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Discussion Paper
Atmos. Meas. Tech. Discuss., 6, 10617–10651, 2013
www.atmos-meas-tech-discuss.net/6/10617/2013/ Measurement AMTD
doi:10.5194/amtd-6-10617-2013
© Author(s) 2013. CC Attribution 3.0 License.
Techniques
Discussions 6, 10617–10651, 2013

This discussion paper is/has been under review for the journal Atmospheric Measurement Airborne emission
Techniques (AMT). Please refer to the corresponding final paper in AMT if available. measurements of

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individual ships

Discussion Paper
Airborne emission measurements of SO2, J. Beecken et al.

NOx and particles from individual ships

using sniffer technique Title Page

Abstract Introduction
1 1 1 1 2

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J. Beecken , J. Mellqvist , K. Salo , J. Ekholm , and J.-P. Jalkanen Conclusions References

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1
Chalmers University of Technology, Earth and Space Sciences, Gothenburg, Sweden Tables Figures
2
Finnish Meteorological Institute, Helsinki, Finland

Received: 12 July 2013 – Accepted: 11 November 2013 – Published: 9 December 2013 J I

Correspondence to: J. Beecken (beecken@chalmers.se) J I

Published by Copernicus Publications on behalf of the European Geosciences Union.
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 Discussion Paper
Abstract
AMTD
A dedicated system for airborne ship emission measurements of SO2 , NOx and parti-
cles has been developed and used from several small aircrafts. The system has been 6, 10617–10651, 2013
adapted for fast response measurements at 1 Hz and the use of several of the in-
5 struments is unique. The uncertainty of the given data is about 20.3 % for SO2 and Airborne emission
23.8 % for NOx emission factors. Multiple measurements of 158 ships measured from measurements of

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the air on the Baltic and North Sea during 2011 and 2012 show emission factors of individual ships
18.8 ± 6.5 g kg−1 , 66.6 ± 23.4 g kg−1 , and 1.8 ± 1.3 × 1016 particles kg−1

Discussion Paper
fuel fuel fuel
for SO2 , NOx
and particle number respectively. The particle size distributions were measured for par- J. Beecken et al.
10 ticle diameters between 15 and 560 nm. The mean sizes of the particles are between
50 and 62 nm dependent on the distance to the source and the number size distribution
is mono-modal. Concerning the sulfur fuel content 85 % of the ships comply with the Title Page

IMO limits. The sulfur emission has decreased compared to earlier measurements from Abstract Introduction
2007 to 2009. The presented method can be implemented for regular ship compliance

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15 monitoring. Conclusions References

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Tables Figures
1 Introduction
J I
Ships emit large quantities of air pollutants and it is necessary to reduce these to
improve air quality (Corbett et al., 2007; European Commission, 2009). Most countries J I

have ratified the International Maritime Organization (IMO) Marpol Annex VI protocol Back Close

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20 and EU has adopted directive 2012/33/EU which sets limits on nitrogen oxides (NOx )

Discussion Paper
and sulfur dioxide (SO2 ) emissions from ship exhausts. The regulation includes a global Full Screen / Esc
cap of sulfur fuel content (SFC) and contains provisions allowing for establishment of
special SO2 and NOx Emission Control Areas, i.e. SECA and NECA. The Baltic Sea, Printer-friendly Version
the North Sea, English Channel and the coastal waters around US and Canada are
Interactive Discussion
25 designated as SECA while the North American area also is a NECA. Following the
IMO regulation there will be a global cap of 0.5 % SFC used by vessels from 2020.
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 Discussion Paper
In the SECAs the used SFC must not exceed 0.1 % from 2015. The IMO regulation
regarding NOx is more complicated than for SO2 , since NOx production is dependent AMTD
on the nature of the combustion process rather than being related to fuel composition.
6, 10617–10651, 2013
IMO has therefore chosen emission limits (resolution MEPC.177(58)) that correspond
5 to the total NOx emission in gram per axial shaft energy produced from the engine
in kWh. These limits depend on the engine type and they are therefore given vs. the Airborne emission
rated rotational speed of the specific engines. Ships built between 2000 and 2010 measurements of

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should emit less than a certain limit (tier 1) while ships built after 2011 should emit individual ships

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20 % less (tier 2). In NECA the emissions should be 80 % lower than tier 1 by 2016
J. Beecken et al.
10 (tier 3), although this time limit is presently being renegotiated within IMO.
There are several ways available for the shipping companies to adapt to the new
regulations. It is possible to use alternative fuel i.e. liquefied natural gas (LNG) or
Title Page
methanol. Abatement techniques to reduce both NOx and SO2 emissions are avail-
able. However these possibilities are limited due to high costs for investments in often Abstract Introduction
15 technologies which are under ongoing development. Therefore it is believed that there

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Conclusions References
will be a higher demand and higher prices on low sulfur fuels in the future.

Discussion Paper
In the SECA the cost for ship transport will increase by 50–70 % due to increased Tables Figures
fuel costs (Kalli et al., 2009). There will hence be considerable economic incentive not
to comply with SECA regulation. Today the fuel of the ships is controlled by Port State J I
20 Control authorities conducting random checks of bunker delivery notes, fuel logs and
occasional fuel sample analyses in harbors. This is time consuming and few ships are J I
being controlled. There is no available technique able to control what fuel is used in
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the open sea and in general it is considered easy to tamper with the usage of fuel,

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especially since ships are using several tanks, often with different fuel.

Discussion Paper
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25 Here we present airborne emission measurements of emission factors in mass of
emitted pollutant per amount of consumed fuel for individual ships. One valuable use of Printer-friendly Version
such data is as input data for modeling of the environmental impact of shipping. A new
type of ship emission model that has emerged recently calculates instantaneous emis- Interactive Discussion

sions of ships based on ship movement from Automatic Identification System (AIS),

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ship propulsion (Alföldy et al., 2012) calculations and emission factors (Jalkanen et al.,
2009, 2012). The latter are taken from laboratory tests and occasional on board mea- AMTD
surements (Moldanova et al., 2009; Petzold et al., 2004, 2008). The emission factors
6, 10617–10651, 2013
depend on engine type, fuel type, use of abatement equipment and load. In general
5 there are large uncertainties in the emission factors for some species, such as parti-
cles, and within the SECAs there is additional uncertainty in how well the IMO legisla- Airborne emission
tion will be respected regarding fuel use and abatement technologies. There is hence measurements of

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substantial need for efficient techniques for remote measurements of real ship emis- individual ships

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sions.
J. Beecken et al.
10 The airborne sniffer system described here has been developed as part of a Swedish
national project named Identification of gross polluting ships (IGPS) (Mellqvist and
Berg, 2010, 2013; Mellqvist et al., 2008) aimed at developing a remote surveillance
Title Page
system to control whether individual ships obeys the IMO legislation of reduced sul-
phur fuel content (SFC) and NOx emissions, as discussed above (Alföldy et al., 2012). Abstract Introduction
15 The sniffer system is usually combined with an optical system (Mellqvist and Berg,

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Conclusions References
2013) that can be used as a first alert system and also to quantify the emission in

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g s−1 , but this will not be discussed further here. Tables Figures
The principle of the sniffer method is to obtain emission factors in g pollutant per kg
fuel by measuring the ratio of the concentration of the pollutant vs. the concentration of J I
20 CO2 , inside the emission plume of the ships. This principle has been employed in sev-
eral other studies both from the air, ships and harbors (Alföldy et al., 2012; Balzani Lööv J I
et al., 2013; Chen et al., 2005; Mellqvist and Berg, 2013; Mellqvist et al., 2008; Sinha
Back Close
et al., 2003) but for a relatively small number of vessels. Here we demonstrate a dedi-

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cated system meant for routine surveillance of ship emissions from small airplanes and

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25 other platforms. The system includes a fast electrical mobility system to measure par-
ticle number size distribution, used here in flight for the first time and a custom made Printer-friendly Version
cavity ring down system for fast airborne plume measurements of CO2 and CH4 . In
addition we show unique measurements of 158 individual ships carried out on several Interactive Discussion

occasions per ship in the North and Baltic Seas from a helicopter and two different

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airplanes during 2011 and 2012. This data is compared to data from 2007/2008 (Mel-
lqvist and Berg, 2010, 2013). The emission data for the individual ships has been inter- AMTD
preted against IMO limits and ship and engine type. This paper gives recommendations
6, 10617–10651, 2013
for how future compliance monitoring of ship emissions could be carried out.

