Fine Particulate Matter Emissions from Candles

Zhishi Guo and Ronald Mosley
U.S. Environmental Protection Agency, Office of Research and Development, National Risk
Management Research Laboratory, MD-54, Research Triangle Park, NC 27711

Jenia McBrian and Roy Fortmann
ARCADIS Geraghty & Miller Inc., P.O. Box 13109, Research Triangle Park, NC 27709

ABSTRACT

Five types of candles purchased from local stores were tested for fine particulate matter (PM)

emissions under close-to-realistic conditions in a research house. The test method allows for

determination of both the emission rate and deposition rate. Most tests revealed low PM

emission rate except two, in which excessive sooting occurred and the PM concentration

approached 1000 |ig/m3 with six and nine burning wicks, respectively.  Wax breakthrough

significantly increased the PM emission rate. Smoldering generated more fine PM than several

hours of normal burning, causing very high concentrations in a short period of time, which raises

concern over potentially acute health effects, especially for children and the elderly. A simple

source model is proposed to represent both stable PM emissions during normal combustion

conditions and the sudden concentration surge following flame extinction.

INTRODUCTION

Candles have been associated with human living conditions for at least 1000 years.  Although no

longer a major means of lighting in modem society, they are still widely used in homes, mostly

for creating unique, warm, and tranquil atmospheres. It was believed from observation that the

candle flame produces carbon particles and that, under perfect combustion conditions, the carbon

is totally consumed by the flame. In his famous book The Chemical History of a Candle,

originally published in 1861,1 Michael Faraday — one of the greatest experimental scientists of
                                     1

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all time -- uses simple, yet very ingenious, experimental methods to prove that carbon particles




exist in the candle flame and that it is these solid particles that create "the very beauty and life of




the flame." He further points out that, under imperfect combustion conditions, the carbon




particles cannot be consumed entirely by the flame, resulting in emissions of soot.




In recent years, concerns over the impact of candle burning, especially the property damage they




may cause due to soot deposition, have been on the rise.23'4'5 Analysis of the potential impact on




human health due to inhalation of particulate matter (PM) has also been reported,5 According to




the study by Fine et al.,2 a sooting flame and a smoldering wick produce much higher fine




particle mass emission rates than a quiet normal burning candle and are responsible for the vast




majority of fine particle emissions from this source. Another human-health-related issue




associated with candle burning is the inhalation of particlebome lead (Pb) generated by certain




types of candles, whose wicks have a lead core.6'7




This paper investigates the PM emissions from candles under close-to-realistic conditions and




their contribution to indoor PM levels with emphasis on the fine fraction of the PM — particles




having aerodynamic diameters of less than 2.5 jam (PM2.5).  The goals were to: identify the




emission patterns, measure the emissions under certain real-life scenarios, and determine the key




parameters needed for estimating inhalation exposure.




EXPERIMENTAL





Test Facility




Emissions tests were performed in a research house located in Gary, NC.8  One bedroom, used as




a test chamber, was isolated from the rest of the house by blocking the air supply registers and




closing the interior door. The room has dimensions of 3.78 (length) x 3.28 (width) x 2.44

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(height) m. It has vinyl flooring, painted gypsum board walls, and a textured gypsum board




ceiling. The particle-free air supply was generated by an in-line fan (FanTeck Model FR250, 230




W), which passed outdoor air through a high efficiency particle air (HEPA) filter into the test




room, keeping the room under slightly positive pressure (~2 Pa) to prevent the infiltration of




particles from the outdoors and adjacent rooms. Prior to a test, a stand-alone HEPA filter air




cleaner (Bionaire, Model CH-3580 or Honeywell  Enviracaire, Model 13520) operated inside the




test room for 30 minutes to reduce the background fine PM concentration to less than 2 fig/m3,




A ceiling fan was used to keep the room air well mixed. The test candles were placed on a table




away from the direct air draft created by the ceiling fan. Under the standard test conditions, the




ceiling fan was set at low speed and normal wind  direction (i.e., downward), which gave an




average air speed of 11 cm/s near the top of the candle ~ close to the air speed commonly found




in indoor environments. Other speed/direction combinations of the ceiling fan provided an air




speed range from 14 to 27 cm/s near the candle. When the fan was turned off, the air speed was




reduced to less than 5 cm/s.  Additional discussions of this test facility can be found in these




proceedings.9




Test Specimens




       All candles tested were purchased from local stores and are described in Table 1.

