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FOOD SAFETY other contaminants, pages 340 344, c k winter

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This article focuses on three types of food contaminants: dioxins including dibenzofurans and polychlorinated biphe-nyls, acrylamide, and perchlorate.. It is likely that concerns regardi

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Osterholm MT and Norgan AP (2004) The role of irradiation in

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Other Contaminants

C K Winter, University of California at Davis, Davis,

CA, USA

ª 2005 Elsevier Ltd All rights reserved.

Food may be contaminated with many chemicals

that pose the potential for toxicological

conse-quences in humans consuming the contaminated

food items In addition to the presence of

contami-nants such as mycotoxins, pesticide residues, and

heavy metals, food may contain numerous organic

contaminants that enter the food supply from

envir-onmental sources or as a result of chemical reactions

that occur during food processing This article

focuses on three types of food contaminants: dioxins

(including dibenzofurans and polychlorinated

biphe-nyls), acrylamide, and perchlorate Each of these

classes has been subject to considerable regulatory

scrutiny, scientific study, and popular media

cover-age It is likely that concerns regarding the presence

of these contaminants in the food supply will

con-tinue throughout the next decade or longer, and that

significant efforts will be made to reduce human

exposure to these substances from food This article

discusses how these types of food contaminants

enter the food supply, the types of food items in

which they are most likely to occur, and the

poten-tial toxicological consequences resulting from

expo-sure to these contaminants

Dioxins

Dioxins are organic chemicals that comprise a family of

ubiquitous environmental contaminants Technically

speaking, the dioxins of potential toxicological concern are polychlorinated dibenzo-p-dioxins (PCDDs) They are related, both structurally and toxicologically, to polychlorinated dibenzofurans (PCDFs) and poly-chlorinated biphenyls (PCBs) Structures of generic PCDDs, PCDFs, and PCBs are shown in Figure 1 Due to their structural and toxicological similarity and to avoid confusion, all three related groups of chemicals are considered to represent ‘‘dioxins’’ for the purposes of this article Specific chemicals belong-ing to this family are referred to as congeners Coll-ectively, there are more than 200 dioxin-related congeners, and each possesses unique toxicological and chemical properties

Occurrence in the Environment and in Food PCDDs and PCDFs are primarily introduced into the environment as by-products of combustion pro-cesses These by-products have been identified in the exhaust gases from sources such as cigarette smoke; industrial and municipal waste incinerators; power plants burning coal, oil, or wood; and automobiles

In addition to these human sources, PCDDs and PCDFs are also produced naturally by combustion

in forest fires and from volcanic eruptions

Historically, PCDDs and PCDFs have also been produced as impurities during organic chemical synth-esis The most notable and most toxic dioxin congener, 2,3,7,8-tetrachlorodibenzo-p-dioxin (TCDD), has been shown to be produced in the synthesis of the herbicide 2,4,5-T, one of the herbicide components

of Agent Orange, notoriously used in the Vietnam War Although 2,4,5-T is now banned for use in the United States because of TCDD and other dioxin impurities, health concerns over the expo-sure of military veterans to Agent Orange and to TCDD continue to be raised PCDDs and PCDFs can also be produced through the use of chlorine

PCDD

O O

PCDF

O

PCB

Figure 1 Chemical structures of generic PCDDs, PCDFs, and PCBs.

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to bleach wood pulp, although most bleaching