Airborne emission
5 2 Methods measurements of

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individual ships
In this section the instrumentation, calibration methods and uncertainties are pre-

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sented. A description of the measurement campaigns and the plume sampling pro- J. Beecken et al.
cedure is given here.

2.1 Instrumentation Title Page

10 With the setup presented herein concentrations of CO2 , SO2 , NOx and sub micrometer Abstract Introduction
aerosol particles are measured.

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Conclusions References

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2.1.1 CO2 instrumentation
Tables Figures

A flight modified Picarro G-2301 is used to monitor the concentration of CO2 in the air.
This instrument is a greenhouse gas monitor based on cavity ring-down spectroscopy J I

15 (CRDS) (O’Keefe and Deacon, 1988). The instrument is capable of measuring CO2 , J I
CH4 and relative humidity (RH), the latter for correction issues. The measurements are
conducted sequentially with a time response t90 , i.e. the time to reach from 10 % to Back Close

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90 % of the sample value of less than 1 s. The measurement mode was modified in

Discussion Paper
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order to obtain as many measurements as possible during the short time in which the
20 aircraft traverses a plume. Depending on the needs, a low or high flow mode can be
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selected, with either one or two CO2 measurements per second for each flow setting.
In the latter case, the time slot for the measurement of CH4 is replaced by a second Interactive Discussion
CO2 sample within the same sequence. During the conducted measurement flights the
high flow, 2 Hz CO2 mode was used.
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2.1.2 SO2 instrumentation
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A modified Thermo 43i-TLE trace gas monitor was applied. This instrument analyzes
the volume mixing ratio of SO2 , VMR(SO2 ), in air by stimulating fluorescence by UV 6, 10617–10651, 2013
light (Luke, 1997). The detected intensity of fluorescence light is proportional to the
5 volume mixing ratio of SO2 molecules in the sample gas. In order to gain a higher flow Airborne emission
for faster sampling, a hydrocarbon stripper and the flow meter were removed from the measurements of

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monitor which resulted in a flow rate of 6 LPM. The t90 is about 2 s and the sample rate individual ships

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was set to 1 Hz. The Thermo 43i-TLE shows some cross response to NO and polycyclic
aromatic hydrocarbons (PAH). The VMR (SO2 ) reading increases by 1.5 % of the actual J. Beecken et al.
10 VMR(NO). In this study, this error was reduced by simultaneous measurements of NOx
assuming that the fraction of NO is 80 % (Alföldy et al., 2012). The cross-response of
Title Page
PAH is not important since these species are only present at small levels in ship plumes
(Williams et al., 2009). Abstract Introduction

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2.1.3 NOx instrumentation Conclusions References

Discussion Paper
15 The NOx measurements were performed with a Thermo 42i-TL trace gas monitor. This Tables Figures
instrument measures the VMR(NO) by chemiluminescence caused by the reaction of
NO with ozone (Kley and McFarland, 1980). The intensity of the detected chemilu- J I
minescent light is proportional to the VMR(NO) molecules. In order to measure the
J I
volume mixing ratio of NOx , the instrument was run in a mode in which NO2 is first
20 converted to NO. The sample flow was 1 LPM, which results in t90 of less than 1 s and Back Close

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the sample rate 1 Hz.

Discussion Paper
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2.1.4 Particle instrumentation
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The particle number size distributions ranging from 5.6 to 560 nm of the emitted plumes
were also measured in flight. This was done using the TSI 3090 engine exhaust particle Interactive Discussion

25 sizer (EEPS). The EEPS is developed for the monitoring of size distributions of aerosol

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particles in exhaust gases from combustion engines. It features 10 Hz simultaneous
sampling of 32 measurement channels between 5.6 nm and 560 nm and has a sample AMTD
flow of 10 LPM with a t90 of 0.5 s. The data was integrated for 1 s intervals. Particles in
6, 10617–10651, 2013
the sample air are charged and size selected according to the size dependent mobility
5 in an electrical field (Johnson et al., 2004). The charged particles impact on electrome-
ter plates and the number concentrations in the different size bins are achieved as the Airborne emission
generated current. The EEPS has been used for onboard monitoring of ship emissions measurements of

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(Hallquist et al., 2013) and stationary ship plume measurements (Jonsson et al., 2011) individual ships

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in earlier studies. The EEPS was found to be suitable for this kind of airborne plume
J. Beecken et al.
10 measurements and was to our knowledge used for the first time on an aircraft. When
the EEPS was operated onboard an airplane, it was connected to an isokinetic inlet for
which the flow was optimized for the airspeed during plume measurement. There was
Title Page
no isokinetic inlet used for the helicopter based measurements, because the airspeed
of the helicopter during measurement was much lower. Abstract Introduction

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15 2.2 Calculation of emission factors Conclusions References

Discussion Paper
Emission factors in weight g kg−1 fuel
or particles kg−1
fuel
are obtained as the ratio of the Tables Figures

pollutant x vs. the volume mixing ratio of CO2 . In practice the volume mixing ratios of
J I
P
all measured species are first summed along the plume transect ( [x]) and then these
values are normalized against the corresponding sum for CO2 . In Fig. 1 the volume J I
20 mixing ratios for CO2 , SO2 and NOx and the total concentration of particle number are
shown for one transect through the emission plume. Back Close

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The carbon fuel content is required for the calculation of the emission factors. Studies

Discussion Paper
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show it is 87±1.5 %; for marine gas oil, marine diesel oil and residual oil (Cooper, 2003;
Tuttle, 1995). For the calculations it is assumed that this fraction remains unchanged
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25 after fuel burning and that all burnt carbon is emitted as CO2 . Hence the SO2 emission
−1
factor, EF(SO2 ), in g kgfuel using the atomic respectively molar masses for C and SO2 Interactive Discussion

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 Discussion Paper
can be calculated by
h i m(SO2 ) M(SO2 ) ·
P
SO2,ppb
 P
SO2,ppb
 AMTD
EF (SO2 ) g kg−1
fuel
= = P  = 4.64 P  . (1) 6, 10617–10651, 2013
m(fuel) M(C)/0.87 · CO2,ppm CO2,ppm
The values of SO2 were corrected for the interference of NO. The cross-sensitivity of
Airborne emission
5 the modified instrument was experimentally found to be 1.5 %. A NO to NOx ratio of
measurements of
around 80 % P is assumed (Alföldy et al., 2012).PHence, for samples where NOx was

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individual ships
measured, [SO2 ] was subtracted by 1.2 % of [NOx ] over the same plume sample.

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For samples without measured NOx data, modeled data from the STEAM database J. Beecken et al.
(Jalkanen et al., 2009, 2012) for the NOx to CO2 ratios multiplied with measured CO2
10 data was used for the correction instead. Where neither measured nor modeled NOx
−1
data was available, the EF(NOx ) was assumed to be 65 g kgfuel which was the median Title Page
value of the measured EF(NOx ) of other ships. The missing NOx data for correction of
Abstract Introduction
the SO2 data was then retrieved with Eq. (3) in combination with the measured CO2

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data. For the calculation of the sulfur fuel content (SFC), it is assumed that all sulfur is Conclusions References

Discussion Paper
15 emitted as SO2 . Hence the SFC is calculated by
P  P  Tables Figures
m(S) M(S) · SO2,ppb SO2,ppb
SFC [%] = = P  = 0.232 P  . (2)
m(fuel) M(C)/0.87 · CO2,ppm CO2,ppm J I

The NOx emission factor in g kg−1fuel

is calculated accordingly in Eq. (3) Most of the NOx J I

emission is in form of NO (Alföldy et al., 2012). Nonetheless, for these calculations the Back Close

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20 molecular mass of NOx is assumed to be the molecular mass of NO2 following IMO

Discussion Paper
guidelines (MEPC, 2008). Full Screen / Esc
P  P 
h i m(NO ) M(NO 2 ) · NO 2,ppb NO 2,ppb
EF(NOx ) g kg−1
2
fuel
= = P  = 3.33 P   (3) Printer-friendly Version
m(fuel) M(C)/0.87 · CO2,ppm CO2,ppm
Interactive Discussion
The specific fuel oil consumption (SFOC) in terms of mass of consumed fuel per ax-
25 ial shaft power is retrieved from the STEAM model (Jalkanen et al., 2009, 2012). It
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corresponds to SFOC data supplied by the engine manufacturer through the IHS Fair-
play World Shipping Encyclopedia (IHS, 2009), corrected for the estimated load from AMTD
the ship speed using correction curves supplied by engine manufacturers. The current
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SFOC value for the measured ship was taken from the STEAM database as a function
5 of the ship’s speed at the time of the measurement. The SFOC data is used for the
calculation of the NOx emission per produced energy EFkWh (NOx ) in Airborne emission
measurements of
EFkWh (NOx )[g kWh−1 ] = EF (NOx ) · SFOC(load).