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Table 1. Description of test candles!
Sample ID
PI
P2
P3
BW1
BD1
Type
paraffin/aroma
paraffin/aroma
paraffin/aroma
beeswax
birthday candle b
Shape of
Cross Section
square
square
round
round
round
No, of Wicks
9
9
3
1
1
Color
orange
red
mauve
yellow
white
   a PI and P2 are made by the same manufacturer,
   b Material type was not mentioned on the label.
PM Sampling

Particles with aerodynamic diameters of less than 10 \im (PM10) and less than 2.5 jim were

sampled simultaneously onto Teflon filters, using cyclones (University Research Glass) with

corresponding size cut-points.  Each cyclone has a two-stage filter pack (47-mm, R2PJ047). The

mass concentrations of PM25 and PM 10 were determined gravimetrically. The PM size

distribution and real-time concentration were determined with an electric low pressure impactor,

or ELPI (Dekati Ltd.)10, which measures an aerodynamic diameter range from 0.03 to 10 urn

with 12 stages, and has a response time of 5 sec while experiment data were recorded every 60

sec.

Test Method

The ELPI was used to monitor the indoor PM concentrations throughout the experiment. After

the room was pressurized and the background PM concentration reduced to less than 2 [o.g/m3, the

test candle was lit with a butane lighter. Matches were used to light the birthday candles.  The

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burning duration was 8 minutes for the birthday candles and 4 to 6 hours for the other candles.




In the latter case, the candles were allowed to burn for 1 hour before filter sampling. After the




test candles were extinguished, the EPLI continued to operate for at least 4 more hours. Sulfur




hexafluoride (SF6) tracer gas was injected after the extinction of the flame to determine the




ventilation rate and the PM deposition rate.  No SF6 was injected prior to or during the burning




period because of possible decomposition of SF6 when in contact with a flame, resulting in




interferences."




RESULTS





Correlation Between the Gravimetric Method and ELPI




Comparison of paired fine PM concentration data showed that, in the low concentration range (<




5 M-g/m3), the two methods agree with each other reasonably well and that the ELPI gave higher




readings as the concentration increased (Figure 1). A good correlation exists between the two




methods, however.  In this paper, all the ELPI data were corrected based on Equation 1 :




Equation 1. Correlation between the gravimetric method and ELPI for fine PM concentrations




       In C    =  0.829 In CELPI - 0.475     (r2 = 0.967, n = 14)
where  Cg^ = fine PM concentration from the gravimetric method (p.g/m3), and




       CELPI = fine PM concentration from the ELPI

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Figure 1. Correlation between the gravimetric method and ELPI for fine PM
        1E4
   J:   1E3-
   O)
   ZL

   •c   1E2
   -i—>
   

   6


        1EO-
           1EO
1E1           1E2           1E3
           ELPI (MQ/m3)
1E4
PM Concentrations and Emission Rates by the Gravimetric Method


The average concentration and emission rate calculated from the filter samples are presented in


Table 2. In most cases, the fine PM concentration was low except in two tests for candle P2, in


which excessive sooting occurred and the fine PM concentration reached 955 and 1137 ng/m3,


respectively. These unusually high concentration results were supported by the ELPI data. A


higher burn rate in test C121499 is another indication of possible imperfect combustion.


However, no visual observations were made during these tests and we were unable to determine
the exact causes of the high emission rates.

