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Abstract

Hydrosol beverages in Persian nutrition culture and ethnomedicine are the side products of essential oil industry that are used as delicious drinks or safe remedies. To investigate indications and chemical composition of hydrosol beverages for hyperlipidemia and cardiovascular conditions, Fars province was selected as the field of study. Ethnomedical data were gathered by questionnaires. The constituents of hydrosols were extracted with liquid/liquid extraction and analyzed by gas chromatography–mass spectrometry. Statistical analysis were used to cluster their constituents and find the relevance of their composition. A literature survey was also performed on plants used to prepare them. Thymol was the major or second major component of these beverages, except for wormwood and olive leaf hydrosols. Based on clustering methods, although some similarities could be found, composition of barberry, will fumitory, dill, and aloe hydrosols have more differences than others. These studies may help in developing some functional beverages or new therapeutics.

Keywords

essential oil cardiovascular hydrosol

Cardiovascular disease is a class of diseases that involve the heart or blood vessels and includes coronary artery diseases such as angina, myocardial infarction, stroke, hypertensive heart disease, cardiomyopathy, congenital heart disease, rheumatic heart disease, aortic aneurysms, peripheral artery disease, and venous thrombosis.

Coronary artery disease, stroke, and peripheral artery disease involve atherosclerosis. This also may be caused by high blood pressure, diabetes, smoking, lack of exercise, obesity, hypercholesterolemia, poor diet, and excessive alcohol consumption. According to the World Health Organization estimate, about 31% of all deaths worldwide are due to cardiovascular disease.^1,2

Functional beverages are nonalcoholic drinks that contains ingredients such as herbs, vitamins, minerals, raw fruit, or vegetable, which are consumed to provide specific health benefits beyond those of general nutrition. Most of the well-known functional beverages are used to boost energy, enhance the immune system, or increasing sense of well-being. These are marketed as sports drinks, energy drinks, enhanced fruit drinks, and enhanced water.

Aromatic waters, also known as floral water, distillate water, or hydrosols, are the side products of the essential oil and natural perfumery industry.³ They are prepared by dispersion of the plant materials via industrial hydrodistillation. This water is evaporated simultaneously with the essential oil of the plants as the container is heated. These vapors are condensed and liquefied together in a collecting vessel to give 2 phases. An essential oil phase and aromatic water enriched with different amounts of the volatile constituents of the plant that are partly or completely soluble in water.^4,5 These 2 phases are then separated; the essential oil goes to the pharmaceutical or cosmetic industry while the aromatic water depending on its unique properties is diluted 1:8 or 1:12 with water. They might go directly for marketing in big (250-1000 liters) containers without any further processing or be subjected to pasteurization in the factory. Subsequently, these preparations are kept in small (1-5 liters) plastic or glass containers for retail or wholesale marketing. In Iranian nutrition culture, they are used with sweeteners such as sugar or honey and served as natural delicious drinks. In Persian nutrition culture and folk medicine, aromatic waters are considered as very safe beverages used for medicinal purposes depending on the plants used for their production. Most aromatic waters are monoherbal but some have polyherbal constituents.^6,7 Depending on the plants used for preparation of each aromatic water, an overall nature is considered including, hot, cold, wet, dry, or moderate. They are also used as remedies to treat several conditions in oral and/or topical applications. Some adverse effects have been reported in folk medicine due to their improper application or ingestion. But, in general, they are considered as a safe and effective way of consuming essential oils and vital essence of medicinal plants or vegetables. In contrast to the pure essential oils, which are usually very potent or even harsh in terms of their biological activities, aromatic waters are moderate and balanced by the water and its water soluble volatile components.^8,9 Any of the aromatic waters has its own individual smell and composition, which is considerably different from the pure essential oil with which it was codistilled. The aromatic water has therefore additional properties not possessed by the essential oil alone.¹⁰ The moderate activity of these waters makes facilitates their use as daily soft drinks keeping their therapeutic features.

More than 50 different types of aromatic waters are produced and marketed in Iran, but as far as we know, the chemical constituents and biological activities of most of them have not been evaluated. Also, to the best of our knowledge no commercial products of them has been presented to the world markets. The aim of this study was to investigate constituents of aromatic waters and hydrosols used in Persian nutrition culture and folk medicine for hyperlipidemia and cardiovascular conditions as well as presenting them as potential functional soft drinks. Their nature and therapeutic indications have been also introduced in this study.

Materials and Methods

Information and Sample Collection

Fars Province, which is located in the south of Iran, was selected as the field of study. To gather information about different aromatic waters that are produced and used in Persian nutrition culture and folk medicine, the field study was conducted from March 2013 to March 2014 under the supervision of one local person as a native guide in all visits (84 manufactories). A suitable questionnaire was also prepared for this study, which was filled according to the information gathered in visits of the local manufactories or their shops. The frequency of each therapeutic effects for these aromatic waters from all questionnaires were calculated. The manufactories were also asked to rank these aromatic waters from 1 to 14 according to their mean of annual production over the past 3 years. The aromatic water with the lowest level of production was ranked 1. The ranking values from different manufactories are presented as mean ± standard deviation.

On the other hand, different aromatic waters that are used in Persian folk medicine as cardiovascular tonic or therapeutic beverages were purchased for further analysis. They are listed in Table 1 and coded as 1 to 14.

Table 1.

Plants’ Names and Their Medicinal Parts That Are Used to Prepare Aromatic Waters for Cardiovascular Diseases.

