*3.3. Nutmeg and Mace*

Nutmeg and mace spices are obtained from different parts of the same fruit of the nutmeg (*Myristica fragrans*; Myristicaceae) tree. Nutmeg is the dried kernel of the seed, whereas mace is the dried aril surrounding the seed [21]. Myristic acid's name is derived from *Myristica fragrans*, from which it was first isolated [22]. In the present study, myristic acid was 60.8% of total fatty acids in nutmeg, followed by oleic (C18:1n9c; 13.4%), linoleic (C18:2n6c; 11.9%), and palmitic (C16:0; 8.94%) (Figure 1A). Surprisingly, in mace, linoleic acid was 33.7% of total fatty acids, followed by palmitic (30.6%) and oleic (28.0%). Myristic acid was only 1.59% of the total fatty acids (Figure 1C, Table 2). In the investigations of Al-Khatib et al. [23], myristic acid was recorded as being 79.7% of the total fatty acids in nutmeg. Kozłowska et al. [24] analyzed the fatty acids composition of plant seeds, including anise, coriander, caraway, white mustard, and nutmeg. They reported dominance of oleic (56.5%), palmitic (18.29%), and linoleic (13.6%) acids in nutmeg. These contrasting observations probably arose as these authors reported only above C16 fatty acids. Myristic acid is widely used in the food industry as a flavor ingredient. It is approved as a pharmaceutical excipient by the Food and Drug Administration (FDA) and declared generally recognized as safe (GRAS) by various regulators [25].

#### *3.4. Erucic Acid in White Mustard*

Mustard (*Sinapis alba*; syn *Brassica alba*) seeds are well known for the occurrence of a substantial amount of erucic and eicosenoic acid [24]. In the present study, white mustard seeds were found containing 17.3% and 8.0% of erucic and eicosenoic acid, respectively (Figure 2A, Table 2). High intake of erucic acid is considered harmful for cardiac health [26]. The panel on contaminants in the food chain established a tolerable daily intake (TDI) of 7 mg/kg body weight (BW) for erucic acid based on a no-observed adverse effect level (NOAEL) for myocardial lipidosis in rats and pigs [26]. Considering the 43 mg of total fatty acids/g of white mustard seeds, consumption of 100 g of seeds may provide 7.31 mg of erucic acid. The intake of erucic acid from white mustard used as food condiments in daily food preparations is far below the TDI and is safe for consumption.

**Figure 2.** (**A**) The gas chromatography (GC)-flame ionization detection (FID) profiles of fatty acid methyl esters (FAMEs) of white mustard seeds. (**B**,**C**) The GC-mass spectrum of eicosenoic acid and erucic acid from white mustard seeds. (**D**) The GC-FID profiles of FAMEs of parsley leaves. The numbers, 4, 9, 10, 13, 14, and 16 correspond to peak numbers illustrated in Table 1. BHT: Butylated hydroxytoluene (A synthetic antioxidant used during lipid extraction).

Petroselinic acid (C18:1n12c; an isomer of oleic acid) is the major component of the lipid constituent of Apiaceae family seeds [27,28]. In a previous study [27] of dill (*Anethum graveolens*) seeds, 87.2% of total fatty acids were composed of petroselinic acid. Similarly, in celery (*Apium graveolens*), coriander seeds (*Coriandrum sativum*), and fennel seeds (*Foeniculum vulgare*), petroselinic acid was recorded as being 56.1%, 72.8%, and 31.32% of total fatty acids. In agreement with the present study, we have also recorded the 50.4%, 49.4%, 62.1%, and 63.3% of petroselinic acid in dill, coriander celery, and fennel seeds, respectively (Table 2). And a similar high amount of petroselinic acid was reported to be in the seeds of other Apiaceae family plants, such as caraway (*Carum carvi*, 34.1%) and cumin (*Cuminum cyminum*; 49.9%). In seeds of different varieties of caraway, Reiter et al. [28] recorded 33.5–42.5% of petroselinic acid, which is in agreement with the present study. Petroselinic acid possesses potent anti-inflammatory and antiaging properties by reducing the metabolites of arachidonic acid [29]. And owing to its anti-aging properties, petroselinic acid is widely used in cosmetics or dermatological compositions [29]. Surprisingly, petroselinic acid was not detected in herbs (leaves) of the Apiaceae family member parsley (*Petroselinum crispum*). In the parsley herb, hexadecatrienoic (C16:3n3) was reported to be 17.7% of the total fatty acids (Figure 2D), whereas no other spices were found to contain this fatty acid. Parsley has been previously classified as a "16:3" plant owing to the presence of a significant amount of hexadecatrienoic acid in photosynthetic tissues, which is part of primitive lipid metabolism [30].