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(4) individual ships

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The emission factor for particle number EF(PN) P is calculated in Eq. (5) as the sum of J. Beecken et al.
10 the total concentration of the particle number, [PN], with an assumed emission factor
−1
of CO2 of 3.2 kg kgfuel (Hobbs et al., 2000).
P Title Page
−1 [PN]
EF(PN)[particles kgfuel ] = P · EF (CO2 ) (5)
[CO2 ] Abstract Introduction

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For the calculation of the particle mass distribution, the particle density is assumed Conclusions References
−3

Discussion Paper
15 to be 1 g cm . The emission factor for particle mass,
P EF(PM), was then calculated
P Tables Figures
correspondingly to Eq. (5) by substituting [PN] with [PM].
The Geometric Mean Diameter (GMD) and the corresponding Geometric Standard
Deviation (GSD) were calculated for the size-resolved particle number concentrations J I

by J I
P

n · ln Dp
GMD [nm] = and (6) Back Close

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20
N

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Ph 
2 i 1/2 Full Screen / Esc
n · ln Dp − ln (GMD)
GSD [nm] =   . (7)
 
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N
Interactive Discussion
In Eqs. (6) and (7) n is the number concentration in the Channel, N the integrated
number concentration and Dp the particle diameter, i.e. the midpoint of the channel.
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2.3 Calibrations
AMTD
The measurements of volume mixing ratios taken inside the ship plumes are analyzed
relative to the background and therefore offset errors can be neglected. The accuracy 6, 10617–10651, 2013
over the dynamic range of interest was assured by frequent calibrations with standard
5 gases, obtained from AGA and Air Liquide with mixing accuracies for CO2 of 1 % and Airborne emission
for SO2 and NOx around 5 %. measurements of

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Usually the gases were measured from gas cylinders containing about 204 ppb NOx , individual ships

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401 and 407 ppb SO2 as well as 370.5 and 410.6 ppm CO2 , respectively. During the last
campaign, a standard Thermo 146i Dynamic Gas Calibrator was used instead together J. Beecken et al.
10 with a Thermo 1160 Zero Air Supply, mixing highly concentrated SO2 and NOx , both
at 60 ppm, with filtered zero air. Mixing ratios of 400 ppb for SO2 and 300 ppb for NOx
were used for calibration with the dynamic gas calibrator. The results were used to Title Page

calculate a time series of respective calibration factors and offsets which in turn were Abstract Introduction
used to post calibrate the plume measurements.

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15 The calibrations were usually carried out on the ground before and after the mea- Conclusions References

Discussion Paper
surement flights. The average precision of the measurements of the calibration gases
Tables Figures
was found to be negligible small for CO2 , 1.6 % for SO2 and 0.5 % for NOx .
The calibration factors that were applied to the measured values are linear inter-
J I
polated values from the nearest calibrations. The estimated interpolation error is the
20 average of the standard deviations between adjacent calibration factors. This yields J I
0.1 % for CO2 , 5.4 % for SO2 and 6.3 % for NOx .
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2.4 Uncertainties

Discussion Paper
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The plumes of 158 different ships have been analyzed. Some ships were repeatedly
measured on different occasions so in total 174 plumes were analyzed. The plumes Printer-friendly Version

25 were usually traversed several times for each occasion to improve the statistical va- Interactive Discussion
lidity of the measurements. An average of the precision for all measurements was
calculated as the median value of the individual 1-σ uncertainties of the respective
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emission factors for plumes that were traversed at least three times. For the calculated
emission factors of SO2 and NOx in g kg−1 fuel
this yields measurement precisions of 18.8 AMTD
and 22.4 % respectively.
6, 10617–10651, 2013
The overall uncertainties of the emission factors are calculated as the square root
5 of the sum of all squared uncertainties due to calibrations and measurements for the
respective gas species and CO2 . Hence, adding the square root of the quadratic sums Airborne emission
for the SO2 emission factor this yields a total uncertainty of 20.3 % and correspondingly measurements of

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23.8 % for the NOx emission factor in g kg−1 fuel
. These uncertainties are comparable the individual ships

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uncertainties of land-based measurements by Alföldy et al. (2012) who found values
J. Beecken et al.
10 of 23 % and 26 % for the emission factors of SO2 and NOx respectively. This could be
explained with repeated measurements of the specific plumes by repeated traverses
with the aircrafts, though the sampling period is shorter as compared to land-based
Title Page
measurements.
In a recent study by Balzani et al. (2013) it is reported that about 14 % of the fuel sul- Abstract Introduction
fur content was not emitted as SO2 for measurements using sniffer technique. Hence,

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15
Conclusions References
the overall error is 20.3 % for SO2 with a possible systematic negative bias of 14 %.

Discussion Paper
An additional uncertainty for NOx with regard to the IMO regulation, is the fact that the Tables Figures
−1
emission factors are usually reported in g kWh , which requires a multiplication with
the SFOC. Here, the uncertainty was estimated to be 11 %, assuming the real operation J I
20 deviates from the test bed measurements of the SFOC. This estimation bases on the
average deviation over the range of the SFOC values in the used model database. J I
−1
Thus the total uncertainty for the NOx emission factor in g kWh is added to 26.2 %. Back Close

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A quantification of the uncertainties for the particle measurements has not been
performed at this stage.

Discussion Paper
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25 2.5 Measurement campaigns Printer-friendly Version

The results of four airborne measurements campaigns which were conducted in the Interactive Discussion
years 2011 and 2012 are discussed in this paper. The flights were conducted from

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airports in Roskilde (Denmark), Kiel (Germany) and Ostend (Belgium). A summary of
the presented measurement campaigns is given in Table 1. The measurements were AMTD
made on 25 days within these periods. The campaigns covered different European sea
6, 10617–10651, 2013
areas amongst those the English Channel and the German Bight, but in particular the
5 western Baltic Sea. A map of the monitored regions is shown in Fig. 2.
The measurements were conducted from airplanes, Piper PA31 and Parte- Airborne emission
navia P68B, and a helicopter of type Eurocopter AS365 Dauphin. The choice of in- measurements of

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strumentation depended on the loading possibilities of the respective airborne vehicle. individual ships

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Inlet probes for gas measurements were sited beneath (Piper PA31) or on the side of
J. Beecken et al.
10 the fuselage (Partenavia P68B and Dauphin helicopter) of the aircraft. The Partenavia
was already equipped with an isokinetic inlet which was used for particulate matter
measurements. The particle inlet on the Dauphin was mounted beside the gas inlet,
Title Page
with some distance from the fuselage to minimize effects due to the downwash of the
main rotor. The minimum instrumental setup used during all campaigns consisted of Abstract Introduction
15 a flight modified Picarro G-2301 and a Thermo 43i-TLE for CO2 and SO2 measure-

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Conclusions References
ments, respectively. NOx was measured with the Thermo 42i-TL during all except the

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first campaign. The particle size distributions were measured with the EEPS onboard Tables Figures
the Partenavia airplane and the Dauphin helicopter. A brief overview of the instrumen-
tal setup on each campaign is presented in Table 2. The Partenavia is shown together J I
20 with the rack mounted instrumental setup in Fig. 3.
J I
2.6 Flight procedure during measurements
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The aim of the IGPS project is to relate the measured emission plumes to individual

Discussion Paper
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ships. Therefore it is necessary to identify and locate the ships in the area surround-
ing the measurement. Ships from a certain size and upward are obliged to frequently
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25 broadcast their status by the Automatic Identification System (AIS) which was received
and logged during the measurement flights. This signal contains the ship identification Interactive Discussion
number and name, its position, course and speed and further information. Together
with information about the position of the aircraft and meteorological information, the
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source of an emission plume can be identified and connected to the determined emis-
sion parameters. AMTD
The flights took place above open waters with dense ship traffic. The AIS data was
6, 10617–10651, 2013
used for the selection and localization of the ships to be observed. Additionally, the AIS
5 data contains information about the course and speed of the ship. Together with mete-
orological information about current wind speeds and directions the plume position with Airborne emission
respect to the ship can be calculated according to Berg et al. (2012). The AIS data is measurements of

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presented on the operators screen like the example in Fig. 4 so ships can be selected individual ships

Discussion Paper
before plume measurement and plumes can literally be related to them on the fly.
J. Beecken et al.
10 The plume height is usually between 50 and 70 m. The aircraft traverses the plume in
these heights in a zigzag shaped manner. So the emission of several transects through
the plume of a ship can be measured. The distance from the ship for these manoeuvers
Title Page
is between 25 to 10 km. Ideally, the procedure begins at further distance from the ship
and the ship is approached with each new transect. Abstract Introduction

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Conclusions References

Discussion Paper
15 3 Results
Tables Figures
Here the overall results of the measured ships are presented and discussed. Results
for individual measurements can be found as Supplement to this article. J I

J I
3.1 SO2 emission factors
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The distribution of the number of the observed ships over their SO2 emission factor is

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shown in the histogram in Fig. 5. The maximum of the distribution is found at 20 g kg−1

Discussion Paper
20 Full Screen / Esc
fuel
The first and the third quartile of the SO2 emission factors in the histogram are 15.8
and 21.9 g kg−1
fuel
. This is reasonable because the IMO limit for sulfur in the fuel of ships Printer-friendly Version

in the observed region is 1 % which corresponds to 20 g kg−1 .

