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Preventive Measures Reduce Exposure to Polycyclic Aromatic Hydrocarbons at a Graphite Electrode Plant Author(s): Marco dell'Omo, Giacomo Muzi, Giancarlo Marchionna, Luca Latini, Patrizia Carrieri, Piero Paolemili and Giuseppe Abbritti Source: Occupational and Environmental Medicine, Vol. 55, No. 6 (Jun., 1998), pp. 401-406 Published by: BMJ Publishing Group Stable URL: http://www.jstor.org/stable/27730946 . Accessed: 03/11/2013 17:00
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Occup Environ Med

1998;55:401-406

401

to polycyclic reduce exposure Preventive measures at a graphite electrode aromatic hydrocarbons plant
Marco delPOmo, Giacomo Muzi, Giancarlo Piero Paolemili, Giuseppe Abbritti Marchionna, Luca Latini, Patrizia Carrieri,

Abstract Objective?This of preventive cacy electrode tional plant exposure effi assessed the study measures in a graphite at reducing aimed occupa to polycyclic workers questionnaire shift urine and sample. aromatic

Polycyclic
ubiquitous combustion, organic

aromatic hydrocarbons
contaminants, derived

(PAHs)
from

are
the

of and pyrolysis, pyrosynthesis matter. Environmental exposure

mainly
urban an an smoke,

derives

from

inhalation

of polluted

hydrocarbons
Methods?Electrode swered end of a

(PAHs).
(n=146) provided Urinary

grilled sure to PAHs aluminium, road paving, roofing, quantities and

and sidestream air, mainstream cigarette and smoked and food intake, especially or fish.1 High meat expo occupational occurs coke wood chimney PAHs released tar and and in industries producing electrodes, with creosote, because in

1-hydroxypyrene
marker of exposure

(l-hpur),
to PAHs,

biological
was meas

graphite

impregnation sweeping, are contained

ured by high performance tography coupled with:

detection. tions tions were measured 1-Hydroxypyrene with compared before measures; group of 54 men

liquid chroma (a) fluorescence

concentra the concentra the of a

of

are heating, such as coal

from, organic tar pitches.13 coal exposure settings?for be Several

large on in, and materials

Epidemiological
dence pitches ple, with that

studies have provided

to coal

evi
tar exam

preventive control

implementing and those (6) not occupation

occupational in some industrial

aluminium increased as

ally exposed
Results?After tive

to PAHs.
implementation median of preven concentrations reduced by the -24%, green in -37% electrode and at in end station some and

production?may cancer risk.

associated individual

PAHs found in coal tar pitches have been

tified suspected carcinogenic of inducing urinary in animals cancer and are in humans.1

iden
thus 24

measures, were significantly l-hpur of workers: groups -30% unit, the in one workers baking

Pyrene
PAH hpur), as a

is a PAH which

is usually present

in

at

impregnation respectively. impregnation in the and were

laboratory, a second baking

unit, In workers unit, power

mixtures; its major biomarker

product l-hpur Urinary Institute of Medicine

finishing concentrations 1-hp than for any

to exposure have shown workers

metabolite, for monitoring occupational 7 studies PAHs.5 many Although in increased concentrations l-hpur and car in wood liquefac

(1 1-hydroxypyrene has been proposed

concentrations

unchanged. were

still

bon

significantly
workers (p<0.001

higher
in

in
the

each
control

group
group Concentra

of

in coke, aluminium, employed in foundries, electrode production, in coal with creosote, impregnation

Occupational and Toxicology, of Perugia, University Italy M delPOmo G Muzi L Latini G Abbritti SPSAL ASL 5, Narni

tion,

in

the

oil

shale
few after was

industry,
studies have undertaking industrial carried where contained

and

road

comparison).

