SUZUKI
Tohoku
J. exp. Med.,
Mercury
1976, 119, 353-356
in Cigarettes
TSUGUYOSHI SUZUKI, URUSHIYAMA
SACHIKO
SHISHIDO
and
KENJI
Department of Public Health, Tohoku University School of Medicine, Sendai
, Tohoku
J.
and
foreign brand
the
was and
about
30 ƒÊg
released
in
of in
about
a
URUSHIYAMA,
353-356
by
a
by
domestic
piece
of
products.
In
tobacco
leaf
foreign
products.
5-7 ƒÊg
of
about
By
mercury
the
and
the
in
the
of
only
inorganic in
tobacco
products
length
of
a
collected
amount
domestic
smoke.
domestic
sample was
paper,
unit
Cigarettes. of
smoke
Its
60 ƒÊg
burning, into
and
and
in
cigarettes
method,
machine
was
Mercury in
and
cigarette
foreign
Magos'
smoking
mercury.
both
K.
Mercury
measured
burned of
found
and
(4),
was
was
paper
S.
119
measurement
mercury leaf
SHISHIDO, Med.,
products
domestic for
T.,
exp.
a
mercury;
and
cigarette cigarettes;
smoking.
In
view
of
0.2-2.0 ƒÊg/g et
al.
mercury
1973),
the
report
in
domestic
it
was
planned
that
the
total
products
and
to
examine
mercury
concentrations
0.08-0.34 ƒÊg/g the
contribution
in
in foreign of
cigarettes products
smoking
to
were (Fujii human
uptake.
SAMPLES AND METHODS July
Cigarettes of different brands were purchased from ordinary 1975. All the cigarettes purchased were filter-cigarettes.
retailers
in Sendai
City in
Organic mercury and inorganic mercury were separately measured by Magos' method (1971) in the samples of tobacco leaf, paper and filter. Samples were homogenized in a solution of 45% NaOH and 1% L-cysteine-HCl by glass homogenizer, and the homogenate was measured by flameless atomic absorption spectrometry. To measure the amount of mercury in smoke, a simple smoking machine (Fig. 1) was used. The mercury in smoke was trapped in two serially connected impingers containing each 8 ml of the solution of 1 N H2S04 and 0.5% KMnO4. After smoking experiments, mercury was found only in the first impinger. Smoking experiments were repeated twice: in the first experiment, puff (drawing-in) volume, puff frequency, puff (drawing-in) duration, and smoked length of cigarettes were 100 ml, 0.5/min, 10-15 seconds, and 2.5 3.5 cm, respectively, and in the second experiment, those were 35 ml, 1/min, 2-3 seconds, and 5 cm. After smoking by the machine, butt (leaf and paper), filter, and ash (a collection from 3 or 5 smoked cigarettes) were measured in a way similar to the case of non-smoked cigarettes. The solution of mercury trap was measured after addition of a slight excess of 20% hydroxylamine hydrochloride solution. Received
for publication,
March
10, 1976. 353
354
T. Suzuki
et al.
Fig. 1. A smoking machine used for the present experiment. Lighted cigarettes were puffed by drawing out the piston of glass syringe (the volume was 100 ml) up to a fixed volume, disconnecting the syringe from the impinger, drawing in the piston to the syringe, and connecting again the syringe to the impinger. All procedures were manually conducted. Mercury in smoke was trapped into the solution of 1 N H2S04 and 0.5% KMnO4 in the impinger (the volume was 20 ml).
RESULTS
Mercury in non-smoked cigarettes (Table 1) Organic mercury was not found in any samples. Domestic products had significantly greater amounts inorganic
mercury
in tobacco
leaf,
and
filter,
but
not
and
concentrations
in paper,
than
of
foreign
products.
Mercury in smoke (Table 2) used
Organic mercury was detected only in the filter of cigarettes from the package for the experiment 1. Organic mercury was, however, disregarded in the TABLE 1.
Inorganic
mercury
in non-smoked
cigarettes
Numerals in the table are mean+standard deviation. n.s.: not significant. Each one cigarette was sampled from a package of different brands such as "Peace", "Marina" , "Hi-lite", "Seven Stars", "Luna", "Cherry" and "Hope" in the case of domestic products, and "No. 6", "Atika", "Winston" and "Rothman" in the case of foreign products.
Mercury
TABLE 2.
Numerals
in the
the mean "Peace"
in Cigarettes
355
Mercury in cigarettes before and after smoking
table
are
the
of 5 cigarettes in in both experiments
mean
the
of 3 cigarettes
experiment
2.
