Received: 1 April 2021 | Revised: 24 June 2021 | Accepted: 11 July 2021

DOI: 10.1111/ina.12909

ORIGINAL ARTICLE

Emissions of soot, PAHs, ultrafine particles, NOx, and other

health relevant compounds from stressed burning of candles in
indoor air

Christina Andersen1 | Yuliya Omelekhina1 | Berit Brøndum Rasmussen2 |

Mette Nygaard Bennekov2 | Søren Nielsen Skov3,4 | Morten Køcks3 | Kai Wang2,5 |
Bo Strandberg6 | Fredrik Mattsson1 | Merete Bilde2 | Marianne Glasius2 |
Joakim Pagels1 | Aneta Wierzbicka1

1
Ergonomics and Aerosol Technology,
Lund University, Lund, Sweden Abstract
2
Department of Chemistry, Aarhus Burning candles release a variety of pollutants to indoor air, some of which are of con-
University, Aarhus C, Denmark
3
cern for human health. We studied emissions of particles and gases from the stressed
Danish Technological Institute, Aarhus C,
Denmark burning of five types of pillar candles with different wax and wick compositions. The
4
Department of Clinical Medicine, Aarhus stressed burning was introduced by controlled fluctuating air velocities in a 21.6 m3
University, Aarhus C, Denmark
5
laboratory chamber. The aerosol physicochemical properties were measured both
College of Resources and Environmental
Sciences, China Agricultural University, in well-­mixed chamber air and directly above the candle flame with online and of-
Beijing, China fline techniques. All candles showed different emission profiles over time with high
6
Division of Occupational and
repeatability among replicates. The particle mass emissions from stressed burning
Environmental Medicine, Lund University,
Lund, Sweden for all candle types were dominated by soot (black carbon; BC). The wax and wick
composition strongly influenced emissions of BC, PM2.5, and particle-­phase polycyclic
Correspondence
Aneta Wierzbicka, Ergonomics and aromatic hydrocarbons (PAHs), and to lower degree ultrafine particles, inorganic and
Aerosol Technology, Lund University, Lund
organic carbon fraction of PM, but did not influence NOx, formaldehyde, and gas-­
SE-­22100, Sweden.
Email: aneta.wierzbicka@design.lth.se phase PAHs. Measurements directly above the flame showed empirical evidence of
short-­lived strong emission peaks of soot particles. The results show the importance
Funding information
This work is partly funded by the of including the entire burn time of candles in exposure assessments, as their emis-
Innovation Fund Denmark (IFD) under
sions can vary strongly over time. Preventing stressed burning of candles can reduce
File No. 7048-­0 0002A. Funding by
Ergonomics and Aerosol Technology at exposure to pollutants in indoor air.
Lund University is also acknowledged.
KEYWORDS
aerosol, airborne particles, black carbon, candle emissions, flickering candle flame, gaseous
pollutants

1 | I NTRO D U C TI O N used in religious ceremonies. Christmas time in particular is a high

season for candle burning. Burning candles emit particle and gas-­
Burning of candles is a common activity in many cultures around phase pollutants. Examples of pollutants emitted by candle burning
the world. It is associated with a cozy atmosphere and is commonly are aerosol soot particles (black carbon [BC]),1–­3 ultrafine particles

This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium,
provided the original work is properly cited.
© 2021 The Authors. Indoor Air published by John Wiley & Sons Ltd.

Indoor Air. 2021;31:2033–2048.  wileyonlinelibrary.com/journal/ina | 2033

 |
2034
(UFPs),4–­7 polycyclic aromatic hydrocarbons (PAHs),8 and NOx.9–­11
Candle emissions have been associated with various adverse health
effects in humans such as reduced cognitive abilities12 and nega-
tive changes in lung function.13 On the contrary, increased power
of high-­frequency spectral band of heart rate variability in healthy
women has been reported after exposure to candle particles from
stressed burn.14 Animal studies conducted on mice exposed to can-
dle soot particles are associated with cytotoxicity and inflammation
15
in the lungs as well as telomere shortening in the lung and spleen,
a marker for the risk of developing cardiovascular diseases.16 In addi-
tion to being a major pollutant in indoor air, candle soot from various
types of stressed burning has attracted a huge interest as a cheap
emerging technology to produce functional nanomaterials with
unique properties such as high hydrophobicity.17
Candle emissions were found to be the primary source to the daily
residential exposure to ultrafine particle number concentrations in a
4 18
study of Danish homes. Wallace et al measured personal exposure
to ultrafine particles and found that for a typical nonsmoking sub-
urban lifestyle, indoor exposure exceeds outdoor exposure to UFPs.
It is well-­known that exposure to PAHs is of health relevance. The
most toxic of the PAHs is benzo[a]pyrene (BaP), which is classified as
a group 1 carcinogen by the International Agency for Research on
Cancer.19 The United States Environmental Protection Agency has
classified a group of 16 priority PAHs. 20 Twelve of these have been
assigned toxic equivalence factors based on their cancer potency
relative to BaP. 21 Alkylated PAHs are also important to include in
emission studies since they reportedly are often more pervasive and
more toxic than the parent PAHs. 22 Thus, maximizing the number
of PAHs included in studies is essential to increasing knowledge
of emission and exposure scenarios as well as the associated risks.
Moreover, the WHO has set an air quality guideline that estimates
the unit risk of BaP level to be 0.12 ng m−3, which will cause an ex-
cess lifetime cancer risk of 1/100 000. 23
Size distributions, total mass emission factors, 24,25 and BC emis-
sion factors1,3 have been reported in a number of studies on can-
dle emissions. Previous studies have also compared the candle soot
morphology with other soot particle sources, and reported that can-
dle soot particles showed a similar type of microstructure as the die-
sel exhaust particles, although the size of the soot aggregates was
26,27
larger. Detailed soot formation inside candle flames has been
studied. 28,29 However, highly time-­resolved emission data of soot,
organic aerosol, PAHs, and inorganic aerosol in the emission zone
near the candle are largely missing. The influence of the wax and
wick composition on the formation of soot during stressed burn is
not known.
It is important to estimate how candles contribute to soot levels
in indoor environments, where we spend the majority of our time.
This is especially important considering the health concerns related
to the exposure to soot/BC.30 NO2 is known to cause health effects
in humans. NOx emissions from the steady burn of candles have pre-
viously been reported.9,11 However, the influence of the wax and
wick composition on the NOx emissions has not been investigated.
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ANDERSEN et al.
Practical implications
• The duration of burning and flame disturbance due to
changing air velocities around the candle influence the
level of emissions of airborne pollutants.
• Optimizing wax and wick composition can reduce emis-
sions of soot (BC), PM2.5, and particle-­phase polycyclic
aromatic hydrocarbons (PAHs), but not emissions of
NOx, formaldehyde, and gas-­phase PAHs at stressed
burn conditions.
• Preventing stressed burning of candles (flame distur-
bance) will reduce exposure to soot (BC), PM2.5, and
particle-­phase polycyclic aromatic hydrocarbons (PAHs).
• Introducing an international compliance standard for
candle manufacturers that includes stressed burn
emissions would enable users and retailers to make in-
formed choices and would reduce exposure to airborne
pollutants.
The aim of this study is to investigate the pollutant emissions,
including particles and gases from five types of pillar candles, during
controlled stressed burn conditions in a chamber. Rasmussen et al31
reported previously detailed descriptions of the wax and wick com-
positions of the same five types of pillar candles along with the
emission characteristics under steady burn conditions. In this study,
the emissions of the same five types of candles during controlled
stressed burn conditions are compared, and further evaluated from
the perspective of the potential impact that flickering candles may
have on indoor air quality in specific emission scenarios.
2 | M ATE R I A L S A N D M E TH O DS
2.1 | Experimental design
2.1.1 | Well-­mixed emissions in a 21.6 m3 chamber
We measured the particle and gas emissions from five types of pil-
lar candles (120 mm in height and 58–­60 mm in diameter) that had
different wax and wick combinations (denoted as candles 1–­5) dur-
ing stressed burning conditions (Table 1). All candles were white and
non-­scented. Three candles of one type were burned at a time for
3.5 h in each of the experiments in a 21.6 m3 stainless steel cham-
ber with an air exchange rate (AER) of 2 h−1.32 Two replicates were
performed for each of the five candle types (ie, three candles of one
type in each experiment, thus variability in six studied candles was
captured). A rotating fan was applied to create a fluctuating air flow
to make the candle flames flicker to create stressed burn conditions
relevant for indoor environments. The length of the wicks was cut to