Aromatic Water Beverage Name	Aromatic Water Name in Persian	Scientific Name	Family	Plant Parts
Aloe	Aragh-e-Sabre zard; Aragh-e-Aloe	Aloe spp.	Xanthorrhoeaceae	Leaf
Azarole hawthorn	Aragh-e-Keyalak	Crataegus azarolus L.	Rosaceae	Leaf and fruits
Barberry	Aragh-e-Zereshk	Berberis vulgaris L.	Berberidaceae	Fruits
Dill	Aragh-e-Shevid	Anethum graveolens L.	Apiaceae	Leaf
Fenugreek	Aragh-e-Shanbaleile	Trigonella foenum-graecum L	Fabaceae	Leaf
Garlic	Aragh-e-Sir	Allium sativum L.	Amaryllidaceae	Bulb
Olive	Aragh-e-Zeytoon	Olea europaea L.	Oleaceae	Leaf
Oriental plane	Aragh-e-Chenar	Platanus orientalis L.	Platanaceae	Leaf
Parsley	Aragh-e-Jafari	Petroselinum crispum Mill.	Apiaceae	Leaf
Poleygermander	Aragh-e-Kalpooreh	Teucrium polium L.	Lamiaceae	Aerial parts
Turnip	Aragh-e-Shalgham	Brassica rapa L.	Brassicaceae	Root
Wormwood	Aragh-e-Dermaneh	Artemisia sieberi Besser	Asteraceae	Aerial parts
Will fumitory	Aragh-e- Shatareh	Fumaria parviflora Lam.	Papaveraceae	Aerial parts
A mixture of nettle, walnut, saatar (Shirazi thyme), olive, and celery leaves	Aragh-e-Taadol	A mixture of the following: Urtica dioica L.	Urticaceae	Leaf
		Juglans regia L.	Juglandaceae	Leaf
		Zataria multiflora Boiss.	Lamiaceae	Leaf
		Olea europaea L.	Oleaceae	Leaf
		Apium graveolens var. dulce	Apiaceae	Aerial parts

Phytochemical Analysis

Essential oils in each sample were extracted using a glass liquid extractor system. Five hundred milliliters of each sample was extracted with 500 mL of petroleum-ether as solvent. Petroleum-ether was heated to evaporation during 150 minutes. The solvent vapor was then transferred to the bottom of the beverage container. The vapor was liquefied in the beverage and due to the lower density it passed through the beverage toward the upper side of the container. At the same time, the essential oil of the sample was transferred from the aqueous phase to the petroleum-ether phase. In order to increase the essential oil concentration in the organic phase, after 150 minutes the used beverage was replaced with fresh beverage and the extraction procedure was continued for another 150 minutes. The extract of each sample was concentrated to approximately 10 mL at 40°C and 60 rpm using a basic rotary evaporator (IKA RV10), equipped with a Heidolph Rotavac vacuum pump.¹¹

Gas Chromatography–Mass Spectrometry

The concentrated extract of each aromatic water beverage was dehydrated and subjected to gas chromatography–mass spectrometry for the analysis of the respective essential oils. Agilent Technologies 7890 Gas Chromatograph with a mass detector (Model 5975C) was used in the present study. The gas chromatograph was equipped with a HP-5MS capillary column (phenyl-methylsiloxan, 30 m, 0.25 mm i.d.; Agilent Technologies; model 19091S-433 [60°C to 325/350°C]) and a mass spectrometer (Agilent Technologies; model 5975C), which was operating in EI mode at 70 eV. The interface temperature was 280°C, and the mass range was 30 to 600 m/z. The oven was heated (5°C/min) from 60°C to 220°C and then it was held for 10 minutes at 220°C. Helium was the carrier gas, and the flow rate was set to 1 mL/min. The components were identified by comparing the mass spectra and retention times with those of reference compounds, or with mass spectra in NIST or Willey libraries or in literature.^12
–14

Statistical Analysis

Principal Component Analysis

In order to cluster the aromatic water samples based on their constituents resulting from gas chromatography–mass spectrometry analyses, principal component analysis was used as an unsupervised clustering analysis technique. Briefly, all aromatic samples together with their corresponding vectors of constituents generated a matrix in MATLAB (Mathworks Inc, Natick, MA). Principal components of the resulted matrix were thereafter extracted using singular value decomposition algorithm as implemented in MATLAB software. Principal component analysis theory is based on a ranking approach where principal components are sorted according to their eigenvalues in such a way that the first one contains the most variation inside the data set. Consequently, the next principal component is extracted to be orthogonal with respect to the previous one. The plot of the first 2 principal components is therefore representative of the whole data in a 2-dimensional space. The orthogonal feature of the first 2 principal components makes a representation of the data set in a 2-dimensional space.

Hierarchical Cluster Analysis

To perform hierarchical cluster analysis, the resultant matrix as prepared in the previous experiment was subjected once again to MATLAB software. Cluster definitions were done by means of Euclidean distance as a way to measure similarities using unweighted pair group method (UPGMA). The plot of the distances versus samples was used to represent the data based on their similarities. The final dendrogram could represent the similarities between the samples via its connectivity patterns.

