Abegglen Etal 2016

www.cloudman.
com
Manuel Abegglen, Institute for Atmospheric and Climate Science
Zurich, June 16, 2016
Chemical Characterization of Freshly Emitted

Particulate Matter from Aircraft Exhaust Using
Single Particle Mass Spectrometry
Manuel Abegglen1, Benjamin Brem2,3, Martin Ellenrieder4, Lukas Durdina2,3,

Theo Rindlisbacher5, Jing Wang2,3, Ulrike Lohmann1, Berko Sierau1
1
1 Institute for Atmospheric and Climate Science, ETH Zurich, Switzerland

2 Laboratory for Advanced Analytical Technologies, Empa, Dübendorf, Switzerland
3 Institute of Environmental Engineering, ETH Zurich, Zurich, Switzerland
4 SR Technics, Zurich, Switzerland
5 Swiss Federal Office of Civil Aviation, Bern, Switzerland
Motivation
30 June 2016 Campaigns ATOFMS
IACETH Conclusions
Motivation
• Aircraft exhaust is a unique anthropogenic source of soot inthe
upper troposphere and near airports
• Aircraft exhaust interacts with radiation and clouds
• Contrail cirrus is the largest aviation related net radiative effect
(Burkhardt & Kärcher, 2011)
• Role of soot in ice nucleation is not yet completely understood
(Zhou & Penner, 2014)
• Metal containing particles are a dominant fractionof ice crystal
residuals (Cziczo et al., 2014)
• Air traffic increases ~5 % per year (ICAO, 2013)
Motivation
IACETH Conclusions
The A-PRIDE Campaigns (Aviation Particle Regulatory

Instrumentation Demonstration Experiments)
• Took place at Zurich Airport in the SR Technics facilities

• Measurements during commercial test procedures using the
aircraft engine test cell
• Sampling and non-volatile particulate matter (nvPM)
measurements according to new aircraft engine nvPM
standard
• The system allows the connection of ancillary instruments for
the purpose of emission research
Motivation
IACETH Conclusions
Aircraft Engine in the Test Cell
Motivation
IACETH Conclusions
Experimental Set-Up at the Zurich Airport
ATOFMS
ATOFMS: Aerosol Time-of-Flight Mass Spectrometer
Motivation
IACETH Conclusions
ATOFMS - Aerosol Time-of-Flight Mass Spectrometer
Model TSI 3800-030
Motivation
IACETH Conclusions
ATOFMS – Aerosol Time-of-Flight Mass Spectrometer

The ATOFMS allows the simultaneous measurement of size and chemical
composition of single airborne particle
Chemical properties Mixing state
• Information on refractory (metals, EC)
and non-refractory material (e.g. Internally Externally
sulfate, organics) mixed mixed
• Chemical composition of individual
particles
• Mixing state
• Non-quantitative
Physical property
• Aerodynamic size
Motivation
IACETH Conclusions
ATOFMS Results from a Turbofan engine
Mass spectra
• Typical EC pattern,
Cn peaks: (m/z = 12
* n)
• Only few negative
spectra were
recorded
• The analyzed
particles represent
the fraction of the
largest exhaust
particles
Motivation
IACETH Conclusions
Identification of Major Average Particle Types
Motivation
IACETH Conclusions
10
Cluster 1 (93,4 %): EC-Na-metal
• Clear EC pattern from fresh soot plus some metals: Silicon, Chromium, Iron
Motivation
IACETH Conclusions
11
Metal Detected in Exhaust Particles

• Determination of the particle fraction containing the
individual metals
• Metals detected (abundance, max. value)
• >10 %: i i Sodium, Iron, Calcium and Chromium
• 1 % – 10 %: Silicon, Aluminium, Cobalt, Copper, Molybdenum and
d i Magnesium
• <1 %: Vanadium, Manganese, Nickel, Barium, Titanium and

r Lead (and Zirconium)
Motivation
IACETH Conclusions
12
Results – Trace elements found in fuel and oil

• Inductively coupled plasma mass spectrometry results from jet fuel and
lubricant oil samples (EMPA)
• Quantitative results obtained with inductively coupled plasma mass
spectrometry
Motivation
IACETH Conclusions
13
Thrust dependent occurrence of metals from fuel and oil
• Ba, Na and Ca:

probably decrease
due to higher particle
concentration
• Na and Ca also
show a decrease in
relative peak area
• Pb: probably stems
from contamination
of the fuel tank (only
tiny amount found in
oil)
Motivation
IACETH Conclusions
Results
14
Thrust dependent occurrence of metals probably from

engine wear (used as alloys)
• Co: (not in fuel or oil)
• Fe (fuel and oil) and Cu
(oil):
• Cu occurs always
together with Fe 
probably from engine
wear
• Conc. decreases
with increasing
thrust
• Cr (also in oil)
• Al (also in fuel and oil)
Motivation
IACETH Conclusions
Results
15
Metals found in fuel, oil and used as alloys in aircraft engines
• Vanadium
• Iron: occurs mainly
with copper 
probably from engine
wear
• Molybdenum: occurs
at highest thrust
• Titanium: probably
underestimated
Motivation
IACETH Conclusions
Results
16
Summary and conclusions
• Measurements were conducted on individual, freshly emitted aircraft exhaust