Hence, this maximum
fuel Interactive Discussion
was expected as measurements were taken mostly from commercially driven cargo,
25 tanker and passenger vessels that were assumed for economic reasons to generally
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run close to the sulfur limit. Hence, a sharp decrease in the number of ships with SO2
emission factors higher than 20 g kg−1fuel
can be seen. AMTD
Yet, the SO2 emission factors of four of the analyzed 174 ship plumes are between
6, 10617–10651, 2013
40 and 44 g kg−1
fuel
. Two of these plumes originated from a fast Ro-Pax ferry which was
5 observed on two different days during the campaign in Roskilde in 2011 – 15 June and
−1 Airborne emission
29 June with SO2 emission factors 42.4 and 40.7 g kgfuel respectively. The other two
plumes with exceptionally high emission factors were emitted from a crude oil tanker measurements of

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and a cargo ship. Considering the uncertainty in the measurements of 20 % it can be individual ships

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found that 85 % of all monitored ships would comply with the sulfur limit of 1 %. Not
J. Beecken et al.
10 considering a systematic bias of 14 % for sulfur that is emitted in other forms than
SO2 , as mentioned in the uncertainty analysis. The results of flight campaigns over
North and Baltic Sea conducted between 2007 and 2009 are shown in the inset in Title Page
Fig. 5 (Berg, 2011; Mellqvist and Berg, 2010, 2013). The overall distribution of the SO2
emission factor was 18 % higher as compared to the distribution found in this study. Abstract Introduction
The reason is that in 2010 the IMO changed the limit for the amount of sulfur in fuel in

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15
Conclusions References
the North and Baltic Sea from 1.5 to 1 %.

Discussion Paper
Tables Figures
3.2 NOx emission factors
J I
NOx emissions were measured for 87 different vessels on 91 different occasions. The
distribution of the number of analyzed ship plumes over NOx emission factors is shown J I
20 in Fig. 6. Most ship plumes emit around 70 g kg−1
fuel
of NOx . The first and third quartiles
−1 Back Close

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are 51.9 and 76.1 g kgfuel . The average NOx emission factor related to the produced en-
−1 −1

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ergy is 13.1 g kWh with respective first and third quartiles of 10.4 and 15.2 g kWh Full Screen / Esc

for the measured plumes. In Table 3, the NOx emission factors are presented for differ-
−1 Printer-friendly Version
ent crankshaft speeds. The highest emission factors with an average of 13.6 g kWh
25 were measured at slower engine speeds with a significant difference to emissions at Interactive Discussion
engine speeds above 500 rpm. For a ship running close to its design speed, which is
typically the case in this study, a difference between the instantaneous emission factor
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and the IMO curve is foreseen for the ships. For instance a typical slow speed, Wärt-
silä engine has 15.8 g kWh−1 at 75 % load while the NOx weighted IMO value here is AMTD
3 % lower (Tadeusz Borkowski, personal communication, 9 June 2013). For measure-
6, 10617–10651, 2013
ments of ships in harbors running at 25 % load this discrepancy becomes much larger.
5 However, considering the instantaneous emissions that were evaluated for this study,
the tier 1 limit would apply to 58 % and the tier 2 limit to 7 % of the observed ships. Airborne emission
Summarized it is seen that 95 % of the analyzed ship plumes would comply with the measurements of

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respective NOx limits considering their instantaneous NOx emission figures. individual ships

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3.3 Particle emission factors J. Beecken et al.

10 Size-resolved particle number distributions were measured between 15 and 560 nm

at different distances to the vessel. Concentrations of particles with diameters below Title Page
15 nm were neglected due to high noise that occurred in the lower size channels of the
Abstract Introduction
EEPS. The distributions in the measured size range are mono-modal.

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The averaged particle diameters and emission factors at different distances to the Conclusions References

Discussion Paper
15 emission source are presented in Table 4. The average geometrical mean diameter
Tables Figures
increases from 50 to 62 nm with increased distance. The half width of the distribution
increases from 49 to 61 nm. In addition the emission factor for particle number (PN)
16 −1 J I
decreases with longer distance from 3 to 1×10 particles kgfuel . The strongest gradient
of the emission factor for particle number as function of distance to the ship can be seen J I
20 for distances below 1 km. However, the emission factor for particle mass (PM) does not
change significantly over distance from its average of 2770 mg kg−1 . Back Close

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fuel
A relation between the averages of the emission factors of PN and PM, which

Discussion Paper
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were binned for the corresponding SO2 emission factors from the measurements,
2
can be seen in Fig. 7. The correlations are good with R values of 0.98 for PN and
Printer-friendly Version
25 0.81 for PM. However, standard deviations for both emission factors are in the order
of their averages. For the PN emission factor, the slope of the found regression is Interactive Discussion
(1.1 ± 0.2)×1015 particles g−1 and compares very well with the one that was presented
15 −1
by Alföldy (Alföldy et al., 2012) with corresponding slope p1,Lit = 1 × 10 particles g .
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As the intercept is around zero and the slope is positive it is assumed that the emitted
particles in the measured size range are sulfur based. AMTD
6, 10617–10651, 2013
4 Discussion
Airborne emission
The emission factors sorted for different ship types are presented in Table 5. A com-
measurements of
parison of the found results with other studies is given in Table 6.

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5
individual ships
The majority of the measured emissions originated from passenger ships, cargo

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ships and tankers. The SO2 emission factors of these three types are around J. Beecken et al.
−1
19.0 g kgfuel . Trailing suction hopper dredger vessels show a much lower average SO2
−1
emission factor of 7.4 g kgfuel . Further, the presented emissions were measured from
10 four different ships of this type. So they seem to run on low sulfur fuel in general. This is Title Page

has also been reported for measurements at the harbor of Rotterdam in 2009 (Alföldy Abstract Introduction
et al., 2012). Passenger and cargo ships and tankers are commercially driven, so the

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−1
emission factor of SO2 is around 19 g kgfuel was expected for these types, because all Conclusions References

Discussion Paper
measurements were conducted in regions with a 1 % limit for sulfur content in the fuel.
Tables Figures
15 The NOx emission factors are similar for the different ship types. Although it can be
seen that cargo ships emit at a slightly higher amount of NOx compared to passenger
J I
ships and tankers. This is also described by Williams et al. (2009) for measurements
in the Mexican Gulf, showing that container carriers and passenger ships emit an av- J I
−1
erage of 60 g kgfuel while larger ships such as bulk freight carriers and tanker ships
−1 Back Close
have average NOx emissions of 87 and 79 g kgfuel , respectively. The averaged NOx

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20

emission factors shown in Table 9 are in agreement with ship-borne measurements

Discussion Paper
Full Screen / Esc
carried out by Williams et al. (2009) and Murphy et al. (2009) who describes simulta-
neous airborne and on-board measurements for one ship. Alföldy et al. (2012) made Printer-friendly Version
measurements on the shore side in the ship channel of Rotterdam measuring an av-
−1
25 erage NOx emission factor of 53.7 g kgfuel which they claim is in agreement with the Interactive Discussion
EDGARv4.2 database (European Commission, 2009). This is significantly below the

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values found for the presented flight measurements but can be explained with typically
different engine load conditions in harbors.
16 −1
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The overall average of the PN emission factor is 1.8 ± 1.3 × 10 particles kgfuel and
−1 6, 10617–10651, 2013
for PM it is 2770 ± 1626 mg kgfuel . These values match very well of other studies on
5 ship emissions (Alföldy et al., 2012; Chen et al., 2005; Jonsson et al., 2011; Lack et al.,
2009; Moldanova et al., 2009; Murphy et al., 2009; Petzold et al., 2008, 2010; Sinha Airborne emission
et al., 2003). Closer to ships typical measured particle concentrations are in the order measurements of

