1. Introduction
The origin of wine is as old as human civilization. Because of the rich, varied composition and its health-promoting effects, the properties of wine have been studied for a long time. The term “wine” originates from the Greek word “Fοινος” which means both wine and vine. It is an alcoholic product obtained as a result of full or partial alcoholic fermentation of grape (grape must), and/or some fruits [1]. Combinations can also be found, but in general, the term wine is mostly related to beverages prepared exclusively from fermented grapes. The economic significance of wine production as a branch of the food industry is of great importance and should not be considered only in the utilization of raw materials, such as grapes or apples (or other fruits), but in the production of a beverage with valuable nutritional, social, cultural, religious, and entertainment aspects [1]. One of the most attractive attributes of wine is its aroma, which is mainly formed in the course of fermentation and during wine aging. In addition to the raw grape material (maturity, variety, sugar content, and so on), which is usually the main target studied by the winemakers, the starter yeasts and microorganisms are also in focus, since their development and metabolism are responsible for aroma formation [2,3,4]. Additionally, the wine flavor can be modulated and improved by supplementations, which can influence the aroma bouquet during the fermentation process or introduce other aroma notes [5,6].
The aromatized wine-type beverages (AWTBs) belong to the group of flavored alcoholic beverages often called “Alcopops”, a name derived from alcoholic and soft (pop) drinks. They could be considered as distilled alcoholic drinks, wine, and malt beverages, to which fruits (mainly fruit juices) or other flavoring agents are added [1,7]. A typical example of such a wine-type beverage is prepacked “sangria”, a mixture of red wine and orange juice. The data suggested that the global sales of aromatized wines from around 500,000 bottles (2010) increased to 20,000,000 bottles in 2015 [8]. In recent years, flavored alcoholic beverages exhibited a stable market share and are estimated at USD 13.84 billion for 2021. The expected augmentation for the next 6–7 years is by 12.5%, and to reach over USD 15 billion [9].
The main method for the production of AWTBs is by maceration of white wine (or beverage on its base; it is also possible to utilize rosé type wines) with herbs, flavorings, plant-based materials, or carbohydrates (or substances derived from them), followed by filtration, blending of batches, and stabilization. The other approach includes obtaining plant extracts first, and then mixing them with wine. Nevertheless, many different approaches, variations, and modifications, depending on the manufacturer, exist [1,6]. The literature describing the utilization of waste raw materials or byproducts from the food or agricultural industry in winemaking is scarce, mainly because of the strict regional regulations. In most cases, byproducts of the wine-making industry are preferred [6,10,11]. In addition, the replacement of sulfur dioxide with byproducts of the olive industry [12] was also investigated. There are few attempts focused on the preparation of nontraditional flavored wines with the addition of byproducts from the essential oil industry [13] or the utilization of rose hips [14].
The rose oil industry, well-developed in Turkey, Bulgaria, Iran, and France, generates large quantities of solid and liquid wastes yearly. Some of these materials have been successfully valorized, but in general, most of the biomass is still discarded. Attempts were extensively focused on searching for approaches for the valorization of rose oil industry byproducts [15]. Due to technological and economic reasons, the distillation of fresh plants does not result in the complete removal of the essential oil and, therefore, valuable substances such as aroma compounds, polyphenols, and polysaccharides can be found in the residues [16]. For this reason, rose byproducts can be used to provide a pleasant rose aroma and health-promoting features of the food products [15].
The amount and type of aroma substances found in wines strongly depend on the grape variety and quality [17]. Some yeast strains used for grape must fermentation naturally yield substances with rose odor, such as cis- and trans-rose oxide, β-damascenone, 2-phenyl ethanol, benzophenone, and phenethyl propionate [4,13], which attribute a pleasant rose aroma to the final bouquet. Additionally, the aroma of wines can be modulated by the addition of herbs, spices, and various aroma compounds, achieving new aromatized wines. Therefore, the main purpose of the present research was to utilize and valorize solid byproducts from the essential rose oil industry for the preparation of new aromatized wine-type beverages having mild and pleasant rose aromas.