processes now use nonchlorine agents such as

hydrogen peroxide

PCBs have been produced synthetically since the

1930s and have been widely used for industrial

applications, such as dielectric fluids in transformers

(due to their inflammability) and capacitors in

elec-trical machinery Like their PCDD and PCDF

coun-terparts, PCBs are extremely persistent in the

environment and are of toxicological concern As a

result, the synthesis and industrial use of PCBs were

significantly curtailed in the 1970s, although

envir-onmental residues of PCBs are still commonly

detected today

Although dioxin release into the environment has

been known to occur for several decades, data are

still limited with respect to the degree to which

dioxins contaminate the food supply Dioxin

analy-sis in the laboratory is extremely expensive because

methods must identify hundreds of different

conge-ners, detection limits are required in the sub-part per

trillion range, and significant precautions must be

taken to minimize exposure of laboratory personnel

to the analytical standards used for dioxin

congeners

Dioxins are highly fat soluble and have been

shown to accumulate in the fat of birds, fish, and

food animals The US Environmental Protection

Agency (EPA) has estimated that more than 95%

of human exposure to dioxins results from dietary

intake of animal fats The major food sources for

dioxin exposure include fish, poultry, meats, milk,

and milk products Dioxins are excreted in human

breast milk and result in exposures to nursing

infants

Historically, it has been shown that human dioxin

exposures, as determined by analyzing human

tis-sues and environmental samples, have decreased

sig-nificantly since 1987 due to engineering controls to

limit dioxin emissions during combustion processes

and to increased regulatory control over other

sources of dioxin exposure Dietary dioxin

expo-sures to UK consumers were reduced by nearly

two-thirds from 1982 to 1992, and subsequent

studies showed even lower exposures in 1997

Nevertheless, dioxins are still ubiquitous in the

environment and human exposure still occurs

Toxicological Considerations

Dioxin exposure at significant dose levels has been

linked to a large number of adverse health effects

Large acute exposures, resulting from chemical

acci-dents and/or occupational exposure to dioxins, have

caused a severe skin condition known as chloracne

A variety of other skin effects, such as rashes and discoloration, have also been attributed to acute dioxin exposures, as has liver damage

Concerns from chronic exposure to dioxins include cancer, reproductive effects, and develop-mental effects The most toxic dioxin congener, TCDD, was classified by the International Agency for Research on Cancer as a human carcinogen From a biochemical standpoint, PCDDs, PCDFs, and PCBs appear to cause their toxic effects through chemical binding to a specific cellular receptor known as the Ah receptor Specific dioxin congeners vary dramatically with respect to their abilities to bind with the Ah receptor; TCDD binds extremely effectively, whereas other congeners are more lim-ited in their binding capabilities The degree to which various dioxin congeners bind with the Ah receptor seems to be directly related to the number and location of chlorine atoms on the congeners Assessing the potential human health risks from exposure to dioxins presents significant challenges Dioxin levels in specific food items can be quite variable, and, as discussed previously, data concern-ing dioxin levels on foods are frequently not available

Another difficulty encountered in assessing dioxin risks is to appropriately account for exposures to the various congeners and to account for the toxico-logical differences among congeners This is most appropriately achieved through a toxic equivalency factor (TEF) approach that assigns a potency factor

to each of the congeners relative to that of the most toxic dioxin TCDD For example, the TEF for TCDD is 1 and the TEF for 1,2,3,4,7,8-hexachlor-odibenzo-p-dioxin (with chlorines added to the

1 and 2 positions and otherwise similar to TCDD) is 0.1 based on findings that 1,2,3,4,7,8-hexachlorodi-benzo-p-dioxin is 10 times less capable of binding to the Ah receptor than is TCDD To calculate a total dioxin exposure, the dietary contributions of each of the dioxin congeners are multiplied by their corre-sponding TEFs and summed to determine a TCDD equivalent exposure

According to the World Health Organization (WHO), a tolerable daily intake (TDI) for TCDD was established at 10 pg TCDD per kilogram body-weight per day in 1990, although revisions by WHO reduced the TDI range to 1–4 pg/kg/day in 1999 A

1997 UK survey of dioxin consumer exposure pro-vided an upper bound of 1.8 pg TCDD equivalent/ kg/day Surveys from other countries, using slightly different TEF approaches, yielded exposures of 0.7 pg/kg/day in Italy, 1.4 pg/kg/day in Norway, 2.4–3.5 pg/kg/day in Spain, and 0.2 pg/kg/day in New Zealand