tions job,
workers the the

in the workers varied with the highest values being

engaged in the power two

the type of in found

in in

a only paving,6"15 l-hpur concentrations tive measures The graphite exposed l-hpur was and high in some present electrode to PAHs

evaluated preven setting.1617 out at were tar a

in a specific study plant, mainly for

baking impregnation unit. electrode green reduced

station, units and

workers

in coal

pitches. At
preventive exposure plant. con total PAHs, electrode and peak reflects of

this plant, biological

the first of l-hpur workers.18 were taken was

dosimetry
time were

of

(TR), Italy G Marchionna Industrial Toxicology PMP ASL 5, Unit, Terni, Italy P Paolemili Istituto di Superiore Sanit?, Rome, Italy P Carrieri to: Correspondence Dr Marco delPOmo, Istituto diMedicina del Lavoro, Via E dal Pozzo, 06100 Perugia, Italy. Fax: 0039 75 5783654. Accepted 14 December 1997

Conclusions?Implementing measures significantly to The PAHs at a reduction of to, units graphite in median

performed concentrations groups measures to PAHs. of

in 1994, shown

preventive exposure The efficacy aim of

Therefore, to reduce to assess

centrations exposure was most in had tion, needed and health the been

which l-hpur, and internal in workers

dose

of

this

study

the by

evident where

taken.

preventive an Despite

employed measures overall reduc are to of PAHs

these

current comparing 1994 concentrations, group Materials STUDY GRAPHITE The of subjects and not

preventive values l-hpur and occupationally

measures with

(b) those

(a) the of a control exposed.

further

preventive to minimise

measures

consequently effects.

exposure risk the

adverse

methods OF

PLANT AND MANUFACTURING ELECTRODES

{Occup Environ Med Keywords: 1-hydroxypyrene;

1998;55:401-406) aromatic hydrocarbon;

polycyclic coal tar pitches

Umbria, trodes

graphite Central (length

in is located plant large elec Italy, and produces 0.9 m) about 2.5-3 m, diameter electrode

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402

dell'Orno, Muzi,

Marchionna,

et al

Coke

Grinding -*

Pitch

Mixing i
Extrusion

Green electrodes

_^=4=?==^
impregnation

Baking

Rebaking t= Graphitisation

Baking impregnation Nos 1-2

Laboratory

Quality testing

Graphitisation

Power

station

=r=
Machining t
Graphite electrodes

Finishing

Figure

Flow

process

and production

units (italic,

bold) at the study plant.

for

the

electric

steel

industry.

Raw

materials

are

the

following

measures

to

reduce

exposure

cokes (fillers) and coal tar pitches petroleum (binders), and the main steps in the electrode production are as follows (fig 1). (1) The coke is ground and sized and then mixed with hot pitch at about 190?C to form a semisolid paste, which is cooled, charged in an
extrusion thus press, and crude extruded carbon at about electrodes 110?C, (green providing

were

implemented
MEASURES unit exhaust the

in 1995-6.

PREVENTIVE Green A new

electrode local over

ventilation press; systems and

installed local

extrusion

was system the existing over the scales

exhaust

ventilation

and

the

tank
cleaned,

containing
system outlets.

liquid pitch
refitted; was the refitted

were
control by

electrodes) of the final size. The electrodes are in water. then rapidly cooled by immersion in the green This is performed process
electrodes unit.

checked, room air

conditioning air emission

moving
one of

the fresh air inlet further away from

the

(2) The
(Hoffmann perature trodes basket,

electrodes

are baked
for 20-25 to about in

in ring furnaces Baking impregnation unit No Instead of being removed

baskets a after impregnation,

furnaces) which rises are then

at a tem days The elec 850?C. a large put metallic into

1 from

the metallic
were

preheated

placed in

electrodes

furnaces,

transported
furnace; pitch ing and here from

in the baskets

to the movable

floor

pressure tank, and impregnated with liquid pitch at about 250?C, to fill the open pores. The impregnated electrodes are rebaked in a
movable floor furnace. These processes are

the heating cleaned the encrusted before the new preheat the baskets cycle.

