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Adulteration of Oregano Herb and Essential OilBy Ezra Bejar,
PhD American
Botanical Council, PO Box 144345, Austin, TX
78714 Correspondence: email
Citation (JAMA
style): Bejar E. Adulteration of oregano herb, and essential oil of oregano. Botanical Adulterants Prevention Bulletin. Austin,
TX: ABC-AHP-NCNPR Botanical Adulterants Prevention Program; 2019.
Keywords: Adulteration, essential oil, Lippia graveolens, Mediterranean
oregano, Mexican oregano, oregano, oregano leaf oil, Origanum onites, Origanum
vulgare subsp. hirtum
Goal: The goal of
this bulletin is to provide timely information and/or updates on issues of intentional and accidental adulteration and mislabeling of oregano
herb and essential oil (EO).* It provides information on issues of
adulteration and mislabeling of oregano (Origanum
vulgare subsp. hirtum, O. onites)
herb used as a spice and herbal remedy, in particular with winter savory (Satureja montana, Lamiaceae) herb, sweet
marjoram (Origanum majorana,
Lamiaceae) herb, Cistus spp.
(Cistaceae) leaf, olive (Olea europaea,
Oleaceae) leaf, thyme (Thymus spp.,
Lamiaceae) herb, summer savory (Satureja
hortensis, Lamiaceae) herb,
strawberry (Fragaria spp., Rosaceae)
leaf, sumac (Rhus spp.,
Anacardiaceae) leaf, hazelnut (Corylus
avellana, Betulaceae) leaf, myrtle (Myrtus
communis, Myrtaceae) leaf, and colored wheat (Triticum aestivum, Poaceae) bran. Additional species in the family
Lamiaceae from the genera Origanum, Thymus, Poliomintha, Plectranthus,
Monarda, and Hyptis or in the family Verbenaceae from the genera Lippia, Aloysia, and Lantana are
known to have “oregano” as part of their common name, and may thus be mistaken
for oregano by purchasing personnel who lack proper training.
The bulletin
also addresses adulteration of oregano (Origanum
vulgare subsp. hirtum) EO, in particular with Origanum and Thymus
species, Spanish thyme blend, and synthetic
carvacrol and thymol. This bulletin may serve as guidance for quality control
personnel, the international herbal products industry and the extended natural
products community in general. It is also intended to present a summary of the
scientific data and methods on the occurrence of species substitution, adulteration,
the market situation, and economic and safety consequences for the consumer and
the industry.
1 General Information
1.1 Common name: Oregano1,2†
1.2 Other common names2-5
Greek oregano:
English: Wild marjoram Danish: Almindelig merian, merianurt Dutch: Oregano,
wilde marjolein French: Origan, origan commun German: Dostenkraut, gemeiner Dost, Oregano, wilder Majoran Greek: Ρίγανη (rigani) Italian: Maggiorana
selvática, origano, origano comune, Norwegian: Bergmynte, oregano Portuguese: Orégano, orégão Spanish: Orégano Swedish: Kungsmynta, oregano Turkish: Kekik, Keklik otu
Turkish oregano:
English: Cretan oregano, Oikea oregano, pot marjoram Danish: Fransk merian, Tyrkisk merian,
pottemerian Dutch: Potmarjolein, Kretenzische oregano, Turkse oregano French: Origan de Chypre, origan crêtois, origan turc German: Französischer Majoran, Kretischer Dost, Kretischer Oregano,
Türkischer Oregano Greek: Τούρκικη ρίγανη (Tourkiki rigani) Italian: Origano siciliano, origano cretico Norwegian: Fransk merian Portuguese: Orégano turco Spanish: Orégano cretense, orégano italiano, orégano,
orégano turco Swedish: Smyrnamejram,
spansk timjan, spansk dosta, fransk mejram, krukmejram Turkish: Bilyali
kekik, Izmir kekiği
1.3 Accepted Latin binomials:
Origanum vulgare L.
subsp. hirtum (Link) letswaart1,6 and Origanum onites L.7
1.4 Synonyms:
Origanum vulgare L.