K-Means Analysis

K-means separates the points of an N-by-P data matrix into K clusters. These partitions are designed in such a way to minimize the sum of the within-cluster sums of point-to-cluster-centroid distances. K-means returns an N-by-1 vector representing the cluster index for each sample. Euclidean distances were used for clustering purposes in this experiment.¹⁵

Results and Discussion

Fars province is located in the south of Iran. It has an area of 122 400 km² and a population of 4.59 million people. Fars, or known in Old Persian as Pârsâ, is the original homeland of the ancient Persians. More than 84 manufactories are producing different medicinal aroma waters with traditional (65 manufactories) or full industrial techniques and equipment (about 19 manufactories). Most of these manufactories are located in Meymand and Darab cities, and their products are distributed all over the country.

Hydrosols and Their Phytochemicals

A list of aromatic waters that are used for hyperlipidemia and cardiovascular conditions was prepared according to indications on package labels or brochures written by their manufacturers or according to the information gathered via questionnaires (Tables 1 and 2).

Table 2.

Aromatic Waters’ Indications in Cardiovascular and Other Diseases.

Aromatic Water Beverage Name	Nature	Cardiovascular Indication	Other Indications	Dosing
Aloe	Cold nature	Anti-anemia Antidiabetic Antihypertension Blood cleansing	Antidandruff and skin lightening Gastrointestinal tonic To treat peptic ulcers To treat insomnia	100 mL BID or TID; before meal
Azarole hawthorn	Cold nature	Antiarrhythmic Anti-atherosclerosis Antipalpitation Cardio tonic	Antidiarrhea Antiepileptic Gastrointestinal tonic	100 mL TID; before meal
Barberry	Cold nature	Antiatherosclerosis Antidiabetic Antihypertension Cholesterol lowering	Antidysentery Choleretic and chologue Liver tonic To treat kidney stones To treat intestinal cancers	150 mL TID; after meal
Dill	Warm nature	Antihypertension Cholesterol lowering	Gastrointestinal tonic Galactogogue, menstruation inducer To treat urinary tract pain	150 mL TID; after meal
Fenugreek	Warm nature	Anti-anemia Antidiabetic Antihypertension	Anti-rickets For weight gain Hair tonic	150 mL TID; before meal
Garlic	Warm nature	Antihypertension Blood thinning Cholesterol lowering	Antibacterial Anthelmintic Hair tonic	100 mL TID; after meal
Olive	Cold nature	Antidiabetic Antihypertension Diuretic	Liver tonic To improve memory To treat headache and toothache	100-250 mL TID; before meal
Oriental plane	Cold nature	Antihypertension	Antipyretic For weight gain Nerve tonic; relief of pain	250 mL TID; before meal
Parsley	Cold nature	Anti-anemia Antihypertension Blood cleansing Diuretic	Anti-arthritis Antipyretic Galactogogue Gastrointestinal tonic	100 mL TID; before meal
Poleygermander	Warm nature	Antihypertension Antidiabetic Blood cleansing	Antiasthma Antibacterial Antiemetic Appetizer and liver tonic	100 mL TID; before meal
Turnip	Warm nature	Antihypertension Antidiabetic	Appetizer Antitussive Eye tonic	100 mL TID; before meal
Wormwood		Antihypertension Diuretic Perspirant	Antidiarrhea Appetizer Vermicide	100 mL TID; before meal
Will fumitory	Moderate nature	Antihypertension Blood cleansing Diuretic	Anti-scurvy Digestant	100 mL TID; before meal
Taadol (a mixture of nettle, walnut, saatar, olive and celery leaves)	Warm nature	Anti-atherosclerosis Antihypertension Antidiabetic Blood thinning Lipid lowering		100 mL TID; before meal

The aim of this study was to investigate the aromatic waters that are used in Persian nutrition culture and folk medicine, but some aromatic waters listed in Tables 1 and 2 have been mentioned also in some traditional manuscript such as Qarabadin-e-salehi ¹⁶ and Qarabadin-e-kabir.¹⁷ Most current ethnopharmacological knowledge in Iran has been derived from historical manuscripts.¹⁸

Traditional knowledge of aromatic waters recorded in historical manuscripts can help unravel the ethnopharmacological roots of traditional Iranian concepts and herbal classifications.

As seen in Table 1, the plants that are used to prepare these beverages belong to 11 different plants families. Apiaceae, Lamiaceae, and Asteraceae had a greater proportion than other families. The percentage of frequency of each cardiovascular application for these aromatic waters in all gathered questionnaires is shown in Figure 1. The higher percentage of frequency can show the higher importance of an application for a beverage. For example, in all questionnaires (100%), oriental plane aromatic water was suggested as a hypotensive and dill aromatic water as a hypolipidemic agent. while only a few informants believed that aloe aromatic water has anti-anemia properties. In ethnomedical surveys, cultural importance of species can reflect more accurate and more informants’ data obtained from questionnaires.¹⁹

Figure 1.

Frequency of citations in questionnaires for aromatic waters with cardiovascular effects.

As seen in Figure 1, most of these beverages were believed to show antihypertension properties. The second frequently cited application was antidiabetic effects.

In order to roughly evaluate the popularity of these aromatic waters in folk medicine, manufactories were also asked to rank these aromatic waters from 1 to 14 according to their mean of annual production over the past 3 years. Since these data were confidential for these manufactories, we used a ranking system. The aromatic water with the lowest level of production was ranked 1. The obtained ranking data from different manufactories are presented as mean ± standard deviation in Figure 2. Dill, will fumitory, Taadol, and oriental plane aromatic waters had higher annual production levels during the past 3 years. This popularity might be due to their efficacy, differences in prevalence of cardiovascular conditions in the region, or even the aromatic waters’ taste, aroma, or possible side effects during longer period of consumption.