impregnation

carried out in two similar baking impregnation units (No 1 and No 2). (3) The electrodes are coated with graphite by electrical heat treatment at 2800-3000?C. are shaped and end products (4) The finished by machine tools.
During and dling the manufacturing process, of raw materials and heating may vapours. the han particu cause the Workers

Laboratory New local installed the paste. STUDY over

exhaust

ventilation the of the

systems cooling crude

were

the mixer, press

extrusion

and tank, electrode

POPULATION

AND ANALYSIS

OF URINARY

1-HYDROXYPYRENE

tar pitches of the coal larly in dusts and release of PAHs

In December
the green

1996, all the workers

unit, baking

(n=146)
impregnation

at

electrode

are usually highly exposed during steps (1) and (2), but when engaged in steps (3) and (4) are
usually some less at risk. laboratory workers, Moreover, who at the plant, bake, extrude,

units Nos
power station

1 and 2, finishing,
units answered

laboratory, and
a questionnaire

about smoking habits and current jobs. They also provided urine samples at the end of the
working week for l-hpur measurement.

and impregnate smaller electrodes for quality in the control analysis, and all the workers is fuelled by recycled power station, which
pitches, are at risk of exposure to PAHs.

Only data from the 103 workers with the same smoking habit as in 1994, who were still the same job were compared with performing
1994 sons). l-hpur values (within subject compari

All
exposure

the workers
to PAHs

in the plant were

with l-hpur in

tested for
1994,18 and

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Prevention

of exposure

toPAHs

at a graphite

electrode plant

403

Maximum T

value range

were

used. on

Within

subject

comparisons

were

(<1.5 interquartile from end of box) Upper Median Lower quartile Minimum value quartile

performed
Data workers

by theWilcoxon

matched
in different were group test. Differences

pairs test.
groups analysed were of

l-hpur excretion in the control and U

by the Mann-Whitney considered significant

at p<0.05.

Results
range CURRENT 1-HPUR CONCENTRATIONS CONCENTRATIONS In the 103 workers, v 1.80 l-hpur V 1994

-I-

(<1.5 interquartile from end of box) Point outside this range

concentrations =

were

lower in 1996 than in 1994 (median:

creatinine ug/g creatinine, p

1.13 ug/g
0.0001).

s? 25l c

p = 0.038

I IH
p?0.007 p?0.169 p?0.153

11994 1996
p = 0.953

When
according

workers
to at their

were
job,

divided
l-hpur

into groups
concentrations at

h 1 20
p?0.050

were
workers

significantly
the

lower in 1996 than in 1994 in

electrode unit and the

green 1994

15 10

baking
Compared concentration creatinine n=9) at

impregnation
with v the

unit

No

(fig

2).

median values, l-hpur was about -24% (2.44 ug/g = 3.20 creatinine, p 0.038, ug/g electrode and about unit, green

Green electrodes (n= 9) Figure (1994)

&??

Baking Baking impregnation impregnation 1 2 (n= 18) (n= 33}

Finishing

*A

Laboratory

Power station (n= 9> before

v 3.20 -37% (2.03 ug/g ug/g creatinine n= 18) at the baking creatinine, p=0.007, impregnation No 1 unit. The highest individual values were considerably lower in 1996 than in 1994 in each of these units (fig 2).
A evident reduction in l-hpur concentration with was median also and in laboratory workers,

(n = 19)

(n= 15)

2 Urinary in electrode plant workers concentrations 1-hydroxypyrene and after (1996) implementing preventive measures.

Data
in 1996 a control

from all 146 workers who were enrolled

were compared of group with 54 l-hpur values from non-occupationally were randomly in Perugia, was smokers Cen simi

individual values being, respectively, highest 30% and 65% less in 1996 than in 1994 (0.70
ug/g n=15; creatinine and 1.31 v 1.00 ug/g at the creatinine, ug/g v 3.70 creatinine ug/g p=0.05, cre

atinine, respectively,
In workers

fig 2).
baking impregnation were similar unit in

exposed sampled tral Italy.