subsp. hirtum: Origanum
heracleoticum auct. non L.,1 Origanum hirtum Link,8 Origanum megastachyum Link,9 Origanum neglectum Vogel,9 Origanum smyrnaeum Sm.,9 Origanum vulgare subsp. hirtum
(Link) A. Terracc.10
Origanum onites: Majorana cretica Mill., Majorana
onites (L.) Benth., Origanum orega
Vogel, Origanum pallidum Desf., Origanum smyrnaeum L.9
1.5 Botanical family: Lamiaceae
1.6 Vernacular name use:
There is
much confusion regarding the vernacular name oregano. It is a name given to dozens
of plant species from the families Asteraceae, Fabaceae, Lamiaceae, and
Verbenaceae.11-14
The main genera are Origanum, Lippia, Thymus,
Plectranthus, Lantana, Aloysia, Monarda, and Hyptis. Their commonality is that their leaves or flowering tops
have the flavor recognized as being oregano provided by the mix of carvacrol
and thymol and other volatile compounds.12,14,15
Two main genera are available commercially in North America: Origanum and Lippia. Lippia graveolens (Mexican
oregano) is most frequently used in the United States, Mexico, and Japan.11 Mexican oregano may also
include species from the genera Lantana
or Hyptis. Spanish oregano is not
derived from an Origanum or Lippia species, but from Thymbra capitata (syn. Thymus capitatus).12,13,15
Plectranthus amboinicus (syn. Coleus amboinicus, Lamiaceae) is known
as Cuban oregano or Indian mint.14,16
Limitations with regard to the species permissible for use as a dietary
supplement/herbal medicine or spice ingredient are indicated below.
1.7 Interchangeable use of species:
Dietary supplement and herbal medicine: According
to the American Herbal Products
Associations Herbs of Commerce, 2nd edition,1 products made of Origani herba consist of flowers and
leaves of O. vulgare subsp. hirtum, while the European
Pharmacopoeia (Ph. Eur.) allows two species, O. vulgare subsp. hirtum and
O. onites, to be sold as oregano.17 Dietary
supplement ingredients derived from Lippia
graveolens have to be listed as “Mexican oregano” in the United States.1
Spice: The European Spice Association
(ESA) and the American Spice Trade Association list two species that can be
sold as oregano, O. vulgare subsp. hirtum and O. onites, while the International Organization for Standardization
(ISO) has a broader definition for oregano which includes all species of the
genus Origanum with the exception of O. majorana.18 Spices
derived from Lippia species
(Verbenaceae), particularly L. graveolens,
have to be labeled “Mexican oregano.” The draft standard developed by the Joint
FAO/WHO Food Standards Codex Committee on Spices and Culinary Herbs (CCSCH)
includes a number of species that can be marketed as dried oregano, including O. vulgare subsp. hirtum, O. onites, O syriacum, O. vulgare x majoricum, O. vulgare subsp. virens, O. vulgare subsp.
viride, O. vulgare subsp. vulgare, Satureja montana, Lippia graveolens, L. berlandieri, L. palmeri,
and Poliomintha longiflora (Lamiaceae).
Origanum vulgare subsp. hirtum is offered under the trade name
“Greek oregano,” while O. onites is
traded as “Turkish oregano,” “Cretan oregano,” or “Oikea oregano.” Species of
the Lippia and Poliomintha genus are traded as “Mexican oregano.”19 Additional
regional differences in what plant species is used as oregano have been
reported.20
Essential oil (EO): Oregano oil is
generally known as the essential oil obtained by steam distillation of the
flowers and leaves of Origanum vulgare L. subsp. hirtum. The International Nomenclature of Cosmetic Ingredients (INCI) name for oregano oil is “Origanum vulgare leaf oil,” “Origanum
vulgare flower/leaf/stem extract,” or “Origanum vulgare leaf extract.” It is
not known to what extent oils from other Origanum species can be/are
sold as oregano oil, although the essential oils obtained from O. compactum,
O. onites, and Thymbra capitata are commonly labeled as oregano
oils.21,22 According to the International
Trade Centre, oregano oil originating in Turkey may be derived from a
range of species such as Origanum, Satureja, Thymbra, and Thymus.23
1.8 Distribution:
Origanum vulgare is originally from the
Mediterranean region, but is more widely distributed across Europe (including
the British Isles), as well as south and central Asia, and, in North America in
the lower 48 states and Canada.24,25
Origanum vulgare is represented by
six different subspecies (with a circumscribed regional distribution): O. vulgare subsp. glandulosum (Algeria, Tunisia);
O. vulgare subsp. gracile (Central Asia, Iran, India, Turkey,
Afghanistan, Pakistan); O. vulgare
subsp. hirtum (Balkans, Greece,
Cyprus, Turkey); O. vulgare subsp.