Figure 2.

Ranking (1-14) of annual production level of aromatic waters in different manufactories over the past 3 years. Data are presented as mean ± standard deviation.

Most of these beverages are prepared from aerial parts (leaf and fruits) of the plants except in case of turnip (roots) and garlic (bulb). Different indications for cardiovascular conditions including cardiotonic, antihypertension, anti-arrhythmic, antipalpitation, blood cleansing, blood thinning, anti-anemia, anti-atherosclerosis, lipid lowering, antidiabetic, and diuretic were mentioned for these aromatic waters. It should be also mentioned that some of these beverages were believed to have cold nature while others had warm features. Other indications apart from cardiovascular specifications were also mentioned for these beverages, as summarized in Table 2.

As discussed earlier, aromatic waters have their own individual smell and compositions that are considerably irrelevant to the pure essential oils they were codistilled with. Therefore, it was necessary to elucidate chemical constituents of these aromatic waters by gas chromatography–mass spectrometry analysis after liquid-liquid extraction. The results are summarized in Table 3. In most of these aromatic waters, thymol is major or second major component except for wormwood and olive leaf aromatic waters. Carvacrol was also detected in all of these aromatic waters except for azarole hawthorn, wormwood, and olive leaf.

Table 3.

Aromatic Water Constituents Resulting From Gas Chromatography–Mass Spectrometry Analysis.

	Aloe	Azarole hawthorn	Barberry	Dill	Fenugreek	Garlic	Olive	Oriental plane	Parsley	Poley-germander	Taadol	Turnip	Will -fumitory	Worm-wood
2,3-Dimethoxytoluene	—	—	—	—	—	—		2.56	—	—	—	—	—	—
Acetophenone	—	—	—	—	—	—			—	4.41	—	—	—	—
Anethole (E)	—	—	—	0.53	—	—	—	—	—	0.98	—	—	—	—
Anethole (Z)	—	—	—	—	—	—	—	—	—	1.52	—	—	—	—
Apiole	—	—	—	—	—	—	—	—	1.28	—	—	—	—	—
Artemisia alcohol	—	—	—	—	—	—	—	—	—	—	—	—	—	2.99
Beta-fenchyl alcohol	—	—	—	—	—	—	2.14	—	—	—	—	—	—	—
A bisabolol oxide derivative	—	—	—	—	—	—	—	—	—	4.28	—	—	—	—
Bisabolol oxide A (α-)	—	—	39.98	—	—	—	—	—	—	—	—	—	—	—
Bisabolone oxide	—	—	16.54	—	—	—	—	—	—	—	—	—	—	—
Borneol	—	—	—	—	—	—	—	—	—	—	—	—	—	1.84
Camphor	—	—	—	—	—	—	—	—	—	—	—	—	—	23.15
Carvacrol	6.17		6.69	12.14	5.31	24.07	—	—	2.74	36.90	13.80	22.22	—	1.30
Carvone	3.89	—	—	9.90	12.88	2.37	1.93	23.22	—	—	15.84	5.18	—
1,8-Cineole	3.94	—	—	—	—	1.54	1.24			0.88	0.85	1.29	—	16.80
m-Cumenol	—	—	—	—	—	—	—	—	—	—	—	—	—	0.27
p-Cymen-7-ol	—	—	—	—	—	—	—	—	—	—	—	—	—	—
Damascenone (E-β)	—	—	—	—	—	—	—	—	—	—	—	—	—	—
Davanone	—	—	—	—	—	—			—	—	—	—	—	0.35
Dihydro carveol	—	—	—	—	—	—		5.96	—	—	8.93	—	—
Dihydro carveol (iso)		—	—	—	—	—	—	—	—	—	—	—	—	—
Dihydro carveol (neo)	1.87	—	—	—	—	1.83	—	—	—	—		2.35	—	—
Dihydro carvone (cis)	1.80	—	—	1.32	5.31	5.06	—	—	—	—	5.76	1.09	—	—
Dihydro carvone (trans)	—	—	—	0.66	2.74	1.79	—	—	—	—	—	—	—	—
Dihydroactinidiolide	—	—	—	—	—	—	6.43		—	—	—	—	6.70	—
Dill apiole	—	—	—	5.96	—	6.15	1.34	8.02	—	—	—	0.67	20.29	—
Dill ether	—	—	—	40.91	—	4.32	—	—	1.56	—	—	—	—	—
Ethylbenzene	—	—	—	—	—	—	—	1.26	—	—	—	—	—	—
Ethanone, 1-[2-(1,1-dimethylethyl)-1H-imidazol-4-yl])	—	—	—	—	—	—	—	—	—	—	1.08	—	—	—
Eugenol	—		—	0.91	—	—	—	—	—	5.09			—	—
Fenchone	—		—	—	—	0.36	—	—	—	—	—	0.58	—	—
Guaiacol (ρ-vinyl)	—		—	—	—	—	0.70	—	—	—	—	—	—	—
Hexadecanoic acid	—	7.71	—	—	—	—		—	—	—	—	—	—	—
Intermedeol (neo)	—	—	—	—	—	—		—	—	—	—	—	—	0.37
Methyleugenol	—	—	—	—	—	—	0.68	—	—	—	—	—	—
Jasmine (Z)	—	—	—	—	—	—	—	—	—	—	—	—	—	0.25
Linalool	—	—	—	—	—	0.48	—	—	—	—	—	0.57	—	1.10
Menth-2-en-1-ol (cis-ρ-)	—	—	—	—	—	—	—	—	—	—	—		—	0.35
Menthol	37.48	—	—	3.80	—	5.20	—	—	—	1.01	—	—	—	—
Menthone (trans)	5.46	—	—	2.41	—	1.13	—	—	—	—	—	0.53	—	—
Menthone (cis)	2.94	—	—	0.82	—	1.28	—	—	—	—	—	—	—	—
Methyl hexadecanoate	—	—	8.47		—	1.08	—	—	—	7.61		2.34	38.40	0.62
Methyl jasmonate (Z)	—	—	—	—	—	—	—	—	—	—	—	—	—	0.35
Methyl octadecanoate	—	—	1.16	—	—	—	—	—	—	—	—	—	5.82	—
Methyl 5-vinylnicotinate	—	—	—	—	—	—	29.75	—	—	—	—	—	—	—
Muurolol (α)	—	—	—	—	—	—	—	—	—	1.47	—	—	—	—
m-Xylene	—	—	—	—	—	—	—	—	—	—	—	—	—	—
Myristicin	—	—	—	—	—	0.33		—	34.00	2.03	—	—	—	0.42
Myrtenol	—	—	—	—	—	—	—	—	—	—	—	—	—	0.83
Nerol	—	—	—	—	—	—	—	—	—	—	—	—	—	0.26
o-Xylene	0.57	—	—	—	—	—	—	2.36	—	—	—	—	—	—
Phenol-4,ethyl-2-methoxy	—	—	—	—	—	—		—	—	—	—	—	7.53	—
Phenyl ethyl alcohol	—	—	—	—	—	—	0.79	—	—	—	—	—	—	—
Piperitenone	2.77	—	—	—	—	2.45	—	—	—	1.52	0.76	2.66	—	—
Piperitone	2.02	—	—	—	—	0.43	—	—	—	—	—	—	—	—
Pulegone	5.38	—	—	0.57	—	3.50	—	5.04	0.99	1.67	6.13	6.07		—
Pulegone ethanoate	—	—	—	—	3.01	—	—	—	—	—	—	—	—	—
p-Xylene	2.74	20.12	—	—	—	—	1.99	12.53	—	—	—	—	—	—
Spathulenol	—	—	—		—	—	—	—	—	—	—	—	—	0.75
Terpinen-4-ol	3.07	—	—	0.56	—	1.07	—	—	—	—	0.49	0.67	—	6.08
Terpineol (α)	1.68	—	—		—	0.46	—	—	—	—			—	1.83
Thujone (cis)	—	—	—	—	—	—	—	—	—	—	—	—	—	0.74
Thujone (trans)	—	—	—	—	—	—	—	—	—	—	—	—	—	5.63
Thymol	11.09	28.71	23.82	19.49	20.04	32.00	4.34	6.25	56.61	26.19	44.98	49.20	6.75	2.93
Thymol ethanoate	—	2.34	—	—	—	0.35	6.49	1.24	—	—	—	—	—	—
Yomogi alcohol	—	—	—	—	—	—	—	—	—	—	—	—	—	—