male

among The percentage

who subjects, the residents of

No

2, in end product
l-hpur

finishing and in the power

station, The

concentrations

in both workers and control subjects (37.7% v 37.0%, respectively). All subjects gave their written informed con sent and the study was approved by the Ethics Committee of the University of Perugia. lar
Details been on reported were centrations sampling l-hpur elsewhere.18 measured and Briefly, by high analysis l-hpur have con

1996 and in 1994 (fig 2).

concentrations of l-hpur from each

group of workers enrolled for within subject did not significantly differ from comparisons
the concentrations measured in other not workers

performing
within

the same job but not considered

comparisons (data

for

subject

shown;

perform

ance
underwent

liquid

chromatography
detection, enzymatic

coupled

with
CURRENT PLANT Urinary l-HPlR EXCRETION V CONTROL GROUP 1-hp group concentrations AT THE ELECTRODE were

Mann-Whitney

U test).

fluorescence

after urine samples a solid and hydrolysis et al to Jongeneelen clean up according phase were cor Measurements of (1987).5 l-hpur rected for urinary creatinine. STATISTICAL ANALYSIS

significantly

higher
control

in each group
(p<0.001

of workers
for any

than in the
comparison).

Statistical
PC ues Table software. were 1

analysis was performed

As skewed, the distributions only

by SPSS
of l-hpur

for
val tests

Concentrations in the 146 workers varied with the type of job (table). The highest individual l-hpur concentrations were between five and nine times higher in
workers and at the green electrode unit, at the two

non-parametric in graphite

Urinary

1-hydroxypyrene

electrode workers

in the control group

1-Hydroxypyrene (pglg creatinine) Median Electrode workers Unit: Green carbon Baking impregnation Baking impregnation Finishing Laboratory Power station Control group *p<0.001 v Control 1 2 146 13 25 55 25 18 10 54 1.44 2.44* 2.25* 1.91* 0.66* 0.66* 3.35* 0.13 Mean 2.24 3.16 2.38 1.91 0.69 0.60 5.83 0.19 25% 0.76 1.30 1.07 1.06 0.35 0.28 2.19 0.05 75?/ 2.70 4.20 2.82 3.14 0.96 0.85 11.68 0.24 Min 0.08 0.69 0.38 0.36 0.13 0.08 1.31 0.01 Max 13.8 8.665 7.78 12.20 1.78 1.31 13.80 1.56

group.

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404

delVOmo, Muzi,

Marchionna,

et al

15

of box and whisker Definitions plots as for figure 2 I I Non-smokers Smokers p< 0.001 p< 0.040

SS12

p< 0.018 o o o

smoking habits in 1996 as in 1994, thus avoid of exposure to ing the risk of misclassification PAHs. We performed within subject compari
sons evant of l-hpur variation the thus data, between controlling people The effects in for the rel of activity of age

Si 9h
S ? 6L

Io

pyrene
influence

biotrasforming
results.19

enzymes which might 20

?l 3 0

and

Control group (n = 54)

Low occupational High occupational exposure to PAH exposure to PAH (n = 103) (n = 43) on urinary 1-hydroxypyrene

et

in exposure to PAHs from diet at differences times could have only the two sampling
influenced quently l-hpur exposure to due we l-hpur presume results Conse marginally.20 the reduction that reflects of PAHs, was cur of at at the the the in

Figure 3 Effect concentrations.

of smoking

which concentrations, internal dose to, and the preventive measures.

total

baking
power

impregnation
station than

units,
in

and in those in the

the control group.