#### *3.5. Fat Quality Indices*

The present study is based on the fatty acid composition of 34 spices and herbs. We evaluated them for fat quality indices, including the *n*–6/*n*–3 ratio, AI, TI, and h/H fatty acid ratios (Table 3). Among the studied spices and food condiments, the ratio of *n*–6/*n*–3 PUFAs was found to be in the range of 0.36 (oregano) to 85.99 (cumin). In view of health benefits associated with the consumption of *n*−6/*n*−3 PUFAs ratio of 0.5–2.0 (nearest to 1:1), lipids obtained from leaf spices, including tarragon (0.76), bay leaf (1.33), basil (0.55), marjoram (0.75), parsley (0.48), white mustard (0.95), sage (0.86), and thyme (0.52) can be considered to be beneficial. In general, the high occurrence of α-linolenic acids compared to linoleic acid is responsible for the low *n*−6/*n*−3 ratio in leaves (photosynthetic tissue).

In view of the high risk of CVD and other chronic diseases that are associated with the dietary intake of SFAs [11], fats with a PUFAs/SFAs ratio lower than 0.45 are not advised for diet [31]. In the present study, PUFAs/SFAs ratios ranged from 0.17 (nutmeg) to 4.90 (cumin). Low PUFAs/SFAs ratios of 0.17 in nutmeg lipids are the result of the dominance of myristic acid (an SFA; Figure 1A), whereas in the case of cumin, linoleic acid is dominant over SFAs. In addition to the nutmeg, low PUFAs/SFAs ratios (<0.44) were recorded from galangal root (0.29), lemongrass (0.24), rosemary (0.28), and sage (0.38) because of the occurrence of a substantial amount of palmitic acid (Figure S2).

Fats with lower AI and TI and higher ratios of h/H fatty acids are recommended for minimizing the risk of CVD [32]. In the present study, a significant difference was recorded for AI, TI values as well as h/H fatty acids among the studied spices and herbs. The lowest significant values of the AI (0.06) and the highest ratios of h/H fatty acids (17.0) were obtained from cumin seeds (Table 3, Figure 3), because of the presence of a low amount of atherogenic lauric, myristic, and palmitic fatty acids, and high amounts of hypocholesterolemic C18:1 MUFAs and PUFAs. Whereas the lowest significant values of TI (0.08) were recorded in white mustard, due to the low contents SFAs and high content of PUFAs.

Overall, based on a higher ratio of h/H fatty acids and their lower AI and TI values, cumin, coriander, fennel, and dill spices have the healthiest fatty acid profiles (Figure 3). These spices belong to the Apiaceae family. White mustard also represents a higher ratio of h/H fatty acids and lower values of AI and TI. However, it contains a substantial amount of erucic acid.

In Figure 3, cumin, coriander, fennel, and dill spices top the fat quality indices, the ratio of h/H fatty acids, AI, and TI. However, the occurrence of a very low proportion of α-linolenic acid (a *n*−3 PUFA; 0.35–0.85%) and a fairly good amount of linoleic acid (a *n*–6 PUFA; 19.60–33.34%) in these spices, give rise to the high ratio of *n*–6/*n*–3 PUFAs (24.02–85.99), which is substantially higher than the recommended ratio of 1:1. Considering this, the culinary use of these spices can be recommended with *n*–3 PUFA rich components to obtain the overall *n*–6/*n*–3 PUFAs ratio of 1:1.