ANDERSEN et al.
TA B L E 1 Wax composition of the five pillar candles. These data including detailed wick composition measurements were previously
presented by Rasmussen et al.31 (Table 1 from Rasmussen et al31 is reproduced here)
Candle No. Wax material
1 Animal stearin
2 Paraffin (75%), Palm stearin (25%)
3 Paraffin
4 Palm stearin
5 Paraffin
1 cm before the experiments. The candles were lit with a gas lighter
inside the chamber at the start of the experiment. After 3.5 h, the
experiments ended and emissions during candle extinguishing were
not included in these experiments. The extinguishing emissions
were studied in complementary experiments “Above the flame” and
are described below.
For comparison one steady burn experiment for candle type 1
was performed with an AER of 2 h−1. In the steady burn experi-
ment, the candle flames were not disturbed by fluctuating air ve-
locities. Metal mesh cylinder shields (230 mm in diameter) were
placed around each of the three candles. The fan was in this case
positioned to mix the air in the chamber but not to disturb the
flames. The air velocity in all experiments was measured with an
air velocity meter (Swema-­air 300), which was calibrated before the
experiments.
The center of the rotating fan (AEG VL 5527 MS), in the stressed
burn experiments, was placed at a distance of 160 cm from the can-
dles with the neutral position in an angle of approximately 130 de-
grees. The three candles were placed on a table in a triangular shape
with 10 cm between each of the candle edges. The velocimeter was
placed behind the candles, Figure S1.
2.1.2 | Measurements directly above the flame
Highly time-­resolved measurements (1 s) above the flame of a single
candle under similar stressed burn conditions were also performed.
These were complementary measurements to gain mechanistic in-
sight into the emission processes during stressed burn and during
extinguishing the candles. In total 11 measurements were carried
out: five of candle 1, three of candle 5, and one measurement each
of candles 2, 3, and 4. A stainless steel ¼” sampling tube was placed
approximately 4 cm above the flame. It was shifted approximately
1 cm to the side so as not to disturb the flame. An ejector dilutor
(Model DI 100; Dekati; Finland) was used to dilute the emissions (1:8
times) before measurement. Highly time-­resolved measurements
above the flame were also carried out when the candles were extin-
guished with the snuffer. A snuffer is a device, that according to the
candle manufacturer's instructions, should be used to extinguish the
candles by bending the wick and submersing it into the melted wax.
In total, five measurements of the extinguishment were carried out:
that is, one for each of the five candle types.
|
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2035
Wick
Production method No.
Pressed 1
Fully refined paraffin, Pressed 2
Fully refined paraffin Molded, rustic looking 3
Pressed 1
Fully refined paraffin Pressed 5
2.2 | Emission characterization -­equipment and
analysis
2.2.1 | Online characterization
A seven-­wavelength aethalometer (model AE-­33, Magee Sci.) was
used for measurements of equivalent black carbon (eBC) mass con-
centrations. Equivalent black carbon is the terminology used for BC
measurements with optical absorption methods.33 The eBC mass
concentration was derived from the measured changes in attenu-
ation through the filter at 880 nm using the default optical param-
eters used in the software.
Number concentration and particle size distributions were mea-
sured with a nano-­Scanning Mobility Particle Sizer system (nano-­
SMPS) measuring in the range 2.4–­79.1 nm (TSI, DMA 3085, CPC
model 3776, TSI Inc.) and a long SMPS measuring in the range 18.8–­
914 nm (TSI, DMA 3081, CPC model 3775, TSI Inc.). Toward the end
of the experiments, a catalytic stripper (CS) operating at 350°C and
1.5 lpm (Model CS 015, Catalytic Instruments GmbH) was intro-
duced upstream the nano-­SMPS to assess the volatile mass fraction
of particles in the UFP size range. This allowed us to gather informa-
tion on the composition of the UFPs emitted during stressed burn
without the interference of the larger soot mode particles. Losses
in the CS were accounted for using a size-­dependent parameteriza-
tion provided by the manufacturer. For larger particles (>60 nm),
size-­independent thermophoretic losses dominate (27% losses),
as particle size decreases the losses increase due to the additional
mechanism of diffusion. The combined losses from both mechanisms
were as follows: 33% at 30 nm, 56% at 10 nm, and 86% at 5 nm.
A Soot Particle Aerosol Mass Spectrometer (SP-­AMS) was used
to measure the time-­resolved emissions of refractory (dual vaporizer
mode) and non-­refractory (tungsten vaporizer mode) particles, pre-
viously described by Onasch et al34 and DeCarlo et al.35 The SP-­AMS
measured 5 min in the dual vaporizer mode followed by 5 min in the
tungsten vaporizer mode in the well-­mixed chamber measurements.
In the measurements above the flame, the dual vaporizer mode was
used. In the above flame experiments, the SP-­AMS was sampling in
the FAST-­MS mode, which allowed measurements with 1 s time res-
olution. Sampling was done in the closed mode (for background ad-
justments) for 5 s once per minute. The SP-­AMS was calibrated using
nebulized ammonium nitrate and carbon black (regal black, Cabbot
Inc.) particles that were dried and then size selected to 300 nm using
 |
2036
a DMA. Further details are provided in the Appendix S1. Phosphates
were quantified as the sum of the phosphate-­related ions PO, HPO,
PO2, HPO2, PO3, HPO3, PO 4, HPO 4, and H2PO 4.
NO and NO2 were monitored with a chemiluminescence ana-
lyzer (CLD 700 AL, ECO PHYSICS AG). CO2 was measured with a
non-­dispersive infrared CO2 analyzer (LI-­8 020, LI-­COR, Lincoln) and
was below 1500 ppm. O2 (OXROB3, FireStingO2, PyroScience) and
temperature (Swema-­air 300) in the chamber were also measured
during all experiments. Sampling lines for online and offline mea-
surements were situated in chamber air approximately 2 m from the
burning candles.
All the above-­listed instruments were used for particle char-
acterization during the well-­mixed emissions. For measurements
above the flame, the SP-­AMS and the NOx chemiluminescence ana-
lyzer were applied.
2.2.2 | Offline characterization
Sampling for offline analysis was performed from 0.5 to 3.5 h in the
experiment. Blank samples were collected in the chamber with non-­
burning candles.
Organic carbon (OC) and elemental carbon (EC) were deter-
mined on particles collected on quartz fiber filters with the use of
a PM1 pre-­cyclone at a flow rate of 8.5 min−1. Parallel sampling was
used. This means that in one sampling line a quartz filter was used,
while in the other line a quartz filter was placed behind a Teflon fil-
ter, which captured particles and allowed accounting for positive
gas adsorption artifacts of OC on the quartz filter. The samples on
the quartz filters were analyzed with a thermal optical analyzer (DRI
Model 2001 OC/EC Carbon Analyzer, Atmoslytic Inc.) using the
NIOSH NMAM 5040 diesel exhaust protocol. The EC limit of detec-
tion (LOD) was 0.06 µg C cm−2.
Carbonyl compounds were sampled with
2,4-­dinitrophenylhydrazine (DNPH) cartridges with a flow rate of 1 L
min−1 and subsequently analyzed with high-­performance liquid chro-
matography (HPLC) for the following compounds: formaldehyde, ac-
etaldehyde, acetone, acrolein, propionaldehyde, benzaldehyde, and
butyraldehyde.
Samples were collected with a flow rate of 15 L min−1 with two
filters in parallel for subsequent analysis with ion chromatography
−
for the following ions: Cl , NO3−, −3 −2 + + +
PO 4 , SO 4 , Na , NH4 , K , Ca , +2
and Mg+2. The divalent cation Mg+2 was not detected in the emis-
sions from any of the candles. Further details are described in the
Appendix S1.
The sampling equipment and analytical techniques used for
PM2.5, particle-­associated PAHs, and gas-­phase PAHs are thor-
36
oughly described elsewhere with some modifications. In short,
two sampling assemblies were used with a flow rate of 2 L min−1. In
the first assembly, PM2.5 and associated PAHs were sampled on a
filter (Teflo; Pall Corporation, 37 mm diameter, 2 µm pore size), be-
hind a PM2.5 cyclone pre-­separator. In the second assembly, a solid
adsorbent tube (XAD-­II; 120 mg) collected gas-­phase PAHs. A filter,
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ANDERSEN et al.
the same type used for the PM2.5 measurement, was placed in front
of the adsorbent tube. This filter was not analyzed. After gravimetric
analysis, the PM2.5 filters were analyzed for their contents of par-
ticle PAHs, and the XAD-­II tubes for gas-­phase components. The
concentrations of 33 PAHs, including 16 US EPA priority PAHs and
16 alkylated species, were determined. Further details are presented
in the Appendix S1. All results were corrected for the blanks. The
limit of detection (LOD) was calculated as three times the standard
deviation of the values for the blanks or the background noise of
these blanks. A certified reference material (SRM 1649a, urban dust)
was used as quality control. The measured levels of 13 PAHs lie, for
the most part, within 35% of the certified levels. Good precision was
realized for the duplicates of both the gas-­PAHs.
2.2.3 | Toxic equivalence factors for
individual PAHs
The relative importance of individual PAH compounds for the total
cancer risk of the total concentration was calculated with toxic
equivalence factors (TEFs) obtained from Larsen and Larsen24 of the
12 PAHs analyzed in this study. The compounds were ranked ac-
cording to cancer potency relative to BaP (ie, BaP equivalents [BaP
eqs]), with a TEF factor for BaP set to 1. Offline sampling and anal-
yses were used for particle characterization only during the well-­
mixed emission experiments.
2.3 | Data analysis
2.3.1 | Emission factor calculation
General equations describing how emission factors can be derived
from the pollutant concentrations measured in indoor air, on the
basis of mass balance equations for indoor environments, are given
by Koutrakis et al37 and He et al.38 Here, we used a simplified ex-
pression, Equation 1, where the emission factor per candle averaged
over 3.5 or 3 h (see details in the Online and Offline characterization
sections), Sav, was calculated as follows:
Cav ⋅ V ⋅ (a + k)
Sav = (1)
n
where Cav is the average concentration over the time period (either
number or mass concentration of the pollutant), V is the chamber vol-
ume (m3), a is the air exchange rate (h−1), k is the loss rate due to depo-
sition and coagulation (h−1), and n is the number of candles.
The air exchange rate in the chamber was controlled and set
to 2 h−1. The decay rate was determined on the basis of two decay
experiments for candle types 4 and 5, following the stressed burn
experiments after extinguishing the candles. The determined value
of the loss rate (k) used for the calculation of the particle number
emission factors was 2.4 h−1 (strong coagulation effect), and for