2. Materials and Methods
2.1. Materials
The bio-certified Rosa damascena Mill. industrial solid byproducts were collected from EKOMAAT Ltd. Distillery (Mirkovo, Sofia, Bulgaria; 2018). Vitis vinifera L. cv Mavrud with 205 g/L total sugars, pH 3.47, and 6.57 g/L titratable acids (Brestovica, region of Plovdiv, Bulgaria; 2018) was used for the preparation of the AWTBs. The Lallzyme cuvée blanc and the Saccharomyces cerevisiae yeast strain Lalvin D47 were obtained from Lallemand (St Simon, France). The Polymust press and bentonite were obtained from Laffort (Bordeaux, France). The sulfurous acid was provided by the Villa Yustina winery. Acetonitrile, acetic acid, dichloromethane, sodium acetate, pyridine, N,O-Bis-(trimethylsilyl)-trifluoroacetamide (BSTFA), gallic acid, 3,4-dihydroxy benzoic acid, chlorogenic acid, neochlorogenic acid, ellagic acid caffeic acid, p-coumaric acid, ferulic acid, sinapic acid, rosmarinic acid, cichoric acid, cinnamic acid, quercetin, quercetin-3-β-glucoside, myricetin, kaempferol, naringin, catechin, and epicatechin were obtained from Sigma-Aldrich (Rockville, MD, USA). The DPPH (2,2-diphenyl-1-picrylhydrazyl) was from Merck (Darmstadt, Germany).
2.2. Preparative Methods
2.2.1. Preparation of Ethanol–Water Extracts of Rose Oil Industry Byproducts
The ethanol–water extracts were obtained by treatment with 30%, 70%, and 90% ethanol (v/v) of the dried distilled rose biomass. The extraction was carried out twice at 60 °C for 1 h at constant stirring at 150 rpm. In the first extraction, hydromodule 1:10 (50 g rose oil industry byproducts with 500 mL extracting agent) was used. Then, the mixture was kept for 24 h at room temperature and was filtered. A second extraction was carried out with the solid residue under the same conditions, but using 250 mL of extracting agent. After filtration, the two extracts were combined.
2.2.2. Grape Must Preparation
The wines were prepared in the facilities of Villa Yustina winery (Ustina, Plovdiv, Bulgaria). The grapes were crushed in a hydraulic press and 50 mg/L SO2 and 3 g/kg Lallzyme cuvée blanc were added. The must was cooled down to 9 ± 1 °C and kept for 12 h with periodic recirculation. After clarification, the precipitates were removed by filtration. The filtrated must was divided into two parts: (1) 50 L for preparation of rosé wine, and (2) 25 L for preparation of AWTBs with added solid rose byproducts (cofermentation).
2.2.3. Fermentation of the Grape Must
An aliquot of 50 L grape must was transferred to a fermentation vessel, the temperature was raised to 16 ± 1 °C, and inoculated with rehydrated Saccharomyces cerevisiae yeast (0.25 g/L). The fermentation was conducted for 11 days at 16 ± 1 °C. The mixture was filtered to remove the remaining precipitation and solid materials, sulfited with sulfurous acid to a final concentration of 50 mg/L SO2, and 25 g Polymust press (clarification agent for wine treatment) was added. The rosé wine was stored for two weeks, filtered, and divided into two parts of 25 L each.
2.2.4. Aromatized Wine-Type Beverages Preparation
Three types of AWTBs were prepared, namely, variants 1—by the addition of 70% (v/v) ethanolic extracts of rose oil industry byproducts to preliminarily prepared rosé wine, variants 2—by the addition and maceration of solid rose oil industry byproducts to preliminarily prepared rosé wine, and variants 3—by the addition of rose oil industry byproducts to the unfermented grape must and further cofermentation.
The first variants (series ARW_E) were prepared as follows: the preliminarily prepared rosé wine (25 L) was divided into five aliquots, 5 L each, and 70% ethanolic extracts of rose oil industry byproducts were added at different amounts to each batch, namely