are applied in the processing of forming the TMY database. TMYs of 35 cities in China are generated based on the latest and accurate measured weather data (dry bulb temperature, relative humidity, wind velocity, atmospheric pressure, and daily global solar radiation) in the period of 1994–2010. The TMY data and typical solar radiation data are also investigated and analyzed in this paper, which are important in the utilizations of solar energy systems.


2016 ◽  
Vol 113 (51) ◽  
pp. E8210-E8218 ◽  
Author(s):  
Kyu-Tae Lee ◽  
Yuan Yao ◽  
Junwen He ◽  
Brent Fisher ◽  
Xing Sheng ◽  
...  

Emerging classes of concentrator photovoltaic (CPV) modules reach efficiencies that are far greater than those of even the highest performance flat-plate PV technologies, with architectures that have the potential to provide the lowest cost of energy in locations with high direct normal irradiance (DNI). A disadvantage is their inability to effectively use diffuse sunlight, thereby constraining widespread geographic deployment and limiting performance even under the most favorable DNI conditions. This study introduces a module design that integrates capabilities in flat-plate PV directly with the most sophisticated CPV technologies, for capture of both direct and diffuse sunlight, thereby achieving efficiency in PV conversion of the global solar radiation. Specific examples of this scheme exploit commodity silicon (Si) cells integrated with two different CPV module designs, where they capture light that is not efficiently directed by the concentrator optics onto large-scale arrays of miniature multijunction (MJ) solar cells that use advanced III–V semiconductor technologies. In this CPV+scheme (“+” denotes the addition of diffuse collector), the Si and MJ cells operate independently on indirect and direct solar radiation, respectively. On-sun experimental studies of CPV+modules at latitudes of 35.9886° N (Durham, NC), 40.1125° N (Bondville, IL), and 38.9072° N (Washington, DC) show improvements in absolute module efficiencies of between 1.02% and 8.45% over values obtained using otherwise similar CPV modules, depending on weather conditions. These concepts have the potential to expand the geographic reach and improve the cost-effectiveness of the highest efficiency forms of PV power generation.


2009 ◽  
Vol 9 (9) ◽  
pp. 2933-2947 ◽  
Author(s):  
S.-L. Sihto ◽  
H. Vuollekoski ◽  
J. Leppä ◽  
I. Riipinen ◽  
V.-M. Kerminen ◽  
...  

Abstract. We have performed a series of simulations with an aerosol dynamics box model to study the connection between new particle formation and sulphuric acid concentration. For nucleation either activation mechanism with a linear dependence on the sulphuric acid concentration, kinetic mechanism with a squared dependence on the sulphuric acid concentration or ternary H2O-H2SO4-NH3 nucleation was assumed. The aim was to study the factors that affect the sulphuric acid dependence during the early stages of particle growth, and specifically to find conditions which would yield the linear dependence between the particle number concentration at 3–6 nm and sulphuric acid, as observed in field experiments. The simulations showed that the correlation with sulphuric acid may change during the growth from nucleation size to 3–6 nm size range, the main reason being the size dependent growth rate between 1 and 3 nm. In addition, the assumed size for the nucleated clusters had a crucial impact on the sulphuric acid dependence at 3 nm. A linear dependence between the particle number concentration at 3 nm and sulphuric acid was achieved, when activation nucleation mechanism was used with a low saturation vapour pressure for the condensable organic vapour, or with nucleation taking place at ~2 nm instead of ~1 nm. Simulations with activation, kinetic and ternary nucleation showed that ternary nucleation reproduces too steep dependence on sulphuric acid as compared to the linear or square dependence observed in field measurements.


2010 ◽  
Vol 8 (1) ◽  
pp. 149-154 ◽  
Author(s):  
Maciej Jabłoński

AbstractEnriched titanium raw materials with high titanium content called titanium slags are received by the electrothermal reduction of ilmenite. Titanium slags are most frequently used in the titanium dioxide industry. The reaction of titanium slags with sulphuric acid is strongly exothermic and creates danger of thermal explosion. Kinetics of this reaction depends on the parameters such as temperature of initiation, sulphuric acid concentration and dimension of particles of titanium slag. The reaction of titanium slag with sulphuric acid was investigated at non-isothermal conditions in a special construction calorimeter. The observed thermal power changes in the calorimeter (“calorimeter run”), are the basis for estimation of reaction kinetics. A proposed model describing the thermal power changes and taking into account the moment of initiation of reaction is presented. The calorimetric investigations showed, that reaction rate of titanium slags with sulphuric acid depends on initial temperature of reaction, size of particles of titanium raw material and sulphuric acid concentration.


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