ANDERSEN et al.
the calculation of the particle mass emission factors 0.4 h−1 (mass
is conserved upon coagulation so no coagulation effect) These val-
ues were used for calculating emission factors of all particle-­phase
characteristics. No loss rate was included to calculation of emission
factors of gas-­phase components.
3 | R E S U LT S A N D D I S CU S S I O N
3.1 | Time resolved measurement of well-­mixed
emissions in the chamber
The measured equivalent black carbon (eBC, measure of soot parti-
cle mass concentration) and the particle number concentrations (size
interval 3–­8 0 nm) over time are shown in Figure 1 and Figure S2.
The presentation of the size interval 3–­8 0 (nano-­SMPS) is moti-
vated by the largest contribution within this size range to the total
number concentration measured. The comparison of the five differ-
ent candle types illustrates differing time emission profiles of eBC
with relatively high repeatability of the profiles between the two
replicates (three nominally identical candles in each experiment) for
each candle type. The absolute values of the emitted mass concen-
trations of eBC over each of the two full experiments varied by on
average ± 20% from the mean value for each candle type. This is a
measure of the precision (repeatability) of the replicate experiments
that includes both small variations in our ability to control the level
of stress on the candle burning but also includes real differences
caused by variations in emissions between candles of the same type.
A distinct variation between the initial first hour and the remain-
ing time is evident for candles 1–­4 (Figure 1 and Figure S2). Candles
F I G U R E 1 Examples of time traces of eBC in µg m−3 (black) and number concentration in particles cm−3 (gray) of particles in the size range
from 3 to 80 nm for stressed burn experiments with candles 1, 3, 4, and 5. Three candles of each type were used in each experiment. All ten
experiments including replicates can be seen in Figure S2. The breaks in the eBC time trace for candle 5 are due to frequent filter change in
the instrument caused by the high chamber concentrations
|
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2037
1 and 2 show relatively high emissions of eBC in the initial half hour,
followed by a decrease in the concentration. After burning the can-
dles for 1.5–­2 h, the concentrations again increase, particularly for
candle 1. Candles 3 and 4 show opposite emission profiles, with can-
dle 3 showing low eBC emissions in the start-­phase, with increasing
emissions over time, while candle 4 shows a peak emission of eBC in
the start-­up with strongly reduced emissions after the first 1–­1.5 h.
Candle 5 is the only one that shows an increasing eBC concentration
over time, reaching “steady-­state behavior”. After 1–­2 h, candle 5
reached by far highest eBC concentration measured in the cham-
ber (21.6 m3, AER = 2 h−1) ~450 µg m−3 (Figure 1), while the highest
concentration resulting from burning of the remaining candles was
~80 µg m−3 (candle 2). The breaks in the eBC time trace for can-
dle 5 are due to frequent filter changes in the instrument caused
by the high chamber concentrations. The decreased concentration
after each filter change in the later part of experiment 5.1 may be
due to uncertainties in the filter-­loading correction in the instrument
caused by the high eBC concentrations.
There was no clear correlation between burn rate and eBC emis-
sions (Table 2). The reproducible and strongly varying time trends in
eBC emissions between the candles may be explained by variations
in wick-­length and flame height over time, properties that are partly
controlled by the selected wax and wick combinations. In addition,
a rim may develop near the candle edges which can affect the com-
bustion conditions and the impacts of surrounding air currents on
the flame stability. It is expected that soot emissions may vary more
in the period early after igniting the candles when a fresh wick is ig-
nited and the liquid fuel pool develops over time. To shed more light
on the mechanisms of the soot emission, data measured directly
over the flame with high time resolution are described below.
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2038 ANDERSEN et al.