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11 −3 individual ships
of 1 × 10 particles cm so a significant amount of particles would coagulate (Hinds,

Discussion Paper
1999; Willeke and Baron, 1993). Hence coagulation is assumed to be the dominant
J. Beecken et al.
10 process for the decrease seen in the PN emission factor with distance while the PM
emission factor remained stable.
The PN and PM emission factors of the observed passenger ships are at the lower Title Page
limit, whereas cargo ships and tankers show significantly higher emissions. Although
only five plumes of four different passenger ships were analyzed for particulate matter Abstract Introduction
emission factors, it appears that passenger ships emit about half as many particles as

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15
Conclusions References
other ship types. The plumes of the passenger ships were traversed even up to several

Discussion Paper
kilometers away from the ship and the precision is comparatively high. Hence, this Tables Figures
indicates that the PN emission factor of passenger ships generally is small compared
to other types. J I

J I
20 5 Summary and conclusions
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Airborne in-situ measurements of 174 ship plumes from 158 different ships at open

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sea were analyzed for this study. The emission factors of SO2 , NOx and particles with
particle diameters between 15 and 560 nm are presented.
−1 Printer-friendly Version
The average SO2 emission factor is 18.8 ± 6.5 g kgfuel . This corresponds to a sulfur
25 fuel content of around 1 %, which was found for most of the studied ship plumes. The Interactive Discussion
results show that 85 % of the monitored ships comply with the limits that were defined
by the IMO for sulfur content in the observed sea regions. By comparison with earlier
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studies (Berg, 2011; Mellqvist and Berg, 2010, 2013) a reduction of the SO2 emission
factors after the reduction of the sulfur limit in 2010 was observed.
−1
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The average of the engine dependent emission of NOx is 66.6 ± 23.4 g kgfuel . This
6, 10617–10651, 2013
compares very well to earlier studies conducted from measurement platforms on land,
5 water and in the air.
The particle emission factors were presented relative to consumed fuel and engine Airborne emission
power. The PN emission factors decrease with the distance to the plume while the parti- measurements of

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cle diameters increase which was assumed to be due to coagulation. A strong gradient individual ships

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was found for distances up to 1 km. A correlation between average sulfur and particle
J. Beecken et al.
10 emissions was found, although the standard deviation for individual measurements is
very high.
The uncertainty for the SO2 and NOx emissions in g kg−1 fuel
is respectively 20 % and
Title Page
24 % and is comparable to the results of a land-based study (Alföldy et al., 2012). With
this level of uncertainty the developed system can be used for the identification of gross Abstract Introduction
15 polluting ships from airborne platforms. By using aircrafts as operation platforms, the

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Conclusions References
limitation of monitoring ships from stationary land-based sites becomes obsolete. Fur-

Discussion Paper
ther, numerous ships can be reached and controlled within in a short time, especially Tables Figures
when they are making way at open sea. Another benefit of a moving over a station-
ary platform is that a changing wind direction is less critical as the flight path can be J I
20 adapted to the direction of the plume. The main drawback in using airplanes is the very
short time in which a plume is traversed at each transect, because a better averaging J I
could be achieved with longer sampling times for the plumes. On the other hand sam-
Back Close
ples can be taken repeatedly with aircrafts. It is noteworthy that with measurements

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from aircrafts particles of the same plume can be sampled at different distances.

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Full Screen / Esc
25 The system is presently installed more permanently in the mentioned Navajo Piper
aircraft for compliance monitoring. New flight measurements will be carried out, using Printer-friendly Version
also two optical devices.
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Supplementary material related to this article is available online at
http://www.atmos-meas-tech-discuss.net/6/10617/2013/ AMTD
amtd-6-10617-2013-supplement.pdf.
6, 10617–10651, 2013

Acknowledgements. The Swedish innovation agency Vinnova and the Swedish Environmental Airborne emission
5 Protection agency are acknowledged for financial support for the development of the IGPS
measurement system and for carrying out the flight campaign through the projects IGPS-2005-
measurements of

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01835 and IGPS-plius-2008-03884. The Belgian DG environment (Directorate-General for the individual ships

Discussion Paper
Environment of the Federal Public Service Health, Food Chain Safety and Environment) is
J. Beecken et al.
thanked for providing support for the helicopter flights. We also acknowledge the assistance
10 obtained from the helicopter provider NHV. We thank Gisela Carvajal for wind data and Tadeusz
Borkowski for providing typical ship engine data.
Title Page

Abstract Introduction
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Table 1. Description of the airborne measurement campaigns. Measurement flights were con-
ducted on 25 days within these periods. Title Page

Period Airport location Monitored sea area Aircraft Measured substances Abstract Introduction

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10–23 Jun 2011 Roskilde (DK) Western Baltic Sea Piper PA31 CO2 , SO2
Conclusions References
28 Sep–2 Oct 2011 Kiel (D) Western Baltic Sea, Partenavia P68B CO2 , SO2 , NOx , PN, PM

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German Bight
30 May–1 Jun 2012 Ostend (B) English Channel Eurocopter AS365 CO2 , SO2 , NOx , PN, PM Tables Figures
Dauphin
28 Aug–6 Sep 2012 Roskilde (DK) Western Baltic Sea Piper PA31 CO2 , SO2 , NOx
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Table 2. Overview on instrumentation used on the different campaigns.

Parameter Platform Instrument Method Rise/fall time Sampling rate Title Page
Carbon Dioxide Piper PA31 Picarro G2301 Cavity ring-down < 1s 1 Hz/2 Hz
(CO2 ) Partenavia P68B spectroscopy Abstract Introduction
Dauphin

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Sulfur Dioxide Piper PA31 Thermo 43i-TLE Fluorescence 2s 1 Hz Conclusions References

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(SO2 ) Partenavia P68B (modified)
Dauphin Tables Figures
Nitrogen Oxides Partenavia P68B Thermo 42i-TL Chemiluminescence < 1s 1 Hz
(NOx ) Dauphin (modified)
Partcile size Partenavia P68B TSI 3090 Electrical mobility 0.5 s 10 Hz J I
distribution Dauphin
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Table 3. NOx emissions in relation to the rated engine speed of the ships. In total 91 plumes
were analyzed. In this table, ships going on 2-stroke engines are found below 300 rpm. Ships
with higher rated engine speeds were going with 4-stroke engines. In order to see if NOx emis-
Title Page
sions are exceeding the IMO limits, the measurement uncertainty was considered. It should be
considered that in contrast to IMO regulation the measurements only show the instantaneous
Abstract Introduction
emission.

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Conclusions References
Rated engine speed Average EF(NOx ) Average EF(NOx ) Number of plumes Number of plumes

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[rpm] [g kWh−1 ] [g kg−1
fuel
] exceeding IMO limits Tables Figures
0 . . . 300 13.6 ± 5.3 71.3 ± 28.3 44 3
300 . . . 500 13.8 ± 2.4 67.9 ± 10.4 18 –
500 . . . 1000 12.0 ± 3.7 59.7 ± 18.3 28 2 J I
1000 . . . 3000 5.2 26.1 1 –
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Table 4. The Geometric Mean Diameter (GMD), Geometric Standard Deviation (GSD) and
Full Width at Half Maximum (FWHM) as well as the emission factors for particle number and
mass are shown. GMD GSD and FWHM are related to the number weighted concentrations.
Title Page
The values were averaged for intervals of the distance to ship at the moment the plume was
traversed. Distances were retrieved for 202 transects. Abstract Introduction

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Distance to ship GMD GSD FWHM EF(PN) EF(PM) Number of
Conclusions References
[km] [nm] [nm] [nm] [1016 kg−1 ] [mg kg−1 ] plume transects