virens (Morocco, Canary
Islands, Azores, Balearic Islands, Spain, Portugal, Madeira); O. vulgare subsp. viridulum (widerspread across
southern Europe to Iraq, Iran, Afghanistan, Pakistan); and O. vulgare subsp.
vulgare (widespread across
Europe and Asia, naturalized in North America and Venezuela).8,24,26,27 Origanum
onites has a limited geographic range, occurring mainly in Southern Greece,
the Greek islands of the Aegean sea, in some areas of western and southern
Turkey and the island of Sicily.8,24,26-28
1.9 Plant part and form:
Origanum vulgare is a perennial herb, with
green fresh leaves, 3-28 mm long and 2.5-19 mm wide, petiolated or sessile. Laminae
tend to be ovate or ovate-elliptic, with serrated or not serrated margins;
acute or obtuse apex. Flowers are rare, found as broken parts of the corymbs.
Bracts are greenish-yellow and imbricate. The calyx is corolla-like and
inconspicuous. The corolla is white, on top of inflorescences, slightly
conspicuous or inconspicuous.17 Dried leaves and flowers
separated from the stems (stems contain lower amounts of essential oil) of oregano
are used to produce oregano herb and oil.
The EO obtained by steam
distillation from O. vulgare subsp. hirtum has been most frequently used due
to its high EO content and a well-studied composition.27,29-31
O. vulgare subsp. hirtum has two main chemotypes, thymol-type
and carvacrol-type, with intermediate chemotypes containing various amounts of carvacrol
and thymol and a high content of the two precursors, p-cymene and γ-terpinene.27,32
According to ISO, oregano oil is defined
as a yellow to dark brownish-red
colored oil with a characteristic organoleptic profile (having aromatic,
phenolic, and slightly spicy base qualities). The essential oil composition is
60-80% carvacrol, 4-10% p-cymene,
3-9% γ-terpinene, and small amounts of thymol (0.5-5%).6
1.10 General use(s):
Medicinal uses for oregano
date back to the ancient Greek and Roman empires, where
leaves were used to treat different conditions, such as skin sores, aching
muscles, and as an antiseptic.33
Origanum vulgare is employed as a
stimulant, carminative, diaphoretic, and nerve tonic. It is also used in the
treatment of respiratory ailments (asthma, coughs), headaches, toothaches,
rheumatism, as an antibiotic, expectorant in bronchitis, antispasmodic,
appetite stimulant, diuretic, diaphoretic, and as a mild sedative.2,12,33-35
Reported effects include: vasodilation, reduction of blood clotting, as well as
sugar-lowering properties.36 Oregano oil, when applied
topically, works as an emollient, antipruritic (in spider and insect bites),
and is used to treat frostbite and as a protectant against infections in cracks,
bruises, and insect bites.33,35
Oregano herb and oil have been used in European phytomedicine and in the United
States as an analgesic in lozenges, and as an antiseptic in oral health. Carvacrol,
the main active compound in oregano oil, is believed to be responsible for most
of oregano oil’s purported health benefits. A number of in vitro and
in vivo studies support antibiotic, antifungal, anti-inflammatory, and
immune-stimulant properties, as well as carvacrol’s effects on digestive and
cardiovascular health.15
Carvacrol is also used in the United States as a food additive, with
demonstrated antiseptic and antioxidant properties in food preservation.15
2. Market
2.1. Importance in the trade:
2.1.1 Oregano oil
The use of oregano
oil as an ingredient in commercial products is quite extensive. According to KHC
Başer, PhD, Turkey dominates the global supply of oregano oil, providing around
70% of global needs. Annual Turkish oregano oil production in 2014 was estimated
to be in the range of 15 to 20 metric tons. The oil is derived from a number of
species from the genera Origanum, Thymus, Thymbra, and Satureja.15,23
Most oil production is from wild harvested material. Main production sites are
in the Aegean and Mediterranean regions, with more limited production in the Marmara
region. The optimum harvest time for oil production is just as the flower buds
form. In 2018, Turkey exported approximately 66
metric tons of oregano oil for a return of US $5.3 million. (KHC Baser email to
S. Gafner, May 22, 2019)
2.1.2 Oregano herb
Historically,