TA B L E 2 Emission factors and burn

PNC a (2.4–­914 nm) eBC NO NO2 Burn rate
rate per candle based on concentrations
#/h µg h−1 mg h−1 mg h−1 g h−1 averaged over 3.5h (0–­3.5 h of
the experiments) based on online
Candle 1 9.3 × 1013 (±0.2 × 1013) 408 (±50.5) 2.8 (±0.1) 1.0 (±0.1) 7.3 (±0.2)
measurements
Candle 2 9.0 × 1013 (±0.4 × 1013) 634 (±0.5) 4.1 (±0.2) 1.3 (±0.1) 5.1 (±0.3)
13 13
Candle 3 6.3 × 10 (±0.3 × 10 ) 329 (±89.5) 3.4 (±0.2) 1.1 (±0) 4.3 (±0.1)
Candle 4 8.5 × 1013 (±0.35 × 1013) 160 (±68.5) 3.2 (±0.3) 1.1 (±0.1) 5.4 (±0.3)
13
Candle 5 1.5 × 10 (±0) 4346 (±874) 4.7 (±0) 1.5 (±0) 5.9 (±0.1)
Steadyb 8.3 × 1013 2.6 2.8 0.6 7.5 ± 0.2

Average values are given together with range of two replicates (three candles each) in brackets.
Values for burn rate represent average and standard deviation (given as ±) of 6 candles used in two
replicate experiments.
a
Emission factors of PNC based on 3 h average concentrations (ie, 0–­3 h of the experiments), due
to use of the catalytic stripper in the last 30 min of the experiment.
b
One steady burn experiment for candle 1

TA B L E 3 Emission factors of OC, EC,

OC EC PM2.5 Inorg
PM2.5 (gravimetric analysis) and total
µg h−1 µg h−1 µg h−1 µg h−1 particle inorganics

Candle 1 88 (±6) 328 (±53) 283 (±53) 88 (±3)

Candle 2 106 (±16) 382 (±52) 510 (±61) 129 (±7)
Candle 3 140 (±35) 252 (±67) 393 (±57) 28 (±7)
a a,b
Candle 4 46 (±9) 30 (±11) 330 68 (±1)
Candle 5 232 (±143) 3132 (±2145) 3038 (±1691) 53 (±28)
c
Steady 134 ˂DL ˂DL 91

All data are averaged over 3 h (0.5–­3.5 h of the experiments) and reported per candle based on
off-­line analysis.
Average values are given together with range of two replicates (three candles each) in brackets.
<DL indicates that the concentration was below the detection limit
a
Possibly underestimated value, because the peak emissions occurring within the first half hour are
not included (sampling 0.5–­3 h).
b
Value based on single measurement.
c
One steady burn experiment for candle 1

The number concentrations measured in the chamber also
showed high repeatability between replicates both in emission pat-
terns and in concentrations (particles/cm3) (Figure S2). All candles,
except from candle 3, showed peak emissions when the candles
were lit, whereas candle 3 showed more stable emissions, with a
slight increase in particle number concentration over time.
It is worth noting that a relatively stable number concentration
is reached even faster than expected from the air exchange rate
(90% of the steady-­state value reached after 30 min assuming con-
stant emission level and a + k = 2.4 h−1). This could either be due to
strongly increased emissions in the early part of the experiment, or
to coagulation rapidly becoming a dominating loss mechanism of the
particle number as the concentration reaches above ~2 × 106 parti-
cles cm−3, which was described by Wallace et al.5
Candle 5 showed a peak in number concentration (1–­2 × 106 ­#/­cm3)
in the initial half hour after igniting the candles, though with a lower
number concentration than the other candles (2–­3 × 106 ­#/­cm3). This
was followed by a strong decrease in number concentration and a ​si-
multaneous strong increase in soot particle (eBC) mass concentration.
The increased emission of soot particles increased the probability of
coagulation between soot particles and UFPs, which in turn reduced
the measured particle number concentration.
A comparison of eBC concentrations with the AMS time traces
(Figure S3) was carried out. It measured the time-­resolved mass
concentration of organic aerosol (OA) and inorganic aerosol par-
ticle mass concentration in tungsten vaporizer mode and showed
that the mass concentration for all candles during stressed burn
was dominated by eBC, while the organic and inorganic mass con-
centrations were significantly lower. The organic mass concentra-
tion was 15–­25 times lower than that for eBC. The time traces of
eBC, OA, and inorganic components, measured with two different
methods (aethalometer AE33 and HR-­AMS), showed the same
trend in emission profiles of eBC and OA when comparing each of
the individual candle types. However, the inorganic particle com-
ponents did not always follow the same emission profile (Figure 1
and Figure S3).
The above-­described variations in concentrations over time il-
lustrate the importance of including the entire burn time when
 |

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ANDERSEN et al. 2039

evaluating the particle emissions from candles, and that the chosen
burn time will influence the average emissions reported.
3.2 | Emission factors
Table 2 summarizes the calculated emission factors (EFs) based on
the 3.5 h average concentrations of the parameters measured with
online techniques for each of the candle types, presented as emis-
sions per candle. The emission factors of OC, EC, PM2.5, formal-
dehyde (CH2O), and PAHs measured with offline techniques were
averaged from 0.5 to 3.5 h and are presented in Tables 3 and 4.
Candle 5 shows the highest EFs of eBC, EC, PM2.5, particle-­phase
PAHs, and NOx (see Tables 2, 3, and 4). The EF of UFP (2.4–­100 nm)
were of similar order of magnitude for all candles (ie, 1013 particles
per h); however, emissions for candle 5 (1.3 × 1013 particles per h)
were 4 to 6 times lower than for other candles (6.3 × 1013–­9.3 × 1013
particles per h) (Table S1), which is in line with the result discussed
above. It is important to mention that during steady burn candle 5, as
31
reported by Rasmussen et al, also displayed the lowest UFP num-
ber emissions among candles 1–­5. However, the same candle 5 has
the by far highest eBC emission. This illustrates how important it is
to evaluate candles at both steady and stressed burn conditions and
assess different emission characteristics (ie, not only UFP). Candles
1–­4 showed more similar magnitudes of EFs. Candle 4 showed
slightly lower EFs for PM2.5, eBC, and PAHs in the particle-­phase,
while it has the overall highest EF of gas-­phase PAHs among all can-
dle types, see Tables 2, 3, and 4.
3.3 | Soot measured as EC and eBC
Comparison of OC and EC results (Table 3) shows that the emissions
from all candles were dominated by EC during flickering/stressed
burn. The exception is candle 4, where OC and EC concentrations
are low compared to all other candles. The initial half hour was not
included in the OC/EC sampling. EC and eBC were highly correlated
(Figure S4) suggesting that any of them can be used as proxies for
each other when measuring stressed burn emissions from candles
(slope 1.38, r2 = 0.93; Figure S4). As shown in the time-­resolved eBC
measurement (Figure 1), soot emissions were almost exclusively tak-
ing place during the first hour for candle 4, which suggests that the
lack of data for the first 30 min of the experiment caused substan-
tial underestimation of the EC value. Consequently, when compar-
ing soot emissions from different candle types, the values of eBC
are used in this paper because they capture the entire burn period
and all peak contributions during the experiments. For comparison,
a steady burn experiment of candle 1 was included. The emissions of
eBC were low, about 60 to 1700 times lower than at stressed burn
of the five candle types.
The literature data on EC emissions during stressed burn of can-
dles in laboratory studies range from 4.5 to 24.1 mg h−1.1,25 The high-
est value in our study was for candle 5 (3.1 mg h−1) and the lowest
value for candle 4 (0.03 mg h−1). Thus, the EC emission factors found
at the degree of stress used in this study are lower than those found
in the literature. However, the literature data are for tapered candles
that may have higher EC emissions compared to pillar candles at a
given stress level, for example, due to longer wicks. Clearly, more
data are needed for candle emissions from stressed burn. Especially
data for the same candle type used both during controlled stress
levels in the laboratory and under real-­world conditions would be
useful.
Currently, there are no international standards regulating can-
dles manufacturing and sales that would include the emissions of
airborne pollutants at the stressed burn of candles. Within the
European Union, there are several certification schemes for candle
manufacturers, which use a sooting index of candles.39 However,
these emission assessments are conducted at steady burn condi-
tions with a metal mesh shield around the candle preventing dis-
turbance of the candle flame. Including assessments of the stressed

TA B L E 4 Emission factors of formaldehyde (CH2O), PAHs, and benzo[a]pyrene equivalent (BaP eq.)