FOOD SAFETY/Other Contaminants 341

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The US Food and Drug Administration (FDA) has

been monitoring finfish, shellfish, and dairy

pro-ducts for dioxins since 1995 and initiated dioxin

analysis of foods analyzed in its Total Diet Study

in 1999 Specific findings from the FDA’s annual

Total Diet Study can be obtained from the FDA,

although human exposure estimates, in terms of

the amount of TCDD equivalent exposure per

kilo-gram of body weight per day, have not been

pub-lished by the FDA

The EPA recommends that consumers follow the

existing Federal Dietary Guidelines to reduce fat

consumption and, subsequently, dioxin exposure

Such guidelines suggest that consumers choose fish,

lean meat, poultry, and low- or fat-free dairy

pro-ducts while increasing consumption of fruits,

vege-tables, and grains Dioxin exposure can be further

minimized by trimming visible fat from meats,

removing the skin of fish and poultry, reducing the

amount of butter or lard used in cooking, and

repla-cing cooking methods such as frying with methods

such as boiling or oven broiling

Acrylamide

Acrylamide is a widely used and versatile industrial

chemical Its most common use is as a coagulant in

water treatment and purification It is also used as a

soil conditioner, in the sizing of paper and textiles,

in ore processing, and as a construction aid for the

building of tunnels and dam foundations

Acrylamide is considered by the International

Agency for Research on Cancer to be ‘‘probably

carcinogenic to humans’’ based on the results of

several animal carcinogenicity studies As a result,

there has been widespread concern about the

poten-tial risks from exposure to acrylamide among

indus-trial, manufacturing, and laboratory workers

Consumer exposure to acrylamide in treated

drink-ing water has posed a much lower concern since

drinking water is subject to special treatment

tech-niques that control the amount of acrylamide in

drinking water

Swedish researchers developed laboratory

techni-ques that allowed for the detection of biological

reaction products (hemoglobin adducts) of

acryla-mide in human blood samples; results from their

studies allowed correlations to be made between

occupational activities and acrylamide exposures

The findings that acrylamide occurred in tobacco

smoke and that smokers had increased levels of

hemoglobin adducts relative to nonsmokers

pro-vided a suggestion that acrylamide may be formed

during incomplete combustion of organic matter or

during heating Interestingly, the researchers found

significant levels of hemoglobin adducts in blood samples of nonsmoking humans not exposed occupa-tionally to acrylamide This led to speculation that the human diet could contain significant quantities of acrylamide In April 2002, Swedish researchers pub-lished results of research that demonstrated the pre-sence of acrylamide in several common foodstuffs, with the highest levels found in fried and baked foods These findings stimulated worldwide interest

in identifying the potential mechanisms for acryl-amide formation in foods, in assaying a wide variety

of foods for acrylamide levels, and in developing risk assessment and risk mitigation procedures

Occurrence in Food The findings from the initial Swedish study indicated

that the highest levels (150–4000 mg/kg) of

acryla-mide were detected in carbohydrate-rich foods such

as potatoes and in heated commercial potato pro-ducts (potato chips) and crispbread Moderate levels

(5–50 mg/kg) were measured in protein-rich foods

that were heated, whereas unheated or boiled

foods showed no detectable acrylamide (<5 mg/kg).

The governments of several countries throughout the world performed similar analyses of acrylamide

in foods and findings were fairly consistent with those reported in the Swedish study The FDA ana-lyzed dozens of foods for acrylamide levels and con-cluded that the highest levels were observed in

french fries (29 samples; range, 117–1030 mg/kg)

117–2762 mg/kg) Multiple samples from different

lots of the same commercial food products showed significant variability, with the highest levels often several times greater than the lowest levels Com-mercial potato products that could be prepared by baking or by other methods showed much higher levels of acrylamide in the baked products Acryla-mide levels in baby food ranged from below the

detection level (<10 mg/kg) to 130 mg/kg All infant formula samples had levels below 10 mg/kg, and

acrylamide levels in dairy products were also low The widespread findings of acrylamide in food-stuffs throughout the world provided the basis for numerous studies designed to elucidate the mechan-isms for acrylamide formation in foods It has been demonstrated that acrylamide can be formed from classical Maillard reactions as well as from reaction

of the fatty acid oxidation product acrolein with ammonia and subsequent oxidation steps The most plausible explanation for the relatively high acrylamide levels in fried potato products derives from a mechanism involving the reaction of the amino group of the amino acid asparagine with the