Mediterranean oregano herb was produced in Turkey, Greece, Albania, Spain,
Italy, Israel, Morocco, and Egypt.11,37,38
Currently, Chile and Peru are also among the main producing countries.39
A report
from 2002 estimated that over 10,000 tons of dried oregano were harvested from
wild sources in Turkey annually; about a tenth of that production was believed
to be used domestically as condiment or herbal tea, and the remaining 9,000
tons used for EO production or exported as herb. Origanum onites is cultivated in the Aegean part of Turkey in
fields totaling over 6,300 ha in the provinces of Denizli (4000 ha), Izmir
(2000 ha), and Isparta (300 ha). Organic farming of O. onites is also practiced in Western provinces of Turkey.37
In 2011, approximately 12,000 metric tons of oregano (O. vulgare, O. onites, L. graveolens)
were traded globally with Turkey (8,182 tons), Peru (3,324 tons), and Mexico
(215 tons) as the main producers, although numbers from the Food and
Agriculture Organization of the United Nations (FAO) suggest that production in
Mexico is much higher (see below).40,41
More recent figures from a
2016 estimate that the world trade volume of oregano is about 12,000-13,000
tons/year, although data from the Turkish Statistical Institute (TURKSTAT)
indicate a production of 14,724 tons oregano in 2016 in Turkey alone.42 Turkey exported approximately 9-12 thousand tons of
oregano in the years 2011-2016, with approximately 80% cultivated oregano and
the rest wildcrafted.29
Turkey is the major supplier of Mediterranean oregano
herb consisting of over 90% of oregano exports.37
Origanum onites (Turkish oregano)
tops the list of commercial Origanum
species of Turkey. It is obtained both from wild and cultivated plants. The
other Origanum species collected from
the wild for commercial use are the following: O. majorana (sweet marjoram), O.
vulgare subsp. hirtum (Greek
oregano), O. minutiflorum (Spartan
oregano), O. syriacum var. bevanii (Israeli oregano), and O. acutidens, another Turkish endemic
species.37 Herb production reached 17,666 tons in 2018 with a value of US $57 million; unit
export value was US $3.2/kg. (KHC Baser email to S. Gafner, May 22, 2019)
SADER, the
Mexican government’s Secretariat of Agriculture and Rural Development, reports
that Mexico was the second largest producer of oregano (although not
Mediterranean oregano) in 2013 and that oregano production was the highest in
the central and northern Mexican states of from San Luis Potosi north to Baja
California,43 with Chihuahua producing
1,000 tons in the year 2015.44 The FAO stated that Mexico
produced between 5,000-10,000 tons of Mexican oregano per year in between
2014-2018.41 The Mexican oregano (L. graveolens) is used domestically and
also exported to the international market, representing approximately 35–40% of
oregano in the world. Consumption of Mexican oregano is restricted mainly to
two countries outside of Mexico – the United States and Japan – which account
for 90% of the total exports.44,45
2.1.3 Oregano dietary supplements
Oregano dietary supplements have
seen a consistent growth in sales from 2015-2018 in the United States, with
most of the sales in the natural channel (co-ops, associations, independent
retailers and large regional chains), where it has been among the top 12
best-selling herbs.
Table 1: Sales data
for oregano dietary supplements in the herbal category in the United States from
2015-2018.
Channel
|
2015
|
2016
|
2017
|
2018
|
|
Rank
|
Sales [US$]
|
Rank
|
Sales [US$]
|
Rank
|
Sales [US$]
|
Rank
|
Sales [US$]
|
Naturala
|
10
|
7,755,387
|
12
|
7,510,751
|
10
|
8,693,675
|
10
|
9,925,727
|
Mainstream Multi-Outletb
|
59
|
589,106
|
66
|
754,693
|
61
|
921,834
|
n/a
|
n/a
|
a According to SPINS (SPINS does not
track sales from Whole Foods Market.) b Data from 2015–2017 according to
SPINS/IRI. This channel includes the food, drug, and
mass-market sector, military commissaries, and select buyer’s clubs and
so-called dollar stores. SPINS/IRI data does not include discount department
store sales, e.g., possible sales at Walmart and club stores are excluded,
products sold through the internet or health care practitioners, and sales through independent
stores who do not use check out scanners. n/a: not available Sources: Smith et al.,46-49 T. Smith (American Botanical