BaP eq. Gas

CH2O PAH particle PAH gas BaP eq. particle BaP eq. gas + particle

µg h−1 ng h−1 ng h−1 ng h−1 ng h−1 ng h−1

Candle 1 54 (±4.5) 90 (±13.0) 416 (±289.0) 0.79 (±0.11) 0.11 (±0.025) 0.91 (±0.14)
Candle 2 46 (±6.5) 90 (±16.0) 600 (±30.0) 0.78 (±0.07) 0.13 (±0.025) 0.94 (±0.10)
Candle 3 43 (±0.5) 59 (±11.5) 591 (±29.5) 0.44 (±0.07) 0.23 (±0.075) 0.67 (±0.14)
a b a b
Candle 4 49 (±3.0) 25 (±12.5) 1043 0.09 (±0.03) 0.16 0.27a,b
Candle 5 39 (±3.0) 578 (±254.5) 557 (±100.5) 3.86 (±1.95) 0.28 (±0.06) 4.13 (±2.01)
c
Steady 35 26 846 ˂DL 0.11 0.11

PAHs and BaP eq. emission factors are given separately for the particle and gas-­phase. All data are averaged over 3 h (0.5–­3.5 h of the experiments)
and reported per candle based on off-­line analysis. Average values are given together with range of two replicates (three candles each) in brackets.
<DL indicates that the concentration was below the detection limit.
a
Possibly underestimated value, because the peak emissions occurring within the first half hour are not included (sampling 0.5–­3 h).
b
Value based on single measurement.
c
One steady burn experiment for candle 1
 |
2040
burn emissions, which mimic real-­life situations, would allow users to
make informed choices, as well as reduce the emissions of airborne
pollutants.
3.4 | PAHs and benzo[a]pyrene (BaP) equivalent
(BaP eq)
The particle-­phase PAH emissions were low in comparison with gas-­
phase PAH emissions, except from candle 5, which shows the high-
est particle-­phase emissions and is comparable to gas-­phase PAHs
emissions (Table 4). However, it has to be noted that the particle-­
phase contribution to the BaP eq concentration is higher than from
gas-­phase PAHs.
During the steady burn experiment, the particle PAH emissions
were low and comparable to the lowest emissions during stressed
burn (candle 4). However, emissions of gas-­phase PAHs during the
steady burn were relatively high and comparable to the highest
emissions of gas-­phase PAHs during stressed burn for candle 4.
The benzo[a]pyrene equivalent (BaP eq) concentrations of the
particle and gas-­phase PAHs were calculated according to standard
40
methods and are provided as EFs in Table 4. During stressed burn,
the candles show total BaP eq EFs from 0.27 to 4.13 ng h−1, with
candle 5 having the highest EF and candle 4 the lowest. Candles
−1
1–­3 show similar BaP eq EFs of 0.67–­0.94 ng h . Particle-­phase PAH
emissions are the main contributors to the BaP eq. emissions. All five
candles show similar BaP eq. EFs for the gas-­phase PAH emissions.
Gas-­phase PAH emissions were not influenced to a big degree by
wax and wick composition or type of burning (stressed or steady
burn). It is important to include both particle-­and gas-­phase PAHs to
assess the risks and toxicities of PAHs in emissions in environmental
studies.
Polycyclic aromatic hydrocarbons were sampled from 0.5 to
3.5 h. Since candle 4 showed the highest eBC emission in the initial
0–­1 h (Figure 1), the chosen sampling time will likely cause an un-
derestimation of particle-­phase PAH emissions from candle 4. Thus,
the particle-­phase PAH emissions are consistent with the trends ob-
served for eBC EFs where candle 5 showed by far the highest emis-
sions, candle 4 the lowest, and candles 1–­3 intermediate emissions.
3.5 | NOx
The EFs of NOx show similar levels for candles 1–­4, while candle
5 shows slightly higher NOx EFs (Table 2). In contrast to the eBC
emissions, NOx emissions for all candles during stressed burn
showed increasing concentrations over the first hours and then
reached a steady-­state behavior (example for candle 3 showed in
Figure S5). This is expected for the air exchange rate used and a
roughly constant emission factor over time. The similarity in NOx
emissions is consistent with previous reported NOx emissions from
the steady burn of candles.9,11 Derudi et al9 measured NOx emis-
sions (1.7–­2.5 mg h−1) from the steady burn of paraffin candles of
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ANDERSEN et al.
different wax refinements. Klosterköther et al11 reported values of
NO (2.7–­3 mg h−1) and NO2 (1.8–­2.1 mg h−1) for the steady burn of
paraffin container candles and paraffin church candles. Thus, the
slight variation in NOx emissions may be associated with increased
flame height and a higher flame temperature.
The NOx EFs from the steady burn experiment of candle 1 are
provided in Table 2. The steady burn NO and NO2 EFs are similar to
those of the stressed burn of candle 1. The NO values were 2.8 mg
h−1 for steady and stressed burn. The NO2 values were 0.6 and
1.0 mg h−1, respectively, for steady and stressed burn. Thus, NOx
emissions did not show dependence on burning mode of the candles
nor the wax and wick composition.
3.6 | Carbonyl compounds
The EFs of formaldehyde for the time period 0.5–­3.5 h are presented
in Table 4. The measured concentrations of formaldehyde and other
carbonyl compounds (acetaldehyde, acetone, acrolein, propionalde-
hyde, benzaldehyde, and butyraldehyde) are shown in Table S2 for
the same time period. Acrolein was not detected in the emissions
from any of the candles. The five different candle types show very
similar concentrations of emitted carbonyl compounds with their
sum ranging from 7.18 ± 0.18 for µg m−3 candle 2 to 9.32 ± 0.11 µg
m−3 for candle 1. The low emissions were expected, since aldehyde
and carbonyl emissions primarily are related to the addition of fra-
grances or dyes in the candles.9 These results indicate that emissions
of VOCs from the stressed burning of candles are minor compared
to the particle emissions.
3.7 | Inorganic particle emissions
The total inorganic particle EFs are presented in Table 3. The sum-
marized inorganic emissions could explain between ~2% (candle
5) and 31% (candle 1) of PM2.5. This is substantially lower than for
steady burn when PM emissions are commonly dominated by in-
organic emissions.1 The two paraffin candles, 3 and 5, show lower
emitted mass concentrations of inorganic ions (Table 3) compared
to candles 1, 2, and 4. This may be caused by less impregnation (eg,
as flame retardants) needed to protect the wick against the paraf-
fin wax (candles 3 and 5) relative to stearin wax (candles 1, 2, and
4 [Table 1]). Notably, candle 5 is the only one, where the anions are
dominated by nitrate and the cations by sodium (Table S3). All other
candles show anion emissions dominated by phosphates. The inor-
ganic PM from ion chromatography correlated relatively poorly with
EC (r2 = 0.55; Figure S4).
The sum of the inorganic emissions, OC, and EC is higher than
PM2.5 emissions for all candles except candle 4 where the opposite is
observed. The observed differences can be explained by method un-
certainties, possible evaporation of some of the OC before PM2.5 anal-
ysis, and experimental uncertainties/difficulties with filter sampling