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fuel fuel

0 . . . 0.5 44.8 ± 7.6 1.5 ± 0.1 42.8 ± 10.3 2.91 ± 1.59 2533 ± 1302 80 Tables Figures
0.5 . . . 1 49.1 ± 15.7 1.4 ± 0.3 48.1 ± 15.9 2.41 ± 1.36 2947 ± 1762 32
1... 2 51.4 ± 17.2 1.4 ± 0.4 49.5 ± 18.6 1.37 ± 1.05 3118 ± 5481 40
2... 5 52.0 ± 18.8 1.3 ± 0.4 51.5 ± 22.2 0.99 ± 0.48 2078 ± 1673 31 J I
5... 8 53.4 ± 17.9 1.4 ± 0.4 52.1 ± 16.4 1.04 ± 0.67 2140 ± 1292 14
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Table 5. Emission factors of SO2 , NOx and particulate matter emissions for different ship types.
The presented numbers are the mean values and standard deviations for each ship type of
the average for each plume over several transects. The number in brackets is the number of
Title Page
plumes that have been traversed. The same ships may appear twice if they were measured on
several occasions. Abstract Introduction

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Ship type EF(SO2 ) EF(NOx ) EF(NOx ) EF(PM) EF(PN)
−1
[g kgfuel ]
−1
[g kgfuel ]
−1
[g kWh ]
−1
[mg kgfuel ]
16 −1
[10 kgfuel ] Conclusions References

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Passenger 19.1 ± 7.2 (34) 62.0 ± 19.3 (17) 11.9 ± 3.7 (17) 1680 ± 438 (5) 0.91 ± 0.18 (5)
Cargo 18.9 ± 6.2 (80) 70.3 ± 25.4 (45) 13.9 ± 4.8 (45) 3066 ± 1665 (37) 1.90 ± 1.31 (37)
Tables Figures
Tanker 19.2 ± 5.8 (54) 65.4 ± 22.7 (24) 12.5 ± 4.2 (24) 2271 ± 875 (16) 2.01 ± 1.41 (16)
Trailing suction hopper dredger 7.4 ± 8.0 (4) 65.7 ± 5.6 (3) 14.3 ± 1.7 (3) 1725 ± 870 (3) 1.43 ± 0.21 (3)
Unspecified 23.2 ± 3.6 (2) 36.2 ± 14.2 (2) 8.0 ± 3.9 (2) 8362 (1) 1.79 (1) J I
All types 18.8 ± 6.5 (174) 66.6 ± 23.4 (91) 13.1 ± 4.4 (91) 2770 ± 1626 (62) 1.82 ± 1.26 (62)
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Table 6. Comparison of the emission factors found in this study with literature.

Reference EF(SO2 ) EF(NOx ) EF(NOx ) EF(PM) EF(PN) Number of Location

Airborne emission
(platform) g kg−1 g kg−1 g kWh−1 g kg−1 1016 kg−1 Ships (Year) measurements of

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fuel fuel fuel fuel

This study 18.8 ± 6.5 66.6 ± 23.4 13.1 ± 4.4 2.8 ± 1.6 1.8 ± 1.3 174 Open sea, individual ships

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(airborne) (2011/2012)
a a a
Sinha (2003) 2.9 ± 0.2 22.3 ± 1.1 4.0 ± 0.4 2 Open sea J. Beecken et al.
(airborne) 52.2 ± 3.7b 65.5 ± 3.3b 6.2 ± 0.6b (2000)
Chen (2005) 30 ± 4 20 ± 8 4.6 ± 1.4 2 Open sea
(airborne) 23 ± 7 13 ± 8 4.5 ± 1.8 (2002)
Petzold (2008) 1.36 ± 0.24 1 Open sea
Title Page
(airborne/on board) (2004)
Moldanova (2009) 39.3 73.4 14.2 5.3 1 Open Sea
(on board) (2007) Abstract Introduction
c
Murphy (2009) 59.7 ± 0.5 65.7 ± 0.3 20.1 ± 0.1 1.3 ± 0.2 1 Open Sea

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(airborne/on board) (2007) Conclusions References
Williams (2009)d 13.2 ± 10.4 66.4 ± 9.1

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> 200 Open sea
(ship borne) (2006)
e e e Tables Figures
Lack (2010) 49 ± 7.5 3.77 ± 1.3 1.0 ± 0.2 1 Open sea
(airborne) 4.3 ± 0.6f 0.39 ± 0.14f 1.4 ± 0.2f (2004)
Petzold (2010) 3.4 ± 1.3 1 Test rig,
J I
(test-bed, stack) 85–100 % load
Jonsson (2011) 2.05 ± 0.11 2.55 ± 0.11 734 Harbor
(land-based) (2010) J I
a a
Alföldy (2012) 6 53.7 0.8 497 Harbor
(land-based) 14 . . . 18b 1.8b (2009) Back Close

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a
Distillate fuel.

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b
Residual oil. Full Screen / Esc
c
Calculated from known SFC.
d
Averaged data, only moving ships.
e
Before fuel switch to low sulfur fuel.
f
After fuel switch to low sulfur fuel. Printer-friendly Version

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Airborne emission
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J. Beecken et al.

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Abstract Introduction

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Conclusions References

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Fig. 1. Example of a plume transect measurement. The volume mixing ratios of CO2 , SO2

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and NOx are measured. The presented total concentration, TC(PN) of particles is calculated
from the measurement of the particle number over size distribution. The volume mixing ratios
and particle concentration above the respective baselines (black line) are summed along the Printer-friendly Version
transect path. The ratio of the areas (light grey) for SO2 , NOx and TC(PN) to CO2 is proportional
to the respective emission factor expressed in g kg−1 fuel
and particles kg−1
fuel
, respectively. Interactive Discussion

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J. Beecken et al.

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Conclusions References

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Fig. 2. Map showing the flight tracks over the monitored sea regions for the different measure-
ment campaigns; Roskilde (10–23 June 2011), Kiel (28 September–2 October 2011), Ostend
(30 May–1 June 2012) and Roskilde (28 August–6 September 2012). Printer-friendly Version

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Conclusions References

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Fig. 3. Instruments, mounted in racks, for ready installation in the Partenavia P68B airplane

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behind. The particle inlet can be seen on top of the fuselage (picture taken by B. Schneider,

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enviscope GmbH).
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Conclusions References

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Tables Figures

J I

Fig. 4. Map for real-time navigation purpose that is presented to the operator by the IGPS J I
software showing the current locations of surrounding ships and aircraft from the received
Automatic Identification System (AIS) data sent by the ships. The different size of the ships Back Close

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corresponds to their Gross Tonnage. The blue circles around the aircraft’s location indicate the

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distance to the ships and the time to reach these. The two white circles give information about
the ships’ locations relative to the aircraft with respect to north and the current course of the
aircraft respectively. Printer-friendly Version

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Fig. 5. Histogram of the emission factor of SO2 , EF(SO2 ), from airborne measurements for
four campaigns in the years 2011 and 2012. The inset shows according results from earlier Printer-friendly Version
campaigns between 2007 and 2009. The comparison indicates a reduction of EF(SO2 ). This
coincides with the reduction of the limit of sulfer in fuel to 1 %. The corresping values for the Interactive Discussion
sulfur fuel content can be optained by dividing the EF(SO2 ) by 20.

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Fig. 6. Histogram of the NOx emission factor, EF(NOx ), relative to the amount of consumed fuel Printer-friendly Version
from airborne measurements for three campaigns in the years 2011 and 2012.
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Fig. 7. Emission factors of particle number (PN) and particle mass (PM) related to the SO2
emission factor. The results were binned for the SO2 emission factor. The ticks on the x-axis Printer-friendly Version
correspond to the bin edges. The numbers in square brackets indicate the number of individual
plume transects distributed for different SO2 emission factors. The square-shaped markers Interactive Discussion
indicate the values which were taken into account for the calculation of the linear regressions.