Council) e-mail to S. Gafner, February 6, 2018, and K. Kawa (SPINS) e-mail to
S. Gafner, July 11, 2016.
2.2 Market dynamics:
In 2011, high quality dried oregano (min. 2.5% EO content)
of Turkish origin was sold at wholesale prices of US $2.58/kg while material of
lower quality was available at US $1.58/kg. In the same year, oregano (Origanum vulgare) from Peru was priced
at US $3.20/kg and Mexican oregano (Lippia
spp.) originating in Mexico at US $5.51/kg.40 Prices
of dried Turkish oregano in 2016 were US $4.30/kg in the US and US $4.56 in
Europe,50 while Mexican oregano was sold by wildcrafters at a
fraction of a dollar (8-10 pesos/kg) and at US $5.00/kg (100 pesos) by
suppliers.51
An informal investigation of the
retail prices for “oregano” essential oil from Chinese distributors (depending
on amount purchased and if whole herb or leaf) on Alibaba.com showed products
sold for as low as US $1/kg, although starting prices were more often in the US
$10-25/kg range, which is well below the normal price range for authentic
oregano oil. Based on information from the International Trade Centre, the
price of pure oregano oil from Mediterranean source was in the range of 70-120
€/kg in 2014,23,50 with corresponding prices in US $ fluctuating between 80-150/kg.
3. Adulteration
3.1 Known adulterants:
3.1.1 Known adulterants of oregano herb
A survey of the European
market from 2001 to 2007 revealed products frequently labeled and sold as “true”
Mediterranean oregano contained: (1) plants lacking a clearly detectable EO profile,
added as bulk extraneous material including berries (Rubus spp., Rosaceae), hoary rockrose (Cistus ×
incanus, Rosaceae), Sicilian sumac (Rhus
coriaria, Anacardiaceae) and, (2) essential oil-bearing plants with oregano-like
flavor, mostly belonging to the Lamiaceae family (S. montana and O. majorana).52,53
Other reports indicate adulteration of oregano leaves may occur with anise (Pimpinella anisum, Apiaceae) seeds,
myrtle (Myrtus spp., Myrtaceae) leaves,
European hazelnut (Corylus avellana,
Betulaceae) leaves, olive (Olea europaea,
Oleaceae) leaves, and artificially colored wheat (Triticum aestivum, Poaceae) bran.18,37,52,54-56
Given that the definition of the oregano plant encompasses several
species of plants with similar properties, commercial decisions to purchase one
or other oregano species has been largely based on availability of raw material,
cost, and regional acceptability. There is a clear morphological and
organoleptic distinction which can be made between Mediterranean and Mexican oregano
for identity purposes using microscopic, macroscopic, and organoleptic methods.
However, North American and European market trends are predominantly driven by
regional preferences and market acceptability, represented in the U.S. by the American
Spice Trade Association (ASTA) and in Europe by the European Spice Association
(ESA) with their own definitions and cleanliness specifications (see section
1.6).18
3.1.2 Known Adulterants of Oregano Essential
Oil
Adulteration,
such as the use of lower-cost synthetic or natural material added to natural EOs,
is a significant problem in the EO industry.57 Adulteration of oregano oil occurs
with synthetic thymol, carvacrol (or thymol-carvacrol mixtures), or limonene added
from different sources.58,59
Carvacrol can be produced in a synthetic manner using a number of starting
materials, e.g., by alkylation of o-cresol.60,61
“Thyme oil white“ from Spain is a frequent adulterant used to dilute pure EOs. This
is a blend made out of several natural fractions of Spanish thyme (Thymus zygis) oil, plus other oregano
species (besides O. vulgare) with
added natural p-cymene. (E. Schmidt
email, November 29, 2017) Spanish thyme oil contains around 40-50% thymol and
4% carvacrol.58 Adulteration with EO from Thymus spp., or synthetic thymol has
also been found during routine quality control assessments in industry
laboratories (C. Beaumont, [dōTerra] oral communication to S. Gafner, February
7, 2019). Synthetic thymol can be obtained in a similar manner as synthetic
carvacrol, e.g. using m-cresol as a
starting material which is subjected to alkylation with propylene.62
3.2 Sources of information supporting confirmation of adulteration:
3.2.1. Oregano
spice
In its guidance document, ASTA reports that oregano
adulteration is a common practice. The organization reported the sale of
oregano with extraneous matter from different parts of other plants of similar
appearance and determined that this is typically added at the cutting/grinding/blending
stage.63 Oregano is frequently
adulterated with Cistus spp., sumac,
and myrtle. The Cistus genus has 20
species – perennial shrubs found on dry or rocky soils throughout the
Mediterranean region, from Morocco and Portugal to the Middle East. Cistus leaves have a dark green color
that, when added to oregano, makes the adulterated spice visually more appealing
than pure oregano.63 Other herbs which have been
found in oregano include winter savory and sweet marjoram. Seven commercial
Mediterranean oregano samples also exhibited different contamination levels of O. majorana (ranging between 0% and 95%)
and S. montana (ranging between 0%
and 9.7%). These samples were obtained from wholesale traders during a survey
carried out between 2001 and 2009.52
In
a more recent report from the United Kingdom, 53 commercially available oregano
samples were purchased at various retailers, including convenience shops,
supermarkets, and market places in the UK and Ireland.18 In addition, 25 samples were
also purchased from online retailers from EU and non-EU countries. Samples were
tested for identity using spectrometric methods (FTIR and LC-HRMS). Approximately
24% of the total 78 oregano samples tested were adulterated and the amount of
adulterant ranged from 30% to over 70%; two samples had no oregano present. Similar
figures were found for oregano purchased from retail stores and on the Internet.