ANDERSEN et al.
(eg, maintaining constant flow through the filters). In addition, in the
case of candle 4, there is only one available measurement of PM2.5.
Signals from the inorganic ions—­phosphate, ammonia, sulfate, and
nitrate—­were also identified with AMS. These ions were also mea-
sured to be constituents in the candle wicks by Rasmussen et al31
and in the particle emissions with ion chromatography (Table S3). The
AMS signal from the inorganic compounds was significantly lower
than the OA signal (Figure S3). The inorganic signal did not in all cases
follow the emissions of OA, C3+, and PAHs. The inorganic compounds
were not always well correlated with rBC, OA, and PAHs. The inor-
ganic compounds are most likely to be found in the ultrafine particle
mode with sizes below 100 nm as discussed below.1,25 In our study,
the mass-­weighted mode diameter for the UFP mode was 30–­50 nm.
The AMS has a limitation in measuring these particle sizes, because of
a cutoff diameter of around 50 nm. Thus, the measurements depend
on the mixing state, with inorganic components present in the larger
soot mode being detected with much higher efficiency.
3.8 | Particle size distributions and ultrafine
particle emissions
Figure 2 illustrates average (0–­3 h) particle number and mass size
distributions for the replicate experiments of candles 1, 3, and 5
during stressed burning and candle 1 during steady burn in the size
range of 2.4–­914 nm. Particle number size distributions for candles
1–­4 were unimodal with the majority of emitted particles in the UFP
range (<100 nm). The average mode diameters were between 5 and
8 nm for candles 1 to 4. Candle 5 showed a bimodal size distribution
with the modes at 6 nm and ~200 nm. The second mode is formed
by larger soot particles (details below in the section describing
the chemical composition of UFP on the basis of results from the
catalytic striper [CS]). The bimodal number size distribution during
stressed burn was observed earlier by Pagels et al (with modes at
~20–­30 and ~300 nm)1 and by Wallace for citronella candle (with
modes at ~50 and ~200 nm).41 However, unimodal size distribution
at stressed burn was reported by Zai et al24 with only a trace of a
second accumulation mode at ~200 nm.
Number size distributions were converted to mass-­weighted size
distributions by accounting for the size-­dependent effective density
as described in the Appendix S1. Candles 1–­4 showed bimodal mass
size distribution with a UFP mode between 27 and 44 nm and a larger
soot mode between 550 and 900 nm, respectively (Figure 2 and
Figure S6). However, candle 5 showed unimodal mass size distribution
with the mode at 570 nm. It can be also seen that both the number and
mass size distributions of the five candles showed good repeatability
between the two replicate experiments with three candles. Bimodal
(main mode at 290 nm and minor at 50 nm) mass size distribution was
reported by Stabile et al3 during burning of paraffin wax candle.
The particle mass concentration was summed for the UFP mode
(PM 0.1; 2.4–­100 nm) and the soot mode (PM 0.1-­0.9; 100–­914 nm), re-
spectively. The results are shown in Table S1. The soot mode mass
|
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2041
concentration (PM 0.1-­0.9) was highly correlated with both eBC (slope
1.02, r2 = 0.99) and EC (slope 1.42, r2 = 0.94) but correlated less with
inorganic PM (r2 = 0.59) (Figure S4). This was expected because the
main component of the soot mode is eBC/EC with only minor con-
tributions from inorganic matter. The slope above unity for PM0.1–­0.9
vs EC (Figure S4) is most likely due to contributions to PM0.1–­0.9 from
inorganic components and OC.
The UFP mass (PM 0.1) accounted for between 1% (candle 5) and
38% (candle 4) of the total PM 0.9 according to the SMPS measure-
ments. The PM 0.1 was highly correlated with the total mass con-
centration of inorganic ions from ion chromatography (slope 1.37,
r2 = 0.98) (Figure S4). PM0.1 correlated relatively poorly with both
eBC (r2 = 0.58) and EC (r2 = 0.50) (Figure S4).
To investigate the chemical composition of the UFPs, particles
were passed through the catalytic stripper (CS) held at 350°C be-
fore measurement with the nano-­SMPS. The particle mass fraction
(assuming unity particle density of both treated and untreated emis-
sions) surviving the CS after the loss correction was calculated in
the size range 2.4–­60 nm. 60 nm was chosen as the upper limit to
reduce the influence of the soot mode on the heat-­treated samples.
The results from candles 1–­4 showed that the majority of the particle
mass was removed by the CS. The fraction of assessed UFP mass
(2.4–­60 nm) that survived the treatment was 10% for candle 1 (8%
in steady burn experiment), 35% for candle 2, 23% for candle 3, and
14% for candle 4. This suggests that less than 10%–­35% of the UFP
mass consists of EC or other refractory species during stressed burn.
Ammonium phosphate salts (the dominating inorganic component of
stressed burn emissions) and organic aerosol are readily removed by
heating at this temperature.1 Compared to the inorganic composition
(Table S3), candles 2 and 3 with the higher remaining mass fraction
after the CS also contained K+ and Na+ cations in addition to NH4+.
These may constitute alkali salts that are not volatile at 350°C (eg,
potassium phosphate). For candle 5, the situation was different with
83% of the assessed mass surviving the CS. In this case, the soot
mode also extended down below 60 nm which may explain the high
mass fraction that survives the CS. Additionally, NaNO3, a major
contributor to the inorganic emissions for candle 5, decomposed at
380°C and may not have been fully removed from the particles in
the CS.
In summary, candles emit high number concentrations of par-
ticles in the UFP size range during both steady and stressed burn.
Major components of this particle type are water-­soluble inorganic
components such as phosphates, sulfates, and nitrates. This par-
ticle type contains little, if any EC/eBC. The water-­soluble nature
of these particles will affect the lung deposition probability in the
respiratory tract.1 Additionally, candles emit a second type of par-
ticles during stressed burn which have larger sizes and are domi-
nated by soot detected as eBC/EC. This particle type dominated
the mass emissions during stressed burn. This study showed that
by varying the wax and wick combination, the composition and
emission level under stressed burn conditions of both these parti-
cle types can be altered.
 |

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2042 ANDERSEN et al.

F I G U R E 2 Number and mass size distributions of candles 1, 3, and 5 during stressed burn and one experiment for candle 1 during steady
burn. The two replicates for each case are shown. The results are based on measurements with nano-­SMPS and regular SMPS (2.4–­914 nm).
Note the different y-­axis scale in the case of candle 5 (particle number concentration) and for candle 5 and steady burn of candle 1 (particle
mass concentration). Number and mass size distributions for candles 2 and 4 during stressed burn can be seen in Figure S6

F I G U R E 3 AMS time trace of emissions of organic aerosol (OA), rBC, and polycyclic aromatic hydrocarbons (PAHs), as well as NOx and
NO2 time traces. Example of candle 5 above the flame measurements. The graph shows two strong soot (rBC) peaks upon stressing of the
candle flame. The graph supports the coemisssion of OA, and PAHs in the soot peaks, while NOx do not follow a similar pattern. The pie
charts show the percentage distribution of mass concentrations of rBC, OA, and PAHs in each of the two main emission peaks. The upper
pie chart represents the first peak (around 14:16 h) and the lower pie chart the second peak (around 14:17 h)