According to both hierarchical cluster analysis and K-means, oriental plane, fenugreek, and azarole hawthorn aromatic waters make a distinct cluster (Figure 3). The certain similarity of azarole hawthorn and fenugreek was also seen by means of principal component analysis. The reason for the observed similarities between these samples based on clustering analysis was the presence of comparable amounts of thymol (6.2% to 28.7%) in all 3 aromatic waters. In addition, carvone (23.22%) was the main component of oriental plane aromatic water, which was not detected in azarole hawthorn. According to hierarchical cluster analysis, fenugreek and azarole hawthorn made a subcluster that could be pertained to their similar thymol content.

Figure 3.

Cluster analysis of aromatic waters constituents based on principal component analysis (A) and hierarchical cluster analysis (B). The aromatic waters are as follows: 1 = aloe, 2 = oriental plane, 3 = wormwood, 4 = parsley, 5 = poleygermander, 6 = azarole hawthorn, 7 = turnip, 8 = fenugreek, 9 = will fumitory, 10 = dill, 11 = garlic, 12 = olive, 13 = barberry, and 14 = taadol.

Turnip, parsley, taadol, garlic, and poleygermander aromatic waters were classified as one cluster based on clustering analysis. According to K-means, there are 2 subclusters: one for turnip, parsley, taadol due to thymol (44.97% to 56.61%) as their main constituents and another for garlic and poleygermander, which contained 26% to 32% thymol. These aromatic waters (except for parsley) also contained comparable amount of carvacrol, 1,8-cineol, piperitenone, and pulegone. Parsley contained a considerable amount of myristicin (34%), which was not detected in other aromatic waters (Table 4).

Table 4.

Analysis of the Aromatic Waters’ Constituents Based on K-Means (sqEuclidean, 10 Epochs of Training).

Aromatic Waters’ Name	Class
Barberry	I
Dill	II
Parsley, turnip, and taadol	III
Will fumitory	IV
Aloe	V
Garlic and poleygermander	VI
Olive and wormwood	VII
Azarole hawthorn, fenugreek, and oriental plane	VIII

In contrast to other aromatic waters, wormwood and olive leaf had low thymol content (2%-6%). The main component of wormwood was camphor (23%), while in the case of olive leaf methyl 5-vinylnicotinate composed 29.76% of the aromatic water. Since these components were not detected in others they were clustered at distinct groups.