. Experimental
in the The
experiment
brand
conditions
of
are
1, and
cigarettes
described
is in the
text.
I-Hg: inorganic mercury; O-Hg: orgnanic mercury; n.d.: not detected; no measurement. * Leaf and paper. f Calculated values.
smokiug experiment, because the compound any meaniug for mercury uptake of man.
contained
-.
in the filter would
not have
Accordiug to the smoked leugth of cigarettes, the amount of mercury in smoke varied from 13.9 to 34.3 ng. The unit leugth (1 cm, ca. 140 mg of leaf and 6 mg of paper) of cigarettes, when smoked, released about 5 ng of mercury into smoke in the experiment 1, and 7 ng in the experiment 2. DISCUSSION Mercury
concentrations
1.0-2.0 ƒÊg/g were
for
in total
1966
from
each
their
with
the
mercury
in
the
mercury
other
chemicals
decrease enactment
of
results
of
the
present
results
of
this
much
disinfectants in
such
are
the
been as
leaf.
than
Since by
in
is
have
organophosphorus
concentrations
and
study
should
tobacco
et
Thus,
lower
recommended
had
(Fujii
paper,
measurement.
has
mercury
leaf,
the
contamination disinfectants
tobacco
1971
in
seed
seed
filter
and
cigarettes in
other
present
Mercury-containing
domestic
0.2-1.0 ƒÊg/g
mercury,
separately data
in
to
the
the
leaf
from
1973).
about
These
filter
were
the
direct
impossible,
not
results examined
comparison
but
the
levels
data
reported
previously.
been
an
important
source
1967
the
use
government
compounds tobacco
decreased al.
is
of to
or considered
be
of
of
mercurials
as
replaced
by
antibiotics. as
of
a
The result
of
recommendation.
Domestic products have than foreign products.
shown higher levels of mercury in tobacco leaf and The cause is not clear, but the mercury-containing
356
T. Suzuki
fungicide
et al,
is a suspect.
The release of mercury into smoke is primarily a function of mercury concentrations in tobacco leaf and paper, but physico-chemical properties of cigarettes and smoking habits of individual smokers influence the amount of smoke produced as well as the release of mercury into smoke. In the present results, the filter attached to cigarettes was partly effective in trapping mercury, but the amount of mercury found in smoke was 30-50% of the total amount contained in the entire leaf and naner of a cigarette. The
smoke
from
centrated
aerosol,
Hoffmann
1967).
be
vaporized
vapor, of
or
75-85%
mercury
Skerfvine
in
burning which
In
what
combined of
deposited
cigarettes the state
to
mercury may
size
be
is the
exists
chemicals be
retained
smaller
understood
particles
mercury
some will
of
in by in
in
the
as
ranges the
smoke
burning. the
uncommonly
it
is
body,
of
con
(Wynder
is unknown. If
human
state
an
0.1-1.0ƒÊm
aerosol
in
and
and It
may
the
state
the
amount
(Nordberg
of
and
1972).
The daily amount of mercury retained in the body by cigarette smoking will be 336 ng, provided that 20 cigarettes are consumed per day, 60 ng of inorganic mercury are contained in tobacco leaf and paper of a cigarette, 3.5 czn of each piece of cigarettes are smoked, 6 ng of mercury are released in smoke per unit length of cigarettes, and 80% of mercury in smoke are retained in the human body. Needless to say, this single figure is just an approximation based on various assumptive values which do not necessarily represent the standard for individual smokers. Studies on mercury in expired air, and the difference in mercury accumulation between smokers and non-smokers are our next concerns. Acknowledgment This
study
was
supported
by
the
grant
from
the
Ministry
of
Education,
Japan.
References
1) Fujii, M., Kitamura, M. & Kondo, M. (1973) Suigin no bunpu to taikichyu no suigin ni tsuite (Distribution of mercury and mercury in air). Kankyo Hoken Report (Env . Health Report) (Jap.), 26, 5-47. 2) Magos, L. (1971) Selective atomic-absorption determination of inorganic mercury and methylmercury in undigested biological samples. Analyst, 96, 847-853. 3) Nordberg, G.E. & Skerfving, S. (1972) Metabolism. In: Mercury in the Environment, edited by L. Friberg & D. Vestal, The Chemical Rubber Co ., Cleveland, pp. 29-91. 4) Wynder, E,L. & Hoffmann, D. (1967) Tobacco and Tobacco Smoke , Studies in Experimental Carcinogenesis, Academic Press, New York and London .