ANDERSEN et al.
3.9 | Above flame measurements and correlations
between pollutants
Measurements with high time resolution were carried out a few cm
above slightly to the side of the flame during both stressed burn
and upon extinguishing of the candle. The aim was to gain improved
understanding of the particle emission dynamics and pollutant for-
mation mechanisms. Figure 3 shows measurements for candle 5
directly above the flame during stressed burn measured with the
SP-­AMS in dual vaporizer mode with 1 Hz time resolution. The time-­
resolved data show that the particle emissions were dominated by
refractory black carbon (rBC). Organic aerosol (OA) and particle-­
phase PAHs were co-­emitted with rBC in short-­lived strong peaks
from the flickering candle flame. Similar results were found for other
candles (not shown). During stressed burn, rBC constituted about
94% of the sum of rBC, OA, and PAHs. NOx shows a completely dif-
ferent emission pattern, and no clear correlation with rBC, OA, and
PAHs is evident.
Figure 4 shows a time-­resolved AMS measurement above
the flame when candle 2 was extinguished by use of a snuffer.
Figure 4 shows a short-­lived peak of strongly increased OA, PAHs,
and rBC emissions. The particle composition was in this case com-
pletely dominated by OA, which contributed to 79% of the sum of
OA, rBC, and PAHs. This was completely different compared to the
emission peaks during stressed burn.
The correlations between rBC, OA, and PAH emissions mea-
sured above the flame from extinguish emissions are compared to
stressed burn emissions in Figure 5. The graph indicates a correla-
tion between OA, PAHs, and rBC both for extinguishing (OA vs.
2
rBC slope = 3.44, r = 0.86) and for stressed burning (OA vs. rBC
slope = 0.06 and r2 = 0.88). The co-­emission of rBC, OA, and PAHs is
further supported by the linear correlation between PAHs, OA, and
C3+ (marker for rBC) in Figure S7 for candles 2–­5 in well-­mixed air in
the large chamber. The correlation is in this case very high for rBC
+ 2
(C3 ) versus OA (slope = 9.2, r = 0.97) and high also for PAHs versus
+ 2
rBC (C3 ; slope = 90.7, r = 0.93).
We interpret the observed emissions from stressed burn in the
following way: During normal steady candle burning, the candle wax
first evaporates and the volatile organics are then thermochemically
converted in several reaction steps. At lower temperatures, the wax
molecules are first degraded to smaller constituents. At increased
F I G U R E 4 Above flame measurement
of candle 2 during extinguishing,
measured with AMS in dual vaporizer
mode, showing organic aerosol (OA),
PAHs, and rBC concentrations. The pie
chart shows the distribution of the three
components in the peak
|
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2043
temperatures, aromatic rings form that may grow to PAHs, for ex-
ample, and eventually further contribute to soot (rBC) formation.42
It may be that during steady burn almost all larger (particle-­phase)
PAHs are converted to rBC. rBC is later removed in the high-­
temperature oxidation zones at the outer edges of the candle flame
where the hot flame meets oxygen from room air. In these regions,
NOx can be expected to form. Thus, steady burn leads to very low
emissions of particle-­phase PAHs and rBC, but the emissions of NOx
may be considerable.
When the candle flame is cooled down by the surrounding air
flow (flickering) during stressed burn, the oxidation of the soot par-
ticles formed in the candle flame slows down, hence the residence
time in the flame is not sufficient for full oxidation/removal, and the
soot particles can instead be emitted from the flame to room air. In
extreme cases, this phenomenon is visible as black smoke. OA and
PAHs are also emitted as a consequence of the overall cooling of the
flame, though in much lower quantities than rBC particles.
If the flame quenching during stressed burn is more extensive, it
may reach a region where PAHs to rBC conversion is less progressed,
thus resulting in a higher PAH/rBC ratio of the emissions. Our results
are in line with Liang et al43 who reported a higher content of hy-
drocarbons in inner flame soot particles compared to flame tip soot,
which constituted elemental carbon and ash components.
These results indicate, that in time-­resolved measurements,
above the flame and in the well-­mixed chamber measurements, with
use of AMS, the peak increases of one of the parameters—­rBC, OA,
or PAHs—­may be used as a proxy for the emissions of the two other
parameters for stressed burn.
The HR organic mass spectra measured above the flame for can-
dle 2 during stressed burn and extinguishing are shown in Figure 6.
Both spectra are dominated by CH fragments. The high contribution
from CH fragments to the OA may be from aliphatic carbon chains
from unburned-­or thermochemically converted wax, in accordance
with Fine et al. 25 The extinguishing smoke in Figure 6 shows clear
signal at m/z 60 (C2H4O2+) and m/z 73 (C3H5O2+), which commonly
are associated with anhydrous sugars, such as levoglucosan, emitted
from the pyrolysis of cellulose in biomass and are marker ions for
wood smoke.44 The wicks are made of cotton, a biomass consist-
ing of almost pure cellulose. These ions may also have contributions
from carboxylic acids,44 and have been found in the frying of meat
with a content of fatty acids and other cooking events.45,46
 |

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2044 ANDERSEN et al.

Our results suggest that organic aerosol emissions from candle
extinguishing may contain pyrolysis products from cotton in the
wick in addition to the evaporated and pyrolyzed wax components
that were previously reported by Fine et al. 25
F I G U R E 5 Concentrations of organic aerosol (SP) versus
rBC+ during peak emissions in above flame measurements. The
gray scale indicates the polycyclic aromatic hydrocarbon (PAH)
concentration measured with AMS
3.10 | Estimated concentrations from stressed
burning of candles in a 90 m2 apartment on the
basis of EFs
Table 5 provides estimated concentrations of PM2.5, EC, NO2, and
particle-­ and gas-­phase PAHs after burning 5 candles for 3.5 h at
stressed burn conditions in a 90 m2 apartment with all doors open
and a ceiling height of 2.4 m. An air exchange rate of 0.5 h−1 was as-
sumed, and a loss rate of 0.5 h−1 was used attributed to losses due to
deposition onto surfaces in indoor environments. No loss rate was
applied to the NO2 concentrations and gas-­phase PAH (PAHgas). The
highest (candle 5) and lowest (candle 4) emitting candles with re-
spect to eBC were used for the estimation as examples of high and
low emission scenarios.
In the high emission scenario, the PM2.5 and NO2 concentrations
would reach 70 and 38 µg m−3, respectively, and in the low emissions
scenario 8 and 26 µg m−3, respectively. The WHO air quality guide-
lines for PM2.5 are 25 µg m−3 as a 24 h average and 10 µg m−3 as a
yearly average. For NO2, the guidelines are 200 µg m−3 as an hourly
average and 40 µg m−3 as a yearly average.47 The high emission sce-
nario thereby exceeds the concentration of 25 µg m−3 of PM2.5 in the

F I G U R E 6 Mass spectra measured above the flame measurement of candle 2 during flickering (left) and during extinguishing of candle 2
(right), measured with AMS in dual vaporizer mode. The spectra show the HR organic mass spectrum divided into groups depending on the
elemental composition with Cx representing the carbon ions (black), CH representing the hydrocarbon ions (green), CHO representing the
organic ions with one oxygen atom (purple), and CHOgt1 representing the organic ions containing more than one oxygen atom (magenta)

TA B L E 5 Estimated concentrations, on the basis of emission factors, of PM2.5, EC, NO2, PAHs in the gas-­phase and in particles, and the
benzo[a]pyrene equivalent (BaP eq.) concentrations of gas and particle-­phase PAHs in a 90 m2 apartment after 3.5 h of burning 5 candles at
stressed burn conditions, with an air exchange rate of 0.5 h−1, particles and particle-­phase PAH (PAHparticle) losses of 0.5 h−1

BaP
PM2.5 EC NO2 PAHparticle PAHgas PAHparticle+gas eq.particle+gas

µg m−3 µg m−3 µg m−3 ng m−3 ng m−3 ng m−3 ng m−3

Low emissions 8 0.8 26 0.6 24.1 24.7 0.01

(candle 4)
High emissions 70 72 38 13.4 12.9 26.3 0.10
(candle 5)

No losses were applied in the estimation of NO2 and gas-­phase PAH (PAHgas). The two scenarios represent the minimum (candle 4) and maximum
(candle 5) emissions with respect to eBC.