Previously, we had analyzed the total phenolic contents (TPC) and antioxidant activities of 39 spices and herbs (including the 34 spices and herbs investigated in the present study) and found that cloves possess the highest antioxidant activities, followed by allspice, cinnamon, oregano, and marjoram [33]. The high antioxidant activities of these spices and herbs were probably the results of the richness of phenolic compounds, as the antioxidant activities showed a good correlation (0.835–0.966) with TPC. In contrast, in the present study, cumin, coriander, fennel, and dill spices showed the healthiest fatty acid profile among the 34 spices and herbs. These observations show that the selection of healthy spices and herbs may vary with nutrient requirements. Thus, in the present study, cumin, coriander, fennel, and dill spices are the recommendations based on the fatty acid profile. However, other spices and herbs might be richer in other health-beneficial dietary components.



Values are the mean of six determinations. PUFAs: total polyunsaturated fatty acids; MUFAs: total monounsaturated fatty acids; SFAs: total saturated fatty acids; AI: atherogenic index; and TI: thrombogenic index; h/H: ratios of hypocholesterolemic (h)/hypercholesterolemic (H) fatty acids. The letters a and b within a column represent the highest and lowest significant (*p* < 0.05) values, respectively. Sample numbers (S1–S34) correspond to the Table 1.

**Figure 3.** (**A**) Illustrations showing the high content of healthy monounsaturated (MUFAs) and polyunsaturated fatty acids (PUFAs) in cumin, compared to low contents of MUFAs and PUFAs, and high contents of saturated fatty acids (SFAs) in nutmeg. (**B**) Arrangements of studied spices and herbs in ascending/descending order according to the fat quality indices of the ratio of hypocholesterolemic (h)/hypercholesterolemic fatty acids, atherogenic index (AI), and thrombogenic index (TI).

#### **4. Conclusions**

Spices belonging to Apiaceae family plants (cumin, coriander, fennel, and dill) are an exceptionally rich source of monounsaturated fatty acids (MUFAs) in the form of petroselinic acid, a good amount of polyunsaturated fatty acids (PUFAs; linoleic acid), and a small amount of saturated fatty acids. And, with high proportions of MUFAs and PUFAs, the Apiaceae family spices top the fat quality indices, particularly in terms of a higher ratio of hypocholesterolemic/hypercholesterolemic fatty acids, and lower values of the atherogenic index and the thrombogenic index (Figure 3).

**Supplementary Materials:** The following are available online at https://www.mdpi.com/article/ 10.3390/foods10040854/s1, Figure S1: (A) The gas chromatography (GC)-flame ionization detection (FID) profiles of fatty acid methyl esters (FAMEs) of cardamom. (B) The GC-mass spectrum of dominating fatty acid (Palmitic acid); Figure S2. (A–C) The gas chromatography (GC)-flame ionization detection (FID) profiles of fatty acid methyl esters (FAMEs) of lemongrass, rosemary, and Sage. The GC-mass spectrum of dominating fatty acid (Palmitic acid). The numbers, 4, 7, 9, 11, and 14 correspond to peak numbers illustrated in Table 1. BHT: Butylated hydroxytoluene (A synthetic antioxidant used during lipid extraction).

**Author Contributions:** Conceptualization, R.K.S. and A.D.A.; methodology, R.K.S. and A.D.A.; software, R.K.S. and A.D.A.; validation, R.K.S. and A.D.A. and Y.-S.K.; formal analysis, R.K.S.; investigation, R.K.S.; resources, Y.-S.K.; data curation, R.K.S. and A.D.A.; writing—original draft preparation, R.K.S.; writing—review and editing, A.D.A. and Y.-S.K.; visualization, Y.-S.K.; supervision, Y.-S.K.; project administration, R.K.S.; funding acquisition, R.K.S. All authors have read and agreed to the published version of the manuscript.

**Funding:** This paper was supported by the KU Research Professor Program of Konkuk University, Seoul, Republic of Korea and "The APC was supported by Konkuk University research fund (2021A0190061)".

**Acknowledgments:** This paper was supported by the KU Research Professor Program of Konkuk University, Seoul, Korea.

**Conflicts of Interest:** The authors declare no conflict of interest.