Tohoku
J. exp. Med.,
Mercury
1976, 119, 353-356
in Cigarettes
TSUGUYOSHI SUZUKI, URUSHIYAMA
SACHIKO
SHISHIDO
and
KENJI
Department of Public Health, Tohoku University School of Medicine, Sendai
, Tohoku
J.
and
foreign brand
the
was and
about
30 ƒÊg
released
in
of in
about
a
URUSHIYAMA,
353-356
by
a
by
domestic
piece
of
products.
In
tobacco
leaf
foreign
products.
5-7 ƒÊg
of
about
By
mercury
the
and
the
in
the
of
only
inorganic in
tobacco
products
length
of
a
collected
amount
domestic
smoke.
domestic
sample was
paper,
unit
Cigarettes. of
smoke
Its
60 ƒÊg
burning, into
and
and
in
cigarettes
method,
machine
was
Mercury in
and
cigarette
foreign
Magos'
smoking
mercury.
both
K.
Mercury
measured
burned of
found
and
(4),
was
was
paper
S.
119
measurement
mercury leaf
SHISHIDO, Med.,
products
domestic for
T.,
exp.
a
mercury;
and
cigarette cigarettes;
smoking.
In
view
of
0.2-2.0 ƒÊg/g et
al.
mercury
1973),
the
report
in
domestic
it
was
planned
that
the
total
products
and
to
examine
mercury
concentrations
0.08-0.34 ƒÊg/g the
contribution
in
in foreign of
cigarettes products
smoking
to
were (Fujii human
uptake.
SAMPLES AND METHODS July
Cigarettes of different brands were purchased from ordinary 1975. All the cigarettes purchased were filter-cigarettes.
retailers
in Sendai
City in
Organic mercury and inorganic mercury were separately measured by Magos' method (1971) in the samples of tobacco leaf, paper and filter. Samples were homogenized in a solution of 45% NaOH and 1% L-cysteine-HCl by glass homogenizer, and the homogenate was measured by flameless atomic absorption spectrometry. To measure the amount of mercury in smoke, a simple smoking machine (Fig. 1) was used. The mercury in smoke was trapped in two serially connected impingers containing each 8 ml of the solution of 1 N H2S04 and 0.5% KMnO4. After smoking experiments, mercury was found only in the first impinger. Smoking experiments were repeated twice: in the first experiment, puff (drawing-in) volume, puff frequency, puff (drawing-in) duration, and smoked length of cigarettes were 100 ml, 0.5/min, 10-15 seconds, and 2.5 3.5 cm, respectively, and in the second experiment, those were 35 ml, 1/min, 2-3 seconds, and 5 cm. After smoking by the machine, butt (leaf and paper), filter, and ash (a collection from 3 or 5 smoked cigarettes) were measured in a way similar to the case of non-smoked cigarettes. The solution of mercury trap was measured after addition of a slight excess of 20% hydroxylamine hydrochloride solution. Received
for publication,
March
10, 1976. 353
354
T. Suzuki
et al.
Fig. 1. A smoking machine used for the present experiment. Lighted cigarettes were puffed by drawing out the piston of glass syringe (the volume was 100 ml) up to a fixed volume, disconnecting the syringe from the impinger, drawing in the piston to the syringe, and connecting again the syringe to the impinger. All procedures were manually conducted. Mercury in smoke was trapped into the solution of 1 N H2S04 and 0.5% KMnO4 in the impinger (the volume was 20 ml).
RESULTS
Mercury in non-smoked cigarettes (Table 1) Organic mercury was not found in any samples. Domestic products had significantly greater amounts inorganic
mercury
in tobacco
leaf,
and
filter,
but
not
and
concentrations
in paper,
than
of
foreign
products.
Mercury in smoke (Table 2) used
Organic mercury was detected only in the filter of cigarettes from the package for the experiment 1. Organic mercury was, however, disregarded in the TABLE 1.
Inorganic
mercury
in non-smoked
cigarettes
Numerals in the table are mean+standard deviation. n.s.: not significant. Each one cigarette was sampled from a package of different brands such as "Peace", "Marina" , "Hi-lite", "Seven Stars", "Luna", "Cherry" and "Hope" in the case of domestic products, and "No. 6", "Atika", "Winston" and "Rothman" in the case of foreign products.
Mercury
TABLE 2.
Numerals
in the
the mean "Peace"
in Cigarettes
355
Mercury in cigarettes before and after smoking
table
are
the
of 5 cigarettes in in both experiments
mean
the
of 3 cigarettes
experiment
2.