Based on clustering methods applied in this study, although some similarities could be found, composition of barberry, will fumitory, dill, and aloe aromatic waters revealed more differences than others. The main components of these aromatic waters were menthol (37%, aloe), methyl hexadecanoate (38.40%, will fumitory), bisabolol oxide A (39.98%, barberry), and dill ether (40.91%, dill).

Literature Survey

We could not find any reports on chemical composition of aromatic waters of the plants mentioned in Table 1. Thus, it was not possible to compare the results, but the major components of the reported essential oils are summarized in Table 5.

Table 5.

Profile of Essential Oils Reported in the Literature for the Plants Being Used to Prepare Cardiovascular Aromatic Waters and Hydrosols.

Plant Name		Profile of Essential Oils Reported in the Literature
Aloe		Profile of volatile components was not found in literature^24,25
Azarole hawthorn		Fruits: Limonene, 2-furaldehyde, 3-cyclohexane-2-methyl-1-propenyl, γ-terpinene²⁶
Azarole hawthorn		Leaves and flowers: n-Hexadecanoic acid, α-farnesene, alkanes²⁷
Barberry		Fruit: Benzaldehyde, benzyl alcohol, 1-hexanol, and (E)-2-hexenal
Barberry		Leaves and flowers: p-Cymene, limonene, ocimene²⁸
Dill		Limonene, Phellandrene, dihydrocarvone, and carvone²⁹
		α-Phellandrene, myristicin, dill ther, β-phellandrene²²
		Phellandrene, limonene, dill ether²³
Fenugreek		Aerial parts: ω-Cadinene, α-cadinol, γ-eudesmol, and α-bisabolol³⁰
Garlic		Leaves: Diallyl trisulfide, diallyl disulfide, methyl allyl trisulfide²¹
Garlic		Bulb: Diallyl disulfide, diallyl trisulfide, methyl allyl trisulfide²⁰
Olive		Leaf: 2-Hexenal, α-farnesene, linalool³¹
Oriental plane		Leaf: Profile of volatile components was not found in literature³²
Parsley		Myristicin, apiol, α-pinene, β-pinene
		β-Phellandrene, 1,3,8-p-menthatriene, α-,p-dimethylstyrene, myristicin, and β-myrcene³³
		Myristicin, β-phellandrene, p-1,3,8-menthatriene²²
Poleygermander		α-Pinene, β-pinene, and p-cymene³⁴
		α-Cadinol, 3-β-hydroxy-a-muurolene, a-pinene, and β-pinene³⁵
		Caryophyllene, torreyol, α-cadinol, and α-humulene³⁶
		α-Pinene, linalool, caryophyllene oxide, β-pinene, caryophyllene³⁷
Turnip		3-Butenylisothiocyanate, 4-pentenyl isothiocyanate, 2-methyl-5-hexenenitrile³⁸
Turnip		2-Butylisothiocyanate, 3-butenylisothiocyanate, ionone, menthol³⁹
Wormwood		Camphor, 1,8-cineole, and bornyl acetate⁴⁰
		Artemisia ketone, 1, 8-cineole, selin-11-en-4-a-ol, and lavandulon⁴¹
		Camphor, camphene, 1,8-cineol, β-thujone, and α-pinene⁴²
		β-thujone, camphor and α-thujone⁴³
Will fumitory		Profile of volatile components was not found in literature⁴⁴
Taadol	Celery	Leaf: 4-Chloro-4,4-dimethyl-3-(1-imidazolyl)-valerophenone, 1-dodecanol⁴⁵
		Leaf, stalk and roots: (Z)-3-butylidenephthalide, 3-butyl-4,5-dihydrophthalide, and α-thujene⁴⁶
		Leaf: Limonene, β-caryophyllene, and 3-butyl-4,5-dihydrophthalide⁴⁷
		Leaf: α-Pinene, β-pinene, myrcene, limonene, γ-terpinene, β-elemene, β-caryophyllene⁴⁴
	Nettle	Profile of volatile components was not found in literature
	Saatar	Thymol, carvacrol, linalool⁴⁸
	Walnut	Husks: (E)-4,8-Dimethyl-1,3,7-nonatriene, pinocarvone, pinocarveol, myrtenal, myrtenol⁴⁹
		(E,E)-4,8,12-Trimethyl-1,3,7,11-tridecatetraene, caryophyllene epoxide, verbenol, verbenone
		Leaf: Germacrene D, methyl salicylate⁵⁰

For aloe leaf, oriental plane leaf, and will fumitory, we could not find any reports and our article seems to be the first report on their volatile components. For some of these aromatic waters, such as barberry and poleygermander, garlic, and turnip, the major components in the aromatic waters and essential oils are completely different. Different allyl sulfides were reported as the major components of the garlic essential oils^20,21 and isothiocyanate derivatives as the major components of the turnip essential oil but none of these components were detected in the aromatic waters in the present study. In the case of dill essential oil, the major components were reported to be phellandrene, limonene, and myristicin, followed by dill ether.^22,23 In the present study, the major components of dill aromatic water was dill ether (40.9%), followed by thymol and carvacrol. On the other hand, the major components of parsley leaf (myristicin) and wormwood (camphor) were similar in aromatic waters and reported essentials but their percentage as well as nonmajor components are different (Tables 3 and 5). As it was expected, comparing the results of this study on components of the aromatic waters (Table 3) with the reports on essential oils (Table 5) shows that there is a remarkable difference between aromatic waters and essential oil components. This might be due to different water solubility of the volatile components; thus, some of these volatile components did not enter in the water phase while preparing aromatic waters. It seems that it is essential to consider different biological activities for aromatic waters due to different chemical compositions compared with pure essential oils.