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 Airborne Emission Measurements of SO2, NOx and
Particles from Individual Ships using Sniffer Technique

- Supplementary Material -

J. Beecken1, J. Mellqvist1, K. Salo1, J. Ekholm1 and J.-P. Jalkanen2

[1]Chalmers University of Technology, Earth and Space Sciences, Gothenburg, Sweden

[2]Finnish Meteorological Institute, Helsinki, Finland

Correspondence to: J. Beecken (beecken@chalmers.se)

NOx Source
Number
mean EF(SO2) mean EF(NOx) (0:measurement, SOG
IMO Date of
[g/kg_fuel] ± [%] [g/kg_fuel] ± [%] 1:STEAM, [kn]
traverses
2:default)

7016474 29 September 2011 3.33 ± 0.00 7.04 ± 0.00 0 1

7225922 30 September 2011 22.86 ± 4.36 73.52 ± 24.06 0 10.0 2

7360162 11 June 2011 1.88 ± 0.00 55.82 ± 0.00 1 12.5 1

7420223 30 May 2012 3.14 ± 53.87 65.68 ± 36.38 0 10.6 3

7500451 30 May 2012 26.84 ± 21.29 44.13 ± 28.91 0 7

7637448 30 May 2012 2.95 ± 121.12 66.96 ± 35.28 0 12.2 8

7703259 15 June 2011 10.15 ± 0.00 57.77 ± 0.00 1 9.6 1

7721249 28 June 2011 11.32 ± 36.64 80.04 ± 0.21 1 12.2 4

7803190 13 June 2011 19.17 ± 0.10 63.24 ± 0.00 1 19.0 2

7928158 30 September 2011 25.73 ± 0.00 46.26 ± 0.00 0 8.6 1

8020599 29 June 2011 20.64 ± 22.21 66.93 ± 0.00 1 16.3 3

8131893 04 September 2012 32.87 ± 26.23 46.00 ± 12.66 0 8.2 4

8202381 30 May 2012 19.01 ± 7.34 113.36 ± 16.58 0 13.1 6

8207795 31 May 2012 22.28 ± 6.14 93.87 ± 6.25 0 13.2 4

8225498 11 June 2011 17.30 ± 26.96 79.20 ± 0.31 1 11.9 4

8302246 31 August 2012 16.74 ± 0.00 93.95 ± 0.00 1 14.6 1

8306981 29 September 2011 23.47 ± 16.28 69.61 ± 40.64 0 11.7 4

8312057 29 June 2011 14.86 ± 24.25 91.86 ± 0.63 1 12.3 6

8312100 11 June 2011 11.38 ± 0.00 81.84 ± 0.00 1 10.5 1

8401444 10 June 2011 14.29 ± 21.12 69.81 ± 0.21 1 17.6 2

8422034 15 June 2011 19.22 ± 0.00 63.33 ± 0.00 1 12.3 1

8512401 29 June 2011 16.58 ± 40.91 96.14 ± 1.17 1 17.9 10

8521804 30 September 2011 27.80 ± 57.76 55.81 ± 67.03 1 16.1 4

8608195 30 September 2011 25.05 ± 5.03 95.34 ± 15.92 0 3

8618358 04 September 2012 21.32 ± 21.48 69.78 ± 22.65 0 14.1 7

8618358 06 September 2012 15.92 ± 20.72 101.62 ± 29.57 0 16.8 2

8703232 13 June 2011 18.78 ± 0.00 71.78 ± 0.00 1 17.5 1

8705383 29 June 2011 16.25 ± 0.00 72.30 ± 0.00 1 16.3 1

8903155 13 June 2011 19.69 ± 0.00 72.42 ± 0.00 1 15.0 1

8917596 29 August 2012 16.26 ± 22.39 78.98 ± 3.85 0 15.8 3

8993887 02 October 2011 20.62 ± 0.00 26.12 ± 0.00 0 1

9010163 15 June 2011 19.88 ± 15.00 72.43 ± 1.69 1 17.5 4

9010163 29 June 2011 26.42 ± 93.88 70.90 ± 3.21 1 16.6 2

9010163 05 September 2012 16.58 ± 6.29 64.94 ± 12.40 0 17.1 3

9010917 15 June 2011 27.88 ± 0.00 66.19 ± 0.00 1 14.1 1

9016923 15 June 2011 20.37 ± 0.00 64.57 ± 0.00 1 11.9 1

9031260 28 September 2011 8.68 ± 87.54 34.19 ± 76.40 1 9.6 3

9046368 29 August 2012 16.17 ± 7.09 74.39 ± 12.00 0 13.2 3

9073086 01 June 2012 23.63 ± 26.63 48.77 ± 44.99 0 7.3 7

9077587 01 October 2011 21.28 ± 14.91 58.59 ± 12.99 0 10.8 3

9082879 01 October 2011 19.47 ± 27.77 74.94 ± 26.29 0 13.0 5

9104902 29 September 2011 -0.59 ± 84.55 83.68 ± 0.20 1 15.2 2

9106986 31 May 2012 40.55 ± 17.96 70.59 ± 1.20 1 9.1 6

9114737 30 September 2011 2.80 ± 139.93 22.80 ± 133.41 1 10.1 3

9115975 28 September 2011 13.69 ± 0.00 51.23 ± 0.00 0 11.7 1

9124471 01 June 2012 24.85 ± 11.42 55.89 ± 17.65 0 4

9131797 13 June 2011 19.03 ± 13.47 72.37 ± 0.00 1 15.1 3

9131797 27 June 2011 8.54 ± 0.00 72.37 ± 0.00 1 15.3 1

9131797 28 August 2012 18.63 ± 15.27 65.36 ± 22.49 0 15.4 4

9131797 06 September 2012 21.97 ± 3.57 66.97 ± 8.04 0 16.3 2

9133915 01 September 2012 17.61 ± 13.49 56.53 ± 9.10 0 16.1 4

9137997 04 September 2012 16.93 ± 9.65 52.45 ± 24.93 0 18.0 4

9144419 31 August 2012 14.54 ± 19.43 70.52 ± 0.14 1 14.7 4

9144512 05 September 2012 21.38 ± 0.00 69.38 ± 0.00 0 10.9 1

9158458 13 June 2011 20.64 ± 0.00 65.00 ± 0.00 2 1

9166845 01 June 2012 19.17 ± 15.15 70.54 ± 14.04 0 5.7 4

9168946 02 October 2011 13.75 ± 7.52 20.72 ± 13.76 0 0.4 2

9173329 30 June 2011 15.82 ± 0.00 67.09 ± 0.00 1 15.6 1

9177959 01 June 2012 21.83 ± 31.05 63.81 ± 26.72 0 13.9 4

9181077 01 September 2012 13.61 ± 0.00 73.23 ± 0.00 0 18.1 1

9182368 30 May 2012 25.13 ± 28.89 160.86 ± 24.95 0 17.1 5

9184029 01 June 2012 22.84 ± 34.10 79.67 ± 19.27 0 17.5 4

9187916 13 June 2011 18.05 ± 0.00 61.41 ± 0.00 1 11.9 1

9187916 28 September 2011 26.31 ± 19.52 74.01 ± 46.77 0 13.9 2

9188427 10 June 2011 12.98 ± 0.00 71.27 ± 0.00 1 19.4 1

9188518 03 September 2012 14.24 ± 9.97 49.93 ± 1.76 0 17.5 2

9194000 13 June 2011 17.24 ± 9.99 65.00 ± 0.00 2 4

9194012 13 June 2011 18.75 ± 18.08 65.00 ± 0.00 2 2

9194074 30 September 2011 22.70 ± 11.92 97.84 ± 25.57 0 11.9 4

9197521 31 August 2012 18.78 ± 7.47 66.93 ± 0.00 1 14.9 2

9198941 15 June 2011 42.42 ± 31.34 68.81 ± 0.23 1 17.3 3

9198941 29 June 2011 40.69 ± 12.51 76.92 ± 0.01 1 23.4 5

9202546 06 September 2012 21.94 ± 0.00 77.45 ± 0.00 0 15.3 1

9205964 31 May 2012 27.69 ± 5.28 61.79 ± 63.66 0 19.3 3

9207883 06 September 2012 17.15 ± 0.00 77.60 ± 0.00 0 18.1 1

9212589 11 June 2011 16.75 ± 0.00 64.85 ± 0.00 1 12.9 1

9217230 03 September 2012 20.51 ± 22.85 65.30 ± 20.65 0 16.3 9

9217230 06 September 2012 21.69 ± 0.62 69.21 ± 13.24 0 17.1 2

9217242 15 June 2011 17.36 ± 9.50 78.86 ± 0.00 1 18.1 2

9217242 27 June 2011 15.27 ± 0.00 78.85 ± 0.00 1 18.3 1

9217242 03 September 2012 16.84 ± 11.29 48.90 ± 10.65 0 17.2 6

9218014 31 May 2012 28.51 ± 8.47 60.63 ± 19.48 0 16.0 7