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carbonyl group of a reducing sugar such as glucose

during baking and frying This mechanism is shown

in Figure 2 Potatoes are high in asparagine and in

reducing sugars, and they are commonly prepared

for consumption by frying or baking; all of these

factors help explain the relatively high levels of

acrylamide in heated potato products

Toxicological Considerations

Laboratory toxicology studies have indicated that

acrylamide is carcinogenic and also has been

associated with the development of reproductive

toxicity, genotoxicity, and neurotoxicity

Epidemio-logical and analytical studies of people exposed to

acrylamide in the workplace have indicated that

acrylamide does indeed enter the bloodstream of

workers and can be detected and quantified as

hemoglobin adducts, thus indicating both exposure

and absorption of acrylamide Such studies have not,

however, indicated increases in cancer rates among

those exposed occupationally to acrylamide To

date, the only documented toxicological effect

observed in epidemiological studies of workers

exposed to acrylamide is neurotoxicity This effect

is primarily an acute effect caused by large

expo-sures to acrylamide for relatively short periods of

time, leading to nervous system damage, weakness,

and incoordination of limbs

From a biochemical standpoint, it is likely that the

health effects caused by high levels of exposure in

humans and in laboratory animals may result from a

Michael-type nucleophilic addition reaction of

amino acids (both amino and sulfhydryl groups),

peptides, and proteins to acrylamide because of the

presence of the ,-unsaturated conjugated structure

in acrylamide This is a common toxicological

path-way for many reactive compounds It is likely that

high doses of acrylamide may overwhelm the

defen-sive mechanisms of the body such as glutathione

conjugation and may cause reaction with biologi-cally significant nucleophiles, leading to mutations and possible carcinogenicity

Although it is clear that humans have been con-suming significant amounts of acrylamide in their diets for a long time, the relatively new discovery

of acrylamide as a food contaminant has raised several questions Significant efforts are currently being made to better understand the levels of acry-lamide throughout the food chain and to estimate dietary exposure to acrylamide In addition, there is much emphasis on developing food processing approaches that can reduce acrylamide formation Regulatory limits for acrylamide in food have yet

to be established since dietary acrylamide risk assessments are still being developed In the mean-time, the FDA recommends that consumers eat a balanced diet that includes a wide variety of foods low in trans fat and saturated fat and rich in high-fiber grains, fruits, and vegetables

Perchlorate

Perchlorate exists as an anion (ClO4) with a central chlorine atom surrounded by four oxygen atoms arranged in a tetrahedron Perchlorate is manufac-tured in the United States and is used as the primary ingredient of solid rocket propellant Perchlorate wastes from the manufacture and/or improper dis-posal of perchlorate-containing chemicals are fre-quently detected in the soil and water Levels of perchlorate have been detected in 58 California pub-lic water systems and in water samples from 18 states

The widespread water contamination by perchlo-rate and its potential to cause health effects in those consuming contaminated drinking water have led four US agencies—the EPA, Department of Defense, Department of Energy, and National Aeronautics and Space Administration—to request that the

US National Academy of Sciences convene a study

on ‘‘Toxicological Assessment of Perchlorate Ingestion.’’

Occurrence in Food Although the primary concerns from perchlorate contamination result from drinking water con-sumption, recent evidence has indicated that perchlorate may contaminate food items as well

A small survey of 22 lettuce samples purchased in northern California showed perchlorate contami-nation in 4 samples A subsequent study of California lettuce showed detectable perchlorate levels in all 18 samples tested The toxicological

+

NH 2 O

acrylamide

H 2 N

OH

O NH 2

O

asparagine

OH HO

HO

O

glucose heat,

several steps

Figure 2 Proposed mechanism for acrylamide formation in

foods.

FOOD SAFETY/Other Contaminants 343

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significance of such findings has not been