Different cardiovascular effects of the plants used to prepare identified aromatic waters were investigated from the literature and are summarized in Table 6. We could not find any report on cardiovascular activity for any of the aromatic waters. But for some of these plants including fenugreek, wormwood, and celery there are some reports on extracted essential oil. Although it is not possible to compare the observed effects of the essential oils with aromatic waters due to differences in constituents as well as constituent’s concentrations, these reports strengthen the hypothesis of cardiovascular tonic effects for these aromatic waters.

Table 6.

Literature Review on Plants Used in Preparing Aromatic Waters With Cardiovascular Indications.

Aloe spp (Aloe vera, Aloe babadensis)		Antidiabetic and obesity	Phytosterol	In vivo⁵¹
		Antihypertensive	Leaf extracts and constituents (Aloe-emodin. Aloin A, etc)	In vivo⁵²
		Cardioprotective	Leaf gel	In vivo^53,54
		Hypoglycemic and hypolipidemic	Leaf gel	Clinical trial^55 –58
		Hypoglycemic and hypolipidemic	Gel extracts	In vivo^59,60
Azarole howthorn (Crataegus azarolus L.)		Cardioprotective	Aqueous extract of aerial part	In vivo⁶¹
		Antiarrhythmic	Aqueous extract of aerial part	In vivo⁶²
		Anti-atherosclerosis	Aqueous extract of aerial part	In vitro⁶³
		Anti-atherosclerosis	Aqueous extract of aerial part	In vivo^64,65
		Antipalpitation	Aqueous extract of aerial part	Clinical trial^66,67
		Hypotensive	Aqueous extract of aerial part	In vivo⁶⁸
		Positive inotropic and negative chronotropic	Aqueous extract of aerial part	In vivo⁶⁹
		Positive inotropic, diuretic and natriuretic	Procyanidine of the fruit	In vivo⁷⁰
		Vasorelaxant	Aqueous extract of aerial part	In vivo⁷¹
Barberry (Berberis vulgaris L.)		Antihypertension	Fruits in apple vinegar	Clinical trial⁷²
			Fruits aqueous extract	In vivo^73,74
			Methanolic extract of root and bark	In vivo⁷⁵
		Effects on non-alcoholic fatty liver	Fruits aqueous extract	Clinical trial⁷⁶
		Hypoglycemic	Berberine	In vivo⁷⁷
		Hypoglycemic	Fruits aqueous extract	In vivo^78,79
		Hypolipidemic	Fruits aqueous extract	In vivo⁸⁰
		Hypolipidemic	Ethanolic extracts of roots	In vivo⁸¹
Dill (Anethum graveolens L.)		Antihypertension	Hydroalcoholic extract of aerial part	Clinical trial⁸²
		Hypolipidemic	Hydroalcoholic extract of aerial part	Clinical trial^82 –85
		Hypolipidemic	Different fractions of leaves	In vivo⁸⁶
Fenugreek (Trigonella foenum-graecum L.)		Anti-anemia (increase hemoglobin and WBC level)	Seed extracts	Clinical trial⁸⁷
Fenugreek (Trigonella foenum-graecum L.)		Anti-anemia (increase hemoglobin and WBC level)	Seed extracts	In vivo^88 –91
		Antidiabetic	Seed extracts	Clinical trial^92 –95
		Antidiabetic	Seed extracts	In vivo^96 –98
		Antihypertension	Essential oil	In vivo⁹⁹
		Hypolipidemic	Seed extract	Clinical trial¹⁰⁰
			Seed extract	In vivo¹⁰¹
			Leaf extract	In vivo^102,103
Garlic (Allium sativum L.)		Anti-atherosclerosis	Aged garlic extract supplement	Clinical trial^104,105
		Antihypertension	Aqueous extract or powder	Clinical trial^106 –109
		Antihypertension	Aqueous extract or powder	In vivo^110 –112
		Hypoglycemic effects	Aqueous extracts or powder	Clinical trial^113,114
			Bulb extracts or powder	In vivo^115 –118
			Garlic oil	In vivo^117,119
		Hypolipidemic	Aqueous extracts or powder	Clinical trial and In vivo^{114,120 –126}
		Effects on thrombocyte aggregation	Aqueous extract	In vivo^127,128
Olive (Olea europaea L.)		Antihypertension	Leaf extracts	Clinical trial^{129 –134}
			Triterpenoids of the leaf	In vivo^135 –138
			Leaf extracts	In vivo¹³⁵
		Cardiovascular protection	Olive oil	Clinical trial^{131,137 –141}
		Diuretic	Leaf extracts	In vivo¹⁴²
		Hypoglycemic effects	Leaf extracts	Clinical trial and In vivo^143 –145
Parsley (Petroselinum crispum Mill.)		Antidiabetic	Extracts of aerial part	In vivo^146,147
		Antihypertension	Extracts of aerial part	In vivo^146,148
		Antiplatelet	Aqueous extracts	In vitro^148 –150
		Cardiovascular protection	Extracts of aerial part	In vivo^151,152
		Diuretic	Extracts of aerial part	In vivo and in vitro^153,154
Poleygermander (Teucrium polium L.)		Antidiabetic	Extracts of aerial part	Clinical trial¹⁵⁵
Poleygermander (Teucrium polium L.)		Antidiabetic	Extracts of aerial part	In vivo^156 –159
		Antihypertension	Extracts of aerial part	In vivo^160,161
		Hypolipidemic	Aqueous extract of aerial parts	In vivo^{159,162 –164}
Turnip (Brassica rapa L.)		Antidiabetic	Root extracts	In vivo^165 –168
		Hypolipidemic	Seed oil	Clinical trial¹⁶⁹
		Hypolipidemic	Root extracts	In vivo^170,171
Wormwood (Artemisia sieberi Besser)		Antidiabetic	Essential oil from aerial parts	In vivo^172 –174
		Antihypertension	Essential oil	Hypothesis¹⁷⁵
		Cardiovascular protection	Essential oil from aerial parts	In vivo¹⁷⁶
		Hypolipidemic	Hydroethanolic extract	In vivo¹⁷⁷
Will fumitory (Fumaria parviflora Lam.)		Hypoglycemic	Extracts of aerial parts	In vivo^178,179
Will fumitory (Fumaria parviflora Lam.)		Hypolipidemic	Aerial parts	In vivo^180,181
Taadol	Celery (Apium graveolens)	Antihypertension	Extracts of aerial parts	Clinical trial^182,183
Taadol	Celery (Apium graveolens)	Antihypertension	Extracts of aerial parts	In vivo^184 –187
		Hypoglycemic	Extracts of aerial parts	In vivo^188 –190
		Hypolipidemic	Seed extract	In vivo^191 –194
		Hypolipidemic	Essential oil	In vivo¹⁸⁷
	Nettle (Urtica dioica L.)	Antihypertension	Root extracts	Clinical trial¹⁹⁵
			Root extracts	In vivo¹⁹⁶
			Extracts of aerial parts	In vivo^195 –199
		Hypoglycemic	Extracts of aerial parts	Clinical trial²⁰⁰
			Extracts of aerial parts	In vivo^{195,197,199,201 –205}
			Seed extracts	In vivo²⁰⁶
		Hypolipidemic	Extracts of aerial parts	In vivo^207 –209
		Antihypertension	Extracts of aerial parts	In vivo²¹⁰
	Saatar (Zataria multiflora Boiss.)	Antidiabetic	Essential oil	In vivo^208,211,212
	Saatar (Zataria multiflora Boiss.)	Antidiabetic	Extracts of aerial parts	In vivo^210,213
	Walnut (Juglans regia L.)	Antihypertension	Leaf extracts	In vivo²¹⁴
		Antidiabetic	Leaf extracts	Clinical trial²¹⁴
			Seed extract	Clinical trial^215 –218
			Leaf extracts	In vivo²¹⁹
			Septum extract	In vivo²¹⁹
			Flower extract	In vivo²¹⁹
		Hypolipidemic	Seed extract	Clinical trial^{214,219 –223}
		Hypolipidemic	Seed extract	In vivo²²⁴