ANDERSEN et al.
hours of candle burning, but as a single source, it does not exceed
−3
the 24 h 25 µg m average in the given scenario.
It should be pointed out that burning candles are not the only
possible source of particles indoors. It is just one type of indoor
source that contributes to the existing levels indoors, which depends
on the infiltration of outdoor particles (which in turn depends on
the outdoor concentrations, the building envelope, ventilation, and
type of airing practices) and contributions from other indoor sources
such as cooking, smoking, and use of cleaning products. Average in-
door PM2.5 concentrations reported in Scandinavia range from 9.2
to 12.2 µg m−3.48-­53 Therefore, burning candles especially in the case
of the high emission scenario represent a significant contribution to
exposure to particles indoors. Candle burning is an episodic event
that generates high peak concentrations. How frequently these
peaks occur (ie, how frequently candles are burned) depends on the
occupants' habits and vary to a high degree. However, the duration
of elevated concentrations after the candle burning ceases, depends
on the ventilation and airing practices, and in cases with low air ex-
change rates, the elevated concentrations were observed 12.5 h
after the indoor source ceased.54
The NO2 concentrations in both scenarios are well below the
hourly average of 200 µg m−3. However, both scenarios would con-
tribute to NO2 exposures.
Elemental carbon concentrations were estimated to reach 0.8
and 72 µg m−3 in the two scenarios. For comparison, the highest aver-
age personal BC exposures in Stockholm during transport have been
measured to 2.7 µg m−3 during bus transportation.55 Thus, the high
emission scenario would especially add to peak exposures of BC.
The highest air PAH concentrations, a total of 16 US EPA PAHs,
obtained for the two scenarios (Table 5) are equal to those reported
for urban outdoor and indoor air in Gothenburg, Sweden56,57 and
indoor in a rural area where wood combustion for domestic heat-
ing is common,58 and moreover, in restaurant kitchens in Sweden.59
However, the calculated levels of BaP levels in both cases are
below the level set by the WHO as an air quality guideline (0.1 ng
m−3). 22 The European Community has suggested the BaP eq. on
PM10 at an annual standard in ambient air of 1 ng m−3.60 The cancer
potency values in this study were well below those stipulated values.
The concentrations provided in Table 5 were estimated on
the basis of conditions that were considered possible to occur in
Scandinavian homes. The estimated concentrations are both depen-
dent on the number of candles burned, the volume of the apartment,
the air exchange rate, and the level of stressed burn. Burning only
one candle for 3.5 h at the conditions described above would thus
result in five times lower emissions than those presented in Table 5.
However, situations of burning more than five candles or burning
candles in significantly smaller rooms (eg, in the bathroom) are also
common and would generate higher concentrations than presented
in Table 5. In restaurants, the burning of one or more candles per
table in volumes that are comparable or smaller than the volumes
described above are not unusual. Furthermore, the air movements
by door opening, people passing by and talking in near proximity to
the candles are likely to create stressed burning conditions.
|
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2045
3.11 | Limitations
Offline sampling was performed from 0.5 h into the experiment and
did not capture elevated emissions within the first 30 min in the case
of some candle types. Because of this, the presented emission fac-
tors based on offline analysis are underestimated. We have studied
only five different types of pillar candles, with specific wax and wick
composition provided by the manufacturers involved in the study.
Thus, our study captures only a fraction of a vast variety of candle
types available on the market regarding wax and wick composition
and shapes. The degree of stress candles are exposed to from ambi-
ent air movements will vary in different environments. We used one
level of stressed burn in this study. The emission factors of EC in this
study were in between those found for steady burn and stressed
burn in previous studies. However, a direct comparison cannot be
made because the emissions are also affected by the candle shape.
Different candle shapes (eg, tapered candles) have been used in
most of the previous studies. In addition, in the above flame meas-
urements, only one measurement was made for candles 2, 3, and 4,
making uncertainty estimation not possible.
4 | CO N C LU S I O N S
The aerosol particle emissions during stressed burn were investi-
gated for five types of pillar candles with different wax-­wick com-
position. For all five candle types, the particle mass emissions were
dominated by eBC (EC), with minor contributions from inorganic and
organic carbon fraction of PM. The five types of candles showed
variations in emission factors of PM2.5, eBC, and particle PAHs as
well as strong variations in the emission time profiles, when burned
at similar stressed burn conditions. This highlights the importance of
the combination of wax and wick composition to obtain the lowest
possible emissions of eBC, PM2.5, and particle-­phase PAHs. It also
highlights the importance of including the entire burn time in the
evaluation of candle particle emissions, since the average emissions
are affected by the burn time.
Particle size distribution analysis over an extended size range
showed two distinctly different particle types. UFPs below 100 nm
dominated the number emissions in all experiments. The UFP mass
showed strong correlations with the inorganic PM mass from chemical
analysis. UFPs dominated mass emissions during steady burn. During
stressed burn, a larger sized soot mode of eBC (EC) particles, emitted
in addition to UFPs, dominated the mass emissions for all candles.
Measurements directly above the flame showed empirical evi-
dence of short-­lived very strong emission peaks of soot particles.
This provided new fundamental knowledge on the emission mecha-
nisms and dynamics during stressed candle burning, that can be used
in the future formulation of candles with further reduced emissions
during stressed burn. When the candles were extinguished by using
a snuffer to intentionally minimize emissions (in line with recom-
mendations by candle manufacturers), a peak emission of OA was
observed. The OA mass spectra from extinguishing showed markers
 |
2046
of wick pyrolysis products in addition to the previously reported wax
components.
The results reported in this research showed highly correlated
co-­emissions of the health-­relevant particle components eBC, OA,
and PAHs when the candle flame was stressed. This was observed
for both chamber measurements and measurements directly above
the flame. An implication from this is that the emissions of all these
three components increase under stressed burn conditions, and that
the emissions can be significantly reduced by limiting stressed burn
conditions. For all candles, NOx, gas-­phase PAHs, and formaldehyde
did not show clear emission trends from the influence of fluctuating
air velocities, wax and wick composition, or burning mode (stressed
or steady burn). The results show that the burning of candles at
stressed conditions in indoor environments is likely to significantly
add to the exposure to soot (measured as eBC or EC), PM2.5, particle
PAHs, and NOx.
AC K N OW L E D G E M E N T S
This study was conducted as part of the Innovation Fund Denmark
project CANdle Development for Low Emissions (2017–­2020). We
thank Innovation Fund Denmark (www.innov​ation​sfond​en.dk) and
Ergonomics and Aerosol Technology at Lund University for fund-
ing. The project consortium is made up of the following partners:
Danish Technological Institute, Lund University, Aarhus University,
ASP-­Holmblad A/S, Coop Denmark A/S, Danwax ApS, European
Candle Association ASBL, Liljeholmens Stearinfabriks AB, and
Promol -­Industria de vesla S.A. The candles used were provided by
the industrial partners. We thank all partners in the consortium for
discussions. We acknowledge Karin Lovén for performing the OC/
EC analysis at Lund University.
C O N FL I C T O F I N T E R E S T S
The authors declare no competing interests.
AU T H O R C O N T R I B U T I O N S
CA, AW, JP, MB, MG, and MK responsible for conceptualization. CA,
YO, and BS responsible for formal analysis. JP, AW, MB, MG, and MK
responsible for funding acquisition. CA, YO, SNS, BBR, MNB, MK,
and KW responsible for investigation. CA, AW, and JP responsible
for methodology. AW responsible for project administration. AW, JP,
MB, and MG responsible for resources. AW, JP, MB, and MG respon-
sible for supervision. CA, AW, and JP responsible for validation. CA
and YO responsible for visualization. CA wrote the original draft. All
authors contributed to writing review and editing.
ORCID
Yuliya Omelekhina https://orcid.org/0000-0001-6611-1801
Merete Bilde https://orcid.org/0000-0002-2112-514X
Aneta Wierzbicka https://orcid.org/0000-0002-0678-7161
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2048 ANDERSEN et al.

60. Commission E-­E. Directive 2004/107/EC of the European

Parliament and of the Council of 15 December 2004 relating to How to cite this article: Andersen C, Omelekhina Y,
arsenic, cadmium, mercury, nickel and polycyclic aromatic hydro-
Rasmussen BB, et al. Emissions of soot, PAHs, ultrafine
carbons in ambient air. Off J Eur Union L. 2004;23:3-­16.
particles, NOx, and other health relevant compounds from
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S U P P O R T I N G I N FO R M AT I O N
2021;31:2033–­2048. https://doi.org/10.1111/ina.12909
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