The most common adulterants found in the samples were olive leaves and myrtle
leaves. No difference was found between samples purchased in supermarkets and
those online.18
CHOICE,
a consumer advocacy group in Australia, had 12 commercial oregano products
tested, representing more than 80% of the value of Australia’s oregano sales in
the herb and spice product category. Samples were analyzed for authenticity by
Fourier transform infrared (FTIR) spectroscopy and subsequent statistical
testing. The results gave evidence that seven of these products contained less
than 50% oregano and were adulterated with olive leaves or sumac leaves.64-66 The consumer advocate group
referred the issue to the Australian Competition and Consumer Commission.67,68 Based on the complaint, ACCC
initiated its own investigation into a number of oregano brands, and found that
one brand manufactured in Australia and three other products sold as oregano
leaves were mislabeled since they contained substantial amounts of undeclared olive
leaves.67,68
Finally, in a presentation on the quality control of spices,
Larry Lichter, Vice-President of Global Quality and Food Safety at McCormick
& Co., Inc., reported that oregano adulteration is common in non-qualified
supply chains (i.e., the “spot market”, also known as “cash market”, where
commodities are immediately delivered after the sale), with sumac, olive,
strawberry, myrtle, hazelnut, and cistus leaves being the principal
adulterants.69
3.2.2 Oregano
oil
In 2014, an alert on the EU RASFF (Rapid
Alert System for Food and Feed) portal was placed on a
nutritional supplement distributed in the Czech Republic, Germany, Finland, and
Slovakia. The oregano oil product in capsules packed in Finland was found to be
adulterated with litsea (Litsea cubeba,
Lauraceae) oil, a widely used EO in the perfumery and cosmetic industry, but considered
to be a potential allergen due to its citral content.70
Essential oil expert Erich
Schmidt, PhD in his chapter on the adulteration of EOs in the Handbook of Essential Oils, 2nd edition,
reports that: “Origanum oil is adulterated with synthetic thymol and carvacrol,
or with limonene from different sources.” Adulteration with carvacrol is also
mentioned in Hager’s Handbuch der Pharmazeutischen Praxis.13
3.3 Accidental or intentional adulteration:
Both intentional and accidental
substitution seems to occur, based on anecdotal and scientific evidence.18,53
The scenario is complicated by the large heterogeneity of the Origanum genus and by the denomination
of different botanical genera under a single generic name.
According to ASTA, oregano herb adulteration is economically motivated and
intentional.63 Oregano is frequently
adulterated with Cistus spp., to
intentionally give a dark green color when added to oregano. This makes the
adulterated spice more visually appealing than pure oregano. The addition of
undeclared plant materials, such as myrtle, olive, sumac, and hazelnut leaves, may
be accidental, but in most cases these ingredients are added for
financial gain. Adulteration with savory, thyme, or marjoram frequently
reported in the literature is likely accidental.
The adulteration of
oregano EO appears to be economically motivated. The so-called “thyme oil
white” (see section 3.1.2) is available at a lower cost than oregano oil, and
therefore admixture of this oil with oregano oil can increase profit for the
seller.58,71
3.4. Frequency of occurrence:
The frequency of adulteration
of oregano herb appears to be high. Marieschi et al. found that 61 of
the 84 samples (72.6%) obtained from international wholesale traders exporting
to the European Union contained more
than the permissible 2% of foreign matter, including up to 77% winter savory
and up to 95% marjoram. Almost all the samples contained stem parts above the
permissible 2% content (stem contents between 1.5-12% were detected).53
Investigations into the
composition of commercial oregano spice samples in Argentina found that all
samples contained 5% or more of foreign matter. Using macroscopic and
microscopic features, colored wheat bran was detected in four out of six (67%),56 and 10 out of 36 (28%)
samples,55 respectively.