For other plants, different aqueous, ethanol, methanol extracts or plants powders were investigated and it is not clear if the volatile components had a role in observed effects. On the other hand, for many of the plants listed in the Table 6, the medicinal parts that were investigated are different from those that are used to prepare the aromatic waters in Persian ethnomedicine. For oriental plane we could not find any related report. This study was not intended to investigate the efficacy of these aromatic waters, but high production level and consumption of these aromatic waters in Persian nutrition culture and folk medicine might be related to their efficacy.

Overall, this article introduced some aromatic waters that are used for hyperlipidemia and cardiovascular conditions in Persian nutrition culture and folk medicine with different popularity and sales values. As was expected, their chemical composition was different from the essential oils of the plants used for their production. But cluster analysis showed that despite the differences in the plant family and medicinal parts used to prepare them, some similarity can be found in their chemical compositions. In most cases thymol was the major or second major component of these beverages.

Investigating aromatic waters scientifically may lead to the development of some functional beverages and soft drinks as a safe way of administration of essential oils or even new therapeutic components.

Footnotes

Authors’ Note

This study was part of the PharmD thesis project of Seyed Mahmoud Moheimani.

Acknowledgments

The authors also want to thank Nahal Shamaeezadeh (PharmD student at Shiraz University of Medical Sciences) for helping in extraction procedures.

Author Contributions

AH wrote the draft and contributed in guidance and data collection. AS contributed in the guidance and revisions of the final version of the article. SM, MM, and HE contributed in data collection and analyzing data.

Declaration of Conflicting Interests

The authors declared no potential conflicts of interest with respect to the research, authorship, and/or publication of this article.

Funding

The authors disclosed receipt of the following financial support for the research, authorship, and/or publication of this article: This study was funded by Shiraz University of Medical Sciences (Grant # 92-01-70-7065).

Ethical Approval

This study was an experimental and laboratorial work and did not require ethical approval.

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An Overview on Indications and Chemical Composition of Aromatic Waters (Hydrosols) as Functional Beverages in Persian Nutrition Culture and Folk Medicine for Hyperlipidemia and Cardiovascular Conditions

Abstract

Keywords

Materials and Methods

Information and Sample Collection

Phytochemical Analysis

Gas Chromatography–Mass Spectrometry

Statistical Analysis

Principal Component Analysis

Hierarchical Cluster Analysis

K-Means Analysis

Results and Discussion

Hydrosols and Their Phytochemicals

Literature Survey

Footnotes

Authors’ Note

Acknowledgments

Author Contributions

Declaration of Conflicting Interests

Funding

Ethical Approval

References