. Experimental
in the The
experiment
brand
conditions
of
are
1, and
cigarettes
described
is in the
text.
I-Hg: inorganic mercury; O-Hg: orgnanic mercury; n.d.: not detected; no measurement. * Leaf and paper. f Calculated values.
smokiug experiment, because the compound any meaniug for mercury uptake of man.
contained
-.
in the filter would
not have
Accordiug to the smoked leugth of cigarettes, the amount of mercury in smoke varied from 13.9 to 34.3 ng. The unit leugth (1 cm, ca. 140 mg of leaf and 6 mg of paper) of cigarettes, when smoked, released about 5 ng of mercury into smoke in the experiment 1, and 7 ng in the experiment 2. DISCUSSION Mercury
concentrations
1.0-2.0 ƒÊg/g were
for
in total
1966
from
each
their
with
the
mercury
in
the
mercury
other
chemicals
decrease enactment
of
results
of
the
present
results
of
this
much
disinfectants in
such
are
the
been as
leaf.
than
Since by
in
is
have
organophosphorus
concentrations
and
study
should
tobacco
et
Thus,
lower
recommended
had
(Fujii
paper,
measurement.
has
mercury
leaf,
the
contamination disinfectants
tobacco
1971
in
seed
seed
filter
and
cigarettes in
other
present
Mercury-containing
domestic
0.2-1.0 ƒÊg/g
mercury,
separately data
in
to
the
the
leaf
from
1973).
about
These
filter
were
the
direct
impossible,
not
results examined
comparison
but
the
levels
data
reported
previously.
been
an
important
source
1967
the
use
government
compounds tobacco
decreased al.
is
of to
or considered
be
of
of
mercurials
as
replaced
by
antibiotics. as
of
a
The result
of
recommendation.
Domestic products have than foreign products.
shown higher levels of mercury in tobacco leaf and The cause is not clear, but the mercury-containing
356
T. Suzuki
fungicide
et al,
is a suspect.
The release of mercury into smoke is primarily a function of mercury concentrations in tobacco leaf and paper, but physico-chemical properties of cigarettes and smoking habits of individual smokers influence the amount of smoke produced as well as the release of mercury into smoke. In the present results, the filter attached to cigarettes was partly effective in trapping mercury, but the amount of mercury found in smoke was 30-50% of the total amount contained in the entire leaf and naner of a cigarette. The
smoke
from
centrated
aerosol,
Hoffmann
1967).
be
vaporized
vapor, of
or
75-85%
mercury
Skerfvine
in
burning which
In
what
combined of
deposited
cigarettes the state
to
mercury may
size
be
is the
exists
chemicals be
retained
smaller
understood
particles
mercury
some will
of
in by in
in
the
as
ranges the
smoke
burning. the
uncommonly
it
is
body,
of
con
(Wynder
is unknown. If
human
state
an
0.1-1.0ƒÊm
aerosol
in
and
and It
may
the
state
the
amount
(Nordberg
of
and
1972).
The daily amount of mercury retained in the body by cigarette smoking will be 336 ng, provided that 20 cigarettes are consumed per day, 60 ng of inorganic mercury are contained in tobacco leaf and paper of a cigarette, 3.5 czn of each piece of cigarettes are smoked, 6 ng of mercury are released in smoke per unit length of cigarettes, and 80% of mercury in smoke are retained in the human body. Needless to say, this single figure is just an approximation based on various assumptive values which do not necessarily represent the standard for individual smokers. Studies on mercury in expired air, and the difference in mercury accumulation between smokers and non-smokers are our next concerns. Acknowledgment This
study
was
supported
by
the
grant
from
the
Ministry
of
Education,
Japan.
References
1) Fujii, M., Kitamura, M. & Kondo, M. (1973) Suigin no bunpu to taikichyu no suigin ni tsuite (Distribution of mercury and mercury in air). Kankyo Hoken Report (Env . Health Report) (Jap.), 26, 5-47. 2) Magos, L. (1971) Selective atomic-absorption determination of inorganic mercury and methylmercury in undigested biological samples. Analyst, 96, 847-853. 3) Nordberg, G.E. & Skerfving, S. (1972) Metabolism. In: Mercury in the Environment, edited by L. Friberg & D. Vestal, The Chemical Rubber Co ., Cleveland, pp. 29-91. 4) Wynder, E,L. & Hoffmann, D. (1967) Tobacco and Tobacco Smoke , Studies in Experimental Carcinogenesis, Academic Press, New York and London .