particles considering the entire engine operating range
• First in-line measurements of chemical composition of single particles show
• Almost all particles showed EC pattern
• All detected metals were internally mixed with soot
• 36% of the analyzed particles contained a metallic compound
• Most metals are detected in more than one source (fuel, oil, engine wear)
• Cobalt and Zirconium result only from engine wear
Motivation
IACETH Conclusions
17
Thank you for your attention!
Motivation
IACETH Conclusions
18
Acknowledgements:
This research was made possible by
Swiss Federal Office of Civil Aviation
US Federal Aviation Administration
Financial support
Transport Canada
European Aviation Safety Agency
EMPA
SR Technics crew
Frithjof Siegerist Technical assistance
Theo Rindlisbacher
Adrian Wichser
Motivation
IACETH Conclusions
19
Motivation
Health
• The emitted particles are ultrafine Particulate Matter (PM0.1, mean

diameter <100 nm)
• They are less likely to be removed from human respiratory system
and can even enter the blood stream (Terzano et al., 2010)
• Respiratory health problems occur near airports (Keuken et al., 2015)
• Soot can act as carrier for toxic substances (Janssen et al., 2012)
Motivation
IACETH Conclusions
20
Measurements at the Zurich Airport
Campaign Date CPMA ATOFMS
A-PRIDE 4 November 2012  —
Piggyback June 2013  

A-PRIDE 5 July/June 2013  
A-PRIDE 7 October 2014 — 
Piggyback May 2015 — 
Motivation
IACETH Conclusions
21
SR Technics – Aircraft Engine Test Cell
Diluter box
Sampling Line
Instrumentation
Copyright by SR Technics
Motivation
IACETH Conclusions
22
Experimental setup used in the A-PRIDE 4 campaign
Lobo et al., 2015
Motivation
IACETH Conclusions
23
Size Distribution
• Mean dm increases
Normalized concentration,
with thrust
• Particle concentration
dN/dlogDp [cm−3]
increases with thrust
• Except at low thrust
• Smaller than exhaust
particles emitted by
diesel vehicles (e.g.
Olfert et al., 2007)
Electrical mobility diameter, dm [nm]
Motivation
IACETH Conclusions
24
Results: Size of particles analyzed by the ATOFMS
• dae (ATOFMS) was

converted into dm
SMPS • …using shape
factors calculated
from particle mass
ATOFMS (Abegglen et al, 2015)
•  Only the largest

particles could be
analyzed
Motivation
IACETH Conclusions
Results
25
Cluster 3 (1.8 %): Ca-Al-K-Fe-Na (Metal Type Particle)
• Metals appear in the

positive spectra
• Signature of EC/soot
still obvious
• EC mixed with mainly
inorganic compounds:
• 23Na
• 27Al
• 39K
• 40Ca
• 56Fe
Motivation
IACETH Conclusions
26
Results: Single particle spectra III
• Vanadium and
Vanadium oxide
• Iron was found in
a vast majority (up
to 25 %) of the
particles
• The ATOFMS is
very sensitive to
Potassium
Motivation
IACETH Conclusions
Results
27
Cluster 2 (4.5 %): K-Na-EC

• Very pronounced Potassium peak and Sodium with a weak 12C pattern
Motivation
IACETH Conclusions
Results
28
Results: EC/TC-ratio
1 • Determination of EC/TC
ratio according to
0.99 method by Ferge et al.
(2006) using relative
0.98 peak areas
EC/TC
• Prior subtraction of
0.97 peaks from
inorganic
0.96 compounds
• EC defined as m/z =
0.95 Cx + n (n =1, 2, 3)
3 5 7 21 30 65 85 100 120
• TC defined as rest
Engine Thrust
• High EC content
Motivation
IACETH Conclusions
Results

Abegglen Etal 2016

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www.cloudman.

Chemical Characterization of Freshly Emitted

Manuel Abegglen1, Benjamin Brem2,3, Martin Ellenrieder4, Lukas Durdina2,3,

1 Institute for Atmospheric and Climate Science, ETH Zurich, Switzerland

The A-PRIDE Campaigns (Aviation Particle Regulatory

• Took place at Zurich Airport in the SR Technics facilities

Aircraft Engine in the Test Cell

Experimental Set-Up at the Zurich Airport

ATOFMS: Aerosol Time-of-Flight Mass Spectrometer

ATOFMS - Aerosol Time-of-Flight Mass Spectrometer

Model TSI 3800-030

ATOFMS – Aerosol Time-of-Flight Mass Spectrometer

ATOFMS Results from a Turbofan engine

Identification of Major Average Particle Types

Cluster 1 (93,4 %): EC-Na-metal

Metal Detected in Exhaust Particles

• <1 %: Vanadium, Manganese, Nickel, Barium, Titanium and

Results – Trace elements found in fuel and oil

Thrust dependent occurrence of metals from fuel and oil

• Ba, Na and Ca:

Thrust dependent occurrence of metals probably from

Metals found in fuel, oil and used as alloys in aircraft engines

Summary and conclusions

• Measurements were conducted on individual, freshly emitted aircraft exhaust

Thank you for your attention!

• The emitted particles are ultrafine Particulate Matter (PM0.1, mean

Measurements at the Zurich Airport

Campaign Date CPMA ATOFMS

A-PRIDE 4 November 2012  —

Piggyback June 2013  

SR Technics – Aircraft Engine Test Cell

Experimental setup used in the A-PRIDE 4 campaign

Lobo et al., 2015

Results: Size of particles analyzed by the ATOFMS

• dae (ATOFMS) was

•  Only the largest

Cluster 3 (1.8 %): Ca-Al-K-Fe-Na (Metal Type Particle)

• Metals appear in the

Results: Single particle spectra III

Cluster 2 (4.5 %): K-Na-EC

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