Between 30% to over 70% of oregano
samples in the UK and Ireland tested were found to include other non-oregano
materials, with a follow-up investigation of 54 oregano samples suspected to be
adulterated finding that 85% of the products contained 20% or more undeclared
bulking agents (cistus, myrtle, olive or sumac leaves).18,72 An investigation in Denmark
found that four out of 10 oregano herb samples contained between 30-50% bulking
agents such as cistus and olive leaves.73 Over 50%, or seven out of 12
of the popular brands tested in Australia, also contained substantial amounts
of other plant materials.64
The frequency of adulteration of oregano oil is not known as
the information is scant, but suggestive of widespread adulteration. Erich
Schmidt communicated that all of the 38 commercial samples of oregano oil analyzed
in his laboratory were adulterated with Spanish white thyme oil and p-cymene. (E. Schmidt, email November
29, 2017).
3.5 Possible safety/therapeutic issues:
According to ASTA, oregano
herb is commonly adulterated with non-toxic, less expensive leaves, such as
sumac, cistus, or myrtle. This economically motivated adulteration is done with
material that does not present a significant public health risk.63
As mentioned above, one of the adulterating materials of oregano
oil was found to be Litsea cubeba oil.70 This is an EO from a tree
widely found in China, Indonesia, and other parts of Southeast Asia that has
uses in the fragrance industry. The content of citral in the oil is typically about 70%
and is known to be a skin irritant and skin sensitizer.74 Cosmetic regulations in the
EU require citral, when present above 0.01% in rinse-off products (soaps,
shampoos), or above 0.001% in leave-on products (creams, deodorants)), to be
declared as an allergenic compound.75
3.6 Analytical methods to detect
adulteration:
Macroscopic and microscopic methods of analysis for the authentication of
oregano herb have recently been reported.17,53,54,76
Macroscopic identification criteria can be found, e.g., in the monograph of the
European Pharmacopoeia,17 or the publication by Varela
et al.55 Bononi et al. published
microscopy images of oregano, cistus, hazelnut, marjoram, olive, sumac, and
savory leaves.54 The European Pharmacopoeia also
details a thin-layer chromatography (TLC) test which can be used for oregano herb
and oregano EO.17 The extracted oregano herb
sample or the corresponding EO are run on a TLC silica gel plate R with
methylene chloride as the eluent and anisaldehyde as the reagent. Thymol is characterized
visually as a pink zone and carvacrol as a pale violet zone on the TLC plate. A
gas chromatography (GC) procedure for oregano EO has also been reported.17 In addition, ISO provides a
method to determine the identity of oregano oil in accordance with ISO standard
11024 (all parts).6
Gas
chromatography mass spectrometry (GC-MS) and high-performance liquid chromatography
mass spectrometry (HPLC-MS) methods to distinguish oregano leaf from olive leaf,
one of the most common oregano herb adulterants, have been published by Bononi et al.77,78
These methods take advantage of the presence of phenolic compounds, e.g.,
oleuropein in olive leaves, which are absent in oregano. Black et al. developed
and
fully validated a two-tier approach utilizing FTIR with multivariate
statistical analysis and ultra high-performance liquid chromatography high resolution
mass spectrometry (UHPLC-HRMS) to screen for and confirm oregano adulteration
by other plant materials, such as cistus, hazelnut, myrtle, olive, and sumac.18 The same FTIR method
was used by Wielogorska et al., and compared to a UHPLC-MS/MS method using ions
specific for hazelnut, myrtle, olive, and sumac to detect adulteration. The
detection limit (LOD) for FT-IR was established to be 10%; LODs for the
UHPLC-MS/MS method were below 2%, except for cistus leaves, for which no
suitable marker ion was found.72
An
unusual approach to detect oregano herb adulteration was published by Drabova
et al.69 These authors developed a statistical model to predict
oregano adulteration based on the GC-MS/MS analysis of 183 pesticides and
HPLC-MS/MS of 335 pesticides in 42 authentic and 34 adulterated oregano
samples. Using multivariate statistics, a model was constructed with a good
prediction ability according to the authors. Pyriproxyfen,
cyfluthrin, and cyhalothrin were identified as the most important markers of
possible adulteration.79
In response to the CHOICE consumer group food alert in the UK and
Australia,64 Reading Scientific
Services, Ltd., used microscopy and subsequent analyses of the constituents by
GC-MS. In addition, oregano samples were analyzed with Next Generation
Sequencing (NGS) for rapid determination of the DNA