estab-lished, but the studies clearly indicate that

perchlo-rate can enter lettuce, presumably from growing

conditions in which perchlorate has contaminated

water or soil

Milk has also been shown to be subject to

per-chlorate contamination A small survey of seven

milk samples purchased in Lubbock, Texas,

indi-cated that perchlorate was present in all of the

sam-ples at levels ranging from 1.12 to 6.30 mg/l To put

such findings in perspective, the State of California

has adopted an action level of 4 mg/l for perchlorate

in drinking water, whereas the EPA has yet to

estab-lish a specific drinking water limit

Toxicological Considerations

Perchlorate is thought to exert its toxic effects at

high doses by interfering with iodide uptake into

the thyroid gland This inhibition of iodide uptake

can lead to reductions in the secretion of thyroid

hormones that are responsible for the control of

growth, development, and metabolism Disruption

of the pituitary–hypothalamic–thyroid axis by

per-chlorate may lead to serious effects, such as

carci-nogenicity, neurodevelopmental and developmental

changes, reproductive toxicity, and

immunotoxi-city Specific concerns relate to the exposures of

infants, children, and pregnant women because

the thyroid plays a major role in fetal and child

development

The ability of perchlorate to interfere with iodide

uptake is due to its structural similarity with iodide

In recognition of this property, perchlorate has been

used as a drug in the treatment of hyperthyroidism

and for the diagnosis of thyroid or iodine

metabo-lism disorders

Ammonium perchlorate was found to be

nonge-notoxic in a number of tests, which is consistent

with the fact that perchlorate is relatively inert

under physiological conditions and is not

metabo-lized to active metabolites in humans or in test

animals

Workers exposed to airborne levels of perchlorate

absorbed between 0.004 and 167 mg perchlorate per

day These workers showed no evidence of thyroid

abnormality, and a No Observed Adverse Effect

Level was established at 34 mg absorbed

perchlo-rate/day Perchlorate does not accumulate in the

human body, and 85–90% of perchlorate given to

humans is excreted in the urine within 24 h

See also: Cancer: Epidemiology and Associations

Between Diet and Cancer Fish Food Intolerance

Food Safety: Mycotoxins; Pesticides; Bacterial

Contamination; Heavy Metals

Further Reading Becher G (1998) Dietary exposure and human body burden of dioxins and dioxin-like PCBs in Norway Organohalogen Compounds 38: 79–82.

Buckland SJ (1998) Concentrations of PCDDs, PCDFs and PCBs

in New Zealand retain foods and assessment of dietary expo-sure Organohalogen Compounds 38: 71–74.

Environmental Protection Agency (2001) Dioxin: Scientific Highlights from Draft Reassessment Washington, DC: US Environmental Protection Agency, Office of Research and Development.

Food and Drug Administration (2002) Exploratory Data on Acry-lamide in Foods Washington, DC: US Food and Drug Admin-istration, Center for Food Safety and Applied Nutrition Friedman M (2003) Chemistry, biochemistry, and safety of acry-lamide A review Journal of Agricultural and Food Chemistry 51: 4504–4526.

Jimenez B (1996) Estimated intake of PCDDs, PCDFs and co-planar PCBs in individuals from Madrid (Spain) eating an average diet Chemosphere 33: 1465–1474.

Kirk AB, Smith EE, Tian K, Anderson TA, and Dasgupta PK (2003) Perchlorate in milk Environmental Science and Tech-nology 37: 4979–4981.

Sharp R and Walker B (2003) Rocket Science: Perchlorate and the Toxic Legacy of the Cold War Washington, DC: Environmen-tal Working Group.

Tareke E, Rydberg P, Karlsson P, Eriksson S, and Tornqvist M (2002) Analysis of acrylamide, a carcinogen formed in heated foodstuffs Journal of Agricultural and Food Chemistry 50: 4998–5006.

Urbansky ET (2002) Perchlorate as an environmental contaminant Environmental Science and Pollution Research 9: 187–192 Zanotto E (1999) PCDD/Fs in Venetian foods and a quantitative assessment of dietary intake Organohalogen Compounds 44: 13–17.

Heavy Metals

G L Klein, University of Texas Medical Branch at Galveston, Galveston TX, USA

ª 2005 Elsevier Ltd All rights reserved.

Food that we are culturally habituated to consume is usually thought to be safe However, some foods are naturally contaminated with substances, the effects

of which are unknown Crops are sprayed with pesticides while they are being cultivated; some ani-mals are injected with hormones while being raised Meanwhile, other foods are mechanically processed

in ways that could risk contamination This article discusses food contamination with heavy metals, the heavy metals involved, their toxicities, and their sources in the environment A brief consideration

of medical management is also included Five metals are considered in this category: lead, mercury, cad-mium, nickel, and bismuth

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