the highest median Surprisingly, and individual (13.80 creatinine)

ug/g creatinine) l-hpur concentrations

(3.35 ug/g and 13.70

were

an overall reduction, However, despite at some rent to PAHs units exposure electrode electrode, (at the green plant two and units, baking impregnation

found
station. The

in workers
highest l-hpur

in charge
concentrations

of

the power
in workers

is still high, compared with power station) in other units workers (electrode engaged finishing and laboratory analysis) and with the
control exhaust other Even group. ventilation sources of pitch though systems dusts and several were local installed, still vapours

and in in end product finishing engaged laboratory analysis overlapped with the upper limit in the control group (table). Urinary 1-hp in did not differ significantly concentrations
workers employed in the workers at the two baking impregna

exist in the electrode plant, and need to be controlled. Control of workwear policy might
also studies contributes excretion.1317 be advisable, have shown to 21 An field and experimental that skin exposure greatly and PAH intake l-hpur intervention showed study that on coal a improve in result as

tion units
emerged laboratory

(table). No

significant

differences
in the 18 in the

l-hpur concentrations when concentrations

eight workers engaged in producing small trodes for quality testing were compared different the 10 workers performing v 0,52 0.72 creatinine (median: ug/g creatinine; p= 0,59).
To two assess the a first effect of smoking on

elec with tasks ug/g

l-hpur

workers liquefaction ments in workwear significant reduction

may policy in l-hpur excretion.16

We
workers extrusion, electrodes

found
engaged

high

l-hpur concentrations

in
in the

excretion,
groups,

the 146 workers

group with

were
low

divided
occupational

into

baking, and in the power

raw materials, in processing of and impregnation station (high

expo

exposure to PAHs (workers engaged in end product finishing and at the laboratory unit) and a second group with high exposure (work
ers at the green electrode units, and 1-hp and workers at the two baking power sig impregnation station). Urinary in the were

and

concur with sure group). These findings electrode plants in Belgium reports on graphite 22
Germany.9 concentrations to PAHs 2.14 However, exposure levels

seem to be
l-hpur exposure ric mean:

lower in the Italian plant.

In fact

concentrations

workers with among high at the Italian (geomet plant 2.24 median: creatinine; ug/g

than in non in smokers higher nificantly smokers in the control group and in each of the two occupationally exposed groups (fig 3). The
difference tration 0.13 ug/g tional in between smokers creatinine the median and in the in workers and 0.59 l-hpur in non-smokers control with ug/g concen was

ug/g
workers

creatinine;
engaged mean: and

n=103)
in the 5.75

were
extrusion and 5.47

lower than
of electrodes

in

nine;

(geometric n=5

9;

workers,

respectively) n=3 and

creati ug/g and smoking non-smoking or in electrode impreg

ug/g creatinine

0.34 group, low occupa creatinine in

nation
creatinine;

(geometric mean:

7.99

and 9.58 ug/ g

exposure,

workers with high exposure.

Discussion

They

ing workers, were

and smok 5; non-smoking at the Belgian respectively) plant.9 even than in workers lower engaged

in processing
creatinine;

raw materials
or in

(median: 9.6 ug/g

baking (me

n=2),

electrode

This
measures

study shows that implementing

significantly reduced

preventive
exposure to

dian: 23. 4 ug/g creatinine; n=30) and impreg nation (median: 22.0 ug/g creatinine; n=9) at
the German We two and found concentrations occupationally this that plant.22 that smoking in the control increased group and l-hpur in the

PAHs
and most

at a graphite electrode plant. Specifi cally, we found an overall reduction inmedian

peak evident concentrations, l-hpur in workers employed which in the was green

electrode unit, in the baking impregnation unit No 1, and in the laboratory (fig 2). In all these
units preventive measures local had been taken?for ventilation example, installing exhaust

groups exposed rose with increase on

of workers, increased

exposure
effect of

to PAHs
smoking effect

(fig 3). The more marked

l-hpur excretion in the

workers with higher

synergistic

exposure might
smoking

indicate a
and occu

systems, cleaning the metallic baskets of pitch residues. There had been no further modifica flow process, or in tions in the productive
workwear policy. Moreover, we considered only