sequences of all ingredients in a sample.80
Other rapid methods for detection of oregano herb adulterants in
crude material are based on developing and successfully implementing test for molecular
markers. These methods include the comparison of random amplified polymorphic
DNA (RAPD) markers of oregano and Rubus
spp., Cistus incanus, and Rhus coriaria added to oregano as bulk
extraneous material. Out of 20 random primers tested, 13 produced sequences
that allowed discrimination between Origanum
spp. and Rubus caesius, R. coriaria, and C. incanus, with a limit of detection of 1%.53
Sequence characterized amplified region (SCAR) markers for Satureja montana, O. majorana, and olive leaf adulterants were also developed from RAPD
markers.52,81,82
The SCAR primers gave rise to specific sequences and subsequent characterization of bands after gel electrophoresis for the detection of oregano adulterating plants at a concentration of
0.5%.52,81
Volatile adulterants in oregano oil lack the genetic information from
the plant and thus cannot be identified with DNA-based methods. The usefulness
of GC fingerprints to authenticate oregano EOs is hampered by the high
intraspecific variability in the EO composition.83,84 To
detect adulteration of oregano oil with synthetic carvacrol, a GC-stable isotope
ratio (SIR)-MS method is used to measure the stable isotopes. Differences in
the 2H/1H ratio (δ2H) between natural
carvacrol (δ2H: -272 to -264), and synthetic carvacrol (δ2H:
-190 to -225) can be used to determine the presence of undeclared synthetic
carvacrol. (E. Schmidt
email, November 30, 2017)
4. Conclusions
Adulteration
of oregano herb is prevalent, with a number of foreign materials including Origanum spp., Cistus spp., Thymus spp.,
Satureja spp., sumac, olive, and
myrtle leaves frequently detected. The addition of undeclared colored wheat
bran in commercial oregano spice products has been reported from Argentina. Confusion
and variations in the definition of oregano, and the number of species
commercially bearing the same name may result in accidental adulteration by
less thoroughly trained wildcrafters. Regional distinctions and guidelines are established
by spice trade associations, limiting impurities of extraneous materials to 1-2%.
The
prevalence of oregano oil adulteration is just beginning to be understood, and not
much information has been confirmed by laboratory tests and reports in the scientific
literature. It appears that more affordable EO components and byproducts from EO
processing from the fragrance and flavor industries are being mixed with oils
derived from Origanum, Thymus, and species from other genera. Although
ISO has established a standard for only Mediterranean oregano oil based on the distinct
flavor and aroma provided by high carvacrol and low thymol content, the
rationale for this decision does not seem to take into consideration the
complexity of the oregano herb definition including more than two dozen
different plants. Moreover, oregano oil health benefits are very likely shared
by several plant species with the common name “oregano” and not exclusively to Mediterranean
oregano.23 The potential lower cost of raw materials may increase the
opportunity for adulteration of Mediterranean oregano oil with essential oils,
or oil fractions from a large number of other Origanum species and other plants with a similar fragrance profile.
The adulteration
of oregano herb with low-cost materials from other plants is not considered a
health issue. However, some concerns have been raised with certain adulterants
of oregano oil: Allergic reactions may occur in people sensitive to citral when
oregano oil contains sufficient amounts of undeclared essential oils with a
high concentration of citral.
The ability
to sell adulterated oregano at a fraction of the price of high-quality
authentic material leads to a substantial market disadvantage for reputable
oregano suppliers and manufacturers. It also increases the pressure on these
companies to provide ingredients/products at lower cost to stay competitive. Appropriate
quality control procedures need to be in place to ensure the authenticity of
oregano-based ingredients.
* Some authors differentiate the volatile oil obtained
by steam distillation from essential oil. For the purpose of this document, no
such distinction has been made. †
The common name “oregano” is
used for both, O. vulgare subsp. hirtum and O. onites. However, Origanum
vulgare subsp. hirtum is also
known as Greek oregano, while O. onites is commonly referred to as
Turkish oregano (see section 1.6).
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REVISION SUMMARY
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Version 1, E. Bejar, PhD
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