9222118 02 October 2011 8.07 ± 62.49 21.95 ± 28.82 0 7.4 2

9227326 31 May 2012 23.49 ± 8.68 83.34 ± 0.44 1 16.4 6

9230098 04 September 2012 21.31 ± 0.00 55.69 ± 0.00 0 1

9231846 30 September 2011 17.87 ± 16.49 38.47 ± 34.96 0 3

9233234 29 August 2012 26.95 ± 22.11 51.75 ± 14.07 0 10.4 3

9235892 16 June 2011 11.24 ± 19.52 74.44 ± 0.00 1 16.2 2

9244192 28 September 2011 19.03 ± 73.11 68.52 ± 10.55 1 15.7 4

9244295 01 October 2011 20.18 ± 35.73 28.53 ± 21.58 0 6.8 2

9250373 01 June 2012 5.55 ± 110.40 59.50 ± 59.84 0 10.6 4

9251652 11 June 2011 17.82 ± 0.00 75.64 ± 0.00 1 13.3 1

9256078 01 October 2011 20.31 ± 1.30 76.43 ± 2.81 0 13.6 3

9259599 10 June 2011 12.52 ± 15.55 101.94 ± 0.11 1 12.7 3

9259599 27 June 2011 16.53 ± 0.00 100.50 ± 0.00 1 12.0 1

9261401 01 October 2011 17.33 ± 17.23 58.00 ± 11.30 0 13.8 4

9265756 01 October 2011 22.28 ± 0.00 74.50 ± 0.00 0 1

9266853 13 June 2011 17.69 ± 0.00 104.37 ± 0.00 1 14.4 1

9268837 01 June 2012 21.88 ± 17.32 48.21 ± 14.49 0 10.7 3

9276561 11 June 2011 20.28 ± 0.00 91.47 ± 0.00 1 10.3 1

9276561 30 June 2011 15.06 ± 24.14 101.36 ± 0.19 1 12.9 7

9278234 28 September 2011 20.27 ± 15.47 79.20 ± 22.39 0 18.7 7

9278234 30 September 2011 15.00 ± 24.78 61.92 ± 30.67 0 20.5 4

9286554 31 May 2012 24.86 ± 19.26 68.55 ± 12.86 0 15.4 6

9288722 27 June 2011 15.14 ± 25.45 104.41 ± 0.00 1 14.4 3

9290684 27 June 2011 22.33 ± 0.00 63.53 ± 0.00 1 11.4 1

9290842 02 October 2011 20.99 ± 55.28 89.24 ± 67.35 0 14.4 5

9292101 15 June 2011 14.87 ± 14.42 99.41 ± 0.42 1 14.2 3

9294288 01 June 2012 19.07 ± 36.17 51.02 ± 50.27 0 12.4 5

9296195 31 August 2012 30.34 ± 36.46 65.00 ± 0.00 2 5

9297591 01 October 2011 19.37 ± 0.00 45.44 ± 0.00 0 17.0 1

9299733 01 September 2012 19.49 ± 38.82 77.46 ± 53.70 1 14.5 7

9301926 31 August 2012 13.80 ± 38.59 83.02 ± 0.17 1 15.1 4

9307671 31 August 2012 18.49 ± 30.34 77.15 ± 54.80 0 13.2 5

9312195 15 June 2011 17.32 ± 25.78 72.14 ± 0.30 1 16.7 3

9313216 01 October 2011 17.88 ± 41.25 47.89 ± 44.86 0 6

9317755 31 May 2012 18.59 ± 13.37 98.54 ± 0.18 1 13.1 4

9318486 05 September 2012 21.53 ± 0.00 97.19 ± 0.00 0 15.3 1

9319466 05 September 2012 15.76 ± 16.73 78.89 ± 14.60 0 20.2 4

9320556 28 June 2011 15.57 ± 25.71 78.34 ± 0.01 1 22.9 3

9321677 27 June 2011 15.73 ± 8.52 104.46 ± 0.03 1 15.3 4

9328637 03 September 2012 10.16 ± 0.00 72.57 ± 0.00 0 17.5 1

9332066 31 May 2012 23.60 ± 9.49 99.08 ± 0.15 1 14.2 3

9332157 02 October 2011 16.93 ± 3.14 60.45 ± 15.84 0 10.9 2

9336256 15 June 2011 18.72 ± 0.15 77.38 ± 0.00 1 21.5 2

9336505 30 September 2011 14.76 ± 10.59 110.98 ± 11.21 0 14.9 2

9340453 01 October 2011 22.33 ± 14.65 64.23 ± 17.31 0 14.0 4

9346689 15 June 2011 18.88 ± 0.00 53.51 ± 0.00 1 9.4 1

9349863 29 September 2011 23.43 ± 18.38 63.42 ± 3.84 0 18.6 4

9350721 30 September 2011 22.70 ± 32.51 58.66 ± 38.24 0 17.6 5

9352298 01 September 2012 12.92 ± 84.93 45.77 ± 41.60 0 12.7 5

9363027 31 May 2012 24.06 ± 36.07 111.73 ± 47.29 0 12.6 5

9366287 03 September 2012 18.34 ± 0.00 77.39 ± 0.00 0 13.1 1

9369007 15 June 2011 19.18 ± 3.24 61.82 ± 0.10 1 16.9 2

9376828 04 September 2012 22.72 ± 0.89 133.92 ± 2.04 0 11.3 2

9382190 31 May 2012 19.96 ± 9.07 52.80 ± 0.07 1 11.1 5

9382750 31 May 2012 43.86 ± 5.29 81.62 ± 0.00 1 10.7 5

9384095 16 June 2011 18.80 ± 14.68 73.13 ± 0.00 1 13.5 3

9384095 29 June 2011 14.78 ± 47.33 70.56 ± 0.22 1 12.6 4

9387425 29 June 2011 18.97 ± 6.60 84.60 ± 0.08 1 19.2 2

9388522 31 May 2012 21.12 ± 5.81 57.66 ± 0.60 1 13.4 3

9390305 29 September 2011 15.11 ± 67.93 43.36 ± 9.14 0 12.5 3

9396696 31 August 2012 16.95 ± 28.56 67.71 ± 0.15 1 15.2 4

9398448 02 October 2011 18.78 ± 0.00 53.41 ± 0.00 0 1

9399480 13 June 2011 22.40 ± 26.73 85.56 ± 0.41 1 12.5 4

9406582 11 June 2011 6.26 ± 0.00 53.85 ± 0.00 1 8.5 1

9407093 29 September 2011 27.06 ± 11.01 70.78 ± 69.68 0 3

9413420 15 June 2011 18.07 ± 24.08 84.45 ± 0.00 1 12.8 2

9417799 01 June 2012 21.85 ± 17.61 44.88 ± 4.42 0 13.1 4

9423449 30 June 2011 15.83 ± 18.20 61.37 ± 0.00 1 14.6 9

9430193 06 September 2012 18.93 ± 8.39 62.10 ± 40.70 0 14.3 3

9432220 01 October 2011 21.38 ± 28.24 73.68 ± 21.30 0 15.3 3

9440796 31 May 2012 21.95 ± 14.49 100.13 ± 16.75 0 13.4 5

9440801 01 June 2012 17.80 ± 12.61 39.92 ± 53.40 0 18.0 5

9447902 01 June 2012 22.87 ± 14.71 107.02 ± 56.74 0 4

9448035 06 September 2012 20.44 ± 9.19 57.17 ± 13.62 0 3

9451991 31 May 2012 26.28 ± 9.71 81.14 ± 10.27 0 16.4 7

9458080 02 October 2011 25.07 ± 21.34 57.71 ± 59.72 0 3

9458535 31 August 2012 15.40 ± 0.00 65.00 ± 0.00 2 1

9460241 29 June 2011 19.24 ± 30.71 61.37 ± 0.19 1 13.4 4

9461350 01 October 2011 15.04 ± 30.84 58.73 ± 36.59 0 9.4 5

9466350 31 August 2012 19.53 ± 9.66 76.86 ± 29.41 2 4

9480980 01 June 2012 21.34 ± 28.59 62.19 ± 41.08 0 11.8 4

9483499 31 August 2012 9.66 ± 4.99 65.00 ± 0.00 2 2

9483516 05 September 2012 17.07 ± 8.18 71.79 ± 23.01 0 12.7 2

9511533 13 June 2011 15.08 ± 40.92 88.95 ± 0.43 1 13.6 3

9511533 27 June 2011 18.66 ± 2.84 89.00 ± 0.00 1 15.3 2

9525900 31 May 2012 26.17 ± 8.86 65.00 ± 0.00 2 4

9536935 10 June 2011 17.81 ± 0.00 54.76 ± 0.00 1 13.1 1

9558907 30 September 2011 14.70 ± 0.00 73.69 ± 0.00 0 13.6 1

9567453 16 June 2011 18.75 ± 18.49 85.92 ± 0.24 1 13.1 2

9569994 27 June 2011 17.05 ± 4.94 87.29 ± 0.00 1 13.7 2

9591571 01 October 2011 16.71 ± 15.67 52.49 ± 18.86 0 15.4 3

9592288 31 August 2012 8.51 ± 0.00 48.88 ± 0.00 0 1

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