between

pational already
studies,81215 ble. First

exposure been
and of all,

to PAHs. A similar effect has in other hypothesised

three smoking explanations seems are possi to modulate

workers

with

the same

job and with

similar

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Prevention

of exposure

to PAHs

at a graphite

electrode plant

405

PAH metabolism,
biotransformation in vitro the studies

by enhancing
of pyrene shown have into that

the enzymatic
1-hp. the activity Recent of

will the

none

the

less

reduce of action l-hpur in the

this

endorsement workers' encountered the electrode some l-hpur

reducing ranges In

risk, we support at levels aiming to excretion the population. in this excreted non pre expo health the

enzyme pulmonary 10 times is, on average, in current non-smokers.19 to reduce might who masks Even smoke more though

pyrene higher

1-hydroxylase in smokers than smoking and from is

general

Secondly,

report higher

known

mucociliary impair might

consequently workers protection smokers. increases centrations less than

clearance, the removal remove often than

groups concentrations

plant investigated still of workers

than

the lung of PAHs bound

to particles. Thirdly,
their non

occupationally measures ventive sure effects. removal to PAHs These of other

Further subjects. exposed are needed to minimise and the sources risk of adverse include measures

should of PAH policy, health

smoking in this

concentrations, l-hpur in the workers occupational confirms study used

significantly con it affects plant much

workwear appropriate mation programme

an volatiles, an and infor associated

on

risks

This

marker biological be successfully preventive

exposure (fig 3). that is a useful l-hpur to PAHs of exposure and can to in assess work levels Jongeneelen workers?that excreted at 0.2 mg for when benzene the efficacy environments for in of

with
We

exposure

to PAHs

and smoking habits.

thank Dr GA Boyd for her invaluable help.

measures or

polluted
exposure remain

by PAHs. Unfortunately
limits to be action established. oven

the biological
l-hpur 1992

proposed
creatinine l-hpur workers

a tentative biological
for are coke concentration exposed

limit of 4.4 ug/g

is, the these soluble

matter/m3
time matter

(the ACGIH
average tar pitch

threshold
benzene volatiles).23

limit value
soluble Similarly,

weighted of coal of 6.2

Van Rooij
limit

et al in 1993 estimated
ug

a biological

oven creatinine for coke l-hpur/g workers?that the concentration is, l-hpur are exposed at 2 excreted when these workers technical ug benzo(a)pyrene/m3 (the German two limits have These guiding concentration).21 on the grounds been that biological criticised,22 not indices for be should exposure l-hpur a correlation from derived between the internal dose the and dermal value of the airborne absorption Buchet 2.7 ug which be exposure of PAHs et al l-hpur/g l-hpur kept", for increased in to PAHs, in many 1995 creatinine given work

environments. the limit "should to be the

proposed as the it seems

below

concentrations because

preferably threshold workers as

cytogenetic

effects
non-smoking

in peripheral population.24
attractive

blood
compared

lymphocytes
with a refer

of is

ence
rather

This
it derives

biological
from

limit

correlations

between
effect of

the internal dose and the lack of health

the relevance level). However, to the actual end points health lung More neoplasm?need recently, Zober to be and smok

(no effect the measured example, evaluated.

risks?for better

Will

assumed

the upper

reference

limit of
of

l-hpur concentrations ers who were not PAHs level

in a population occupationally

(2.5 ug l-hpu/g creatinine) for a biological monitoring programme.25 et al suggested the 90th percen Angerer using as an tile of the results of biological monitoring action dermal possible.22 level exposure for corrective had been reduced

to exposed as the action

once measures, as much as

According
90/394/EEC,26 not identify which the cancer light of and the a

to
current dose

the
for not

Council
scientific a

Directive
evidence can below in of PAHs

risk will assumption

carcinogen exist. Therefore, that a reduction

exposure

absorption

of carcinogenic

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