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Table 2. Average fine PM concentrations and emission rates based on filter samples
Test
Candle
PI
P2





P3

BW1
Test
ID
C121399
G121699
C121499
C121599
C121799
C041100
C041200
COS 1600
COS 1700
C041700
Wicks
Lighted
9
9
9
6
1
1
1
9c
9C
1
Burn Rate
(g/h/wick)
2.77
3.71
4.67
NAb
2.29
3.33
2.50
3.89
4.00
7.86
Air Speed ACH Concentration
(cm/s) (h-1) (lJ.g/m3)
11
<5
11
11
14
15
27
11
11
14
0.99
0.95
0.98
0.93
1.1
1.56
1.51
1.54
1.5
.1.45
99.6
13.0 a
955
1137
15.8
8.79
8.13
14.9
17.3
4.32
Emission Rate
(^g/h/wick)
329
41
3120
5287
521
411
368
76
87
188
a This value is based on the ELPI data. The result from filter samples was discarded because the
relative standard deviation for duplicate samples was too large.
b Burn rate was not measured in this test.
c Three 3-wick candles.
PM Size Distribution

Most particles emitted from candles were in the fine particle size range.  This is evidenced by the

fact that the filter samples for PM2.5 and PM10 taken in parallel are almost the same in most tests

(Table 3). Typical size distribution for fine PM is shown in Figure 2.  Like some other

combustion sources, two peaks appear in the size distribution.  Although smoldering creates

more larger particles, the shape of the distribution curve did not change significantly.

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Table 3. Comparison of filter samples for PM25 and PMi0
Concentration (|ig/m3) a
PM2J
2.7 ±0.5
8.1 c
10.3 ±0.4
14.9 ±4.6
15.8 ±3.0
17.3 ±1.1
29.2 ± 2.5
49.8 ±1,7
99.6 ± 2.5
955 ± 3.2
1137 ±248
PM10
3.4 ±0.2
8.6 c
11.3 ±0.9
15.2 ±5.1
16.7 ±1.5
18.5 ±1.4
29.1 ±0.1
50.8 c
99.6 ± 2.5
951 ±20.2 :'
1128 ±86.7
Percent
Difference b
23.7
5.5
9.8
1.9
5.1
7.1
-0.5
2.0
0.0
-0.5
-0.8
                  2 Mean ± standard deviation for duplicate samples.
                  b Percent = 2 x (PM10 - PM2.5) / (PM10 + PM2.5) x 100.
                  c Single filter sample.


Figure 2. Fine PM size distribution observed in test COS 1600
                             0.1                      1
                            Aerodynamic Diameter (jjm)
10
                              Normal Burn-e- Smoldering
                                   8

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Emission Patterns




General Emission Patterns




The real-time concentration data from the ELPI were used to determine the PM emission




patterns. In most cases, the fine PM emission rate was fairly steady during the normal burning




period.  However, the emission rate was higher immediately after the candle was lit. Two




slightly different emission patterns are shown in Figures 3 and 4. In both cases, a concentration




surge occurred when the flame was extinguished.  In most tests, the smoldering period generated




more particles in a few seconds than during the whole period of normal burning.  Emissions due




to smoldering are discussed further in the following section. Also note that the emissions data




from filter samples presented in Table 2 do not include the smoldering period because the




sampling pumps were turned off before the candles were extinguished.

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Figure 3. Fine PM concentration profiles for candle P3 in duplicate tests
        0
8
                                 Elapsed Time (h)
                                  10

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Figure 4. Fine PM concentration profile for candle P2 in test C121699
     100
 x~,  8°

 1
 "a*  eo
 0-  40
  
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where  Wx = amount of fine PM emitted during smoldering period (|J.g), Q = ventilation flow rate




       (m3/h), C = fine PM concentration (p.g/m3), t = time (h), V = room volume (m3), tx = time




       at which the flame is extinguished (h), and t,, = time for the last data point (h).




The time-concentration curve was integrated using the trapezoidal rale, and the calculated




emissions from smoldering are presented in Table 4.  It appears that candle P3 emits more fine




PM during the smoldering period than the other two paraffin candles, although it emits less




during the normal burning period (see Table 2). Results in Table 4 also suggest that using a




snuffer to extinguish the flame produced less PM than blowing out the flame.  Blowing out 30




birthday candles produced the highest fine PM concentration in the room (about 500 [ig/m3 in the




mixed air), and the concentration remained above 100 [ig/m3 for more than an hour (Figure 5).




Table 4. Amounts of fine PM emitted due to smoldering
Test ID
C121399
C121699
COS 1900
COS 1600
COS 1700
C052300
COS 1900
C041700
C050800
Candle
PI
P2
P3
BW1
BD1
Number of
wicks
9
9
9
9
9
9
9
1
30
Extinguishing
Method
blowout
blowout
blowout
blowout
blowout
blowout
snuffer
blowout
blowout
Peak Cone.
(|ig/m3)
144
88.3
153
257
250
213
82
32.5
483
Emissions
(Hg/wick)
273
261
262
609
650
554
115
816
151
                                        12

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Figure 5. Fine PM concentration profile for lighting and blowing out 30 birthday candles
     500
       0
          0
50              100             150
        Elapsed Time (min)
200
Emissions after Wax Breakthrough

Wax breakthrough occurs when the rim of the solid wax surrounding the liquid pool softens from

the heat of the flame and slumps off to one side of the candles, causing the release of the liquid

wax from the pool that has concentrated around the wick.  It is one way to cause imperfect

combustion.  Wax breakthrough occurred in one test with candle P3.  As shown in Figure 6, a

higher emission rate resulted.
                                      13

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Figure 6, Effect of wax breakthrough on fine PM emissions (test COS 1800)
        160
      JT120
      Q_

      CD
      C

      LJ.40
                                                           Blowout
Breakthrough
                                468
                                   Elapsed Time (h)
                             10
12
PM Deposition Rates


PM deposition rate is an important parameter to estimate the PM concentrations from indoor air


quality simulation. In this work, the decay part of the ELPI data (i.e., after the candle was


extinguished) was used to estimate this parameter. The first-order deposition rate constant was


calculated by comparing the decay rate for PM with that for the tracer gas. As shown in Figure


7, a U-shaped curve was obtained. Note that the emission rate data presented in Table 2 do not


consider PM deposition and thus should be considered as the lower bound of the actual emission


rate.9
                                      14

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Figure 7. First-order deposition rate constants for test C121699
         0
         0.01
  0.1                    1
Aerodynamic Diameter (|jm)
10
                                      Data
                      Best Fit
MODELING CONSIDERATIONS

Source Model

Considering the unique emission pattern for PM emissions from candles, an average emissions

rate may not be adequate for exposure estimation, especially when acute health effects are of

concern. A simple model, represented by Equations 3 and 4, is proposed to account for

emissions for both normal burning and smoldering:
                                    15

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Equations 3 and 4. Model for PM emissions from candle burning
       D _  D
       -K- — JV.
for to < t < tx
       AC =
             W.
att =
where R = PM emission rate (jJ-g/h), R,, = constant emission rate during the normal combustion


      period from to (burning start time) to t,; (M-g/h). and AC = an instant increase of PM


      concentration in room air at I* (jag/m3).


This model can be easily implemented in a spreadsheet or an indoor air quality simulation


program. An example application of this model is shown in Figure 8.


Figure 8. Modeling of test C051700 using Equations 3 and 4 as a source model
       300
     Q_
     LL
           0
    24           6           8
               Elapsed Time (h)
10
                                    16

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PM Accumulation on Interior Surfaces


With knowledge of both the emission rate and deposition rate, the amount of PM deposited on


interior surfaces can be estimated from Equations 5 and 6. An example simulation shown in


Figure 9 represents a simple case, in which all interior surfaces are treated as the same type and


an average deposition rate constant of 0.4 h"1, which is equivalent to a deposition velocity of 0.2


m/h in the test room, was used for fine PM.


Equations 5 and 6. Estimation of PM deposition on interior surfaces



         dC
       V-r=R
          ai
       dM-
       	'_ 	 r>
            — JLJ,
        dt
where  n = number of interior surface types, S; = area of surface i (m2), Df = PM deposition


       velocity for surface i (m/h), and M; = amount of PM accumulated on surface i
                                       17

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Figure 9. An example simulation of PM accumulation on interior surfaces in the test room
     250
       0
         0
4            6
Elapsed Time (h)
8
10
CONCLUSION

Under normal combustion conditions, the candles tested do not produce significant amounts of

particles — the average PM2,5 emission rate ranges from 41 to 521 jig/h/wick. Excessive sooting

occurred in two tests with average PM2,5 concentration approaching 1000 (J,g/m3 and an emission

rate in the 3000 to 5000 (ig/h/wick range. However, the exact cause of sooting is not clear.

Smoldering often generates more particles than several hours of normal burning. The amount of

PM2-5 emitted from extinguishing the flame ranges from 115 to 569 |ig/wick. In a similar test
                                     18

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with 30 birthday candles, the peak fine PM concentration was near 500 |J,g/m3 after extinguishing




the flames. Given the dramatic concentration surge due to smoldering, using an average




emission rate to represent the fine PM emissions from candles may not be adequate for exposure




estimation in some cases, especially when acute health effects are of concern.  As a first




approximation, a combination of constant and instant source models is recommended.




REFERENCES





1. Faraday, M. The Chemical History of a Candle; originally published in 1861; reprinted by




Cherokee Publishing Company, Atlanta, GA, 1993.




2. Fine, P. M.; Cass, G. R.; Simoneit, B. R. T. Environ, Sci. & Techn.1999, 33, pp 2352-2362.




3. Krause, D. In Indoor Environment: the State of the Industry, Presentations from the 7th Annual




Indoor Environment Conference, IAQ Publications, Inc.; Bethesda, MD, 1999; pp 157-159,




4. Al-Ahmady, K. In Indoor Environment: the State of the Industry, Presentations from the 7th




Annual Indoor Environment Conference, IAQ Publications, Inc.: Bethesda, MD, 1999; pp 159-




164.




5, Krause, J. D. Characterization of scented candle emissions  and associated public health risks,




Master's thesis, University of South Florida, Tampa, FL, 1999.




6. Alphen, M.  The Sci. of the Total Environ. 1999, No. 243/244, pp 53-65.




7. Nriagu, J. O.; Kim, M. The Sci. of the Total Environ., 2000, No. 250, pp 37-41.




8. Jackson, M. D.; Clayton, R. K.; Stephenson, E. E.; Guyton, W. T.; Bunch, J. E. EPA's Indoor




Air Quality Test House, I,  Baseline Studies, in Proceedings of the 1987 EPA/APCA Symposium,




Research Triangle Park, NC, May 3-6,1987, Environmental Monitoring Systems Laboratory,




Research Triangle Park, NC, EPA-600/9-87-010 (NITS PB88-113402), 1987.
                                     19

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9. MeBrian, J.; Fortmann, R,; Guo, Z.; Mosley R. Test methods to characterize particulate matter




emissions and deposition rate in a research house, in these proceedings.




10. Marjamaki, M.; Keskinen, J.; Chen, D. R.; Pui, D. Y. H. J. Aerosol ScL, 2000,31, pp 249-




261.




11. Fisk, W. J.; Wallman, P. H.; Prill, R. J.; Mowris, R. J.; Grimsrud, D. T. Lawrence Berkeley




Laboratory Report, LBL-24216, Berkeley, CA, 1988, pp 6-25.
KEY WORDS




indoor air, candles, soot, emissions, particulate matter
                                       20

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 NRMRL-RTF-P-527
                                TECHNICAL REPORT DATA
                          (Please read /xstmctiora on the reverse before completing}
i. REPORT NO.
     EPA/600/A-00/056
                            2.
4. TITLE AND SUBTITLE
 Fine Partieulate Matter Emissions from Candles
                                                       3. REC
                                                       S. REPORT DATE
                                                       6. PERFORMING ORGANIZATION CODE
7.AUTH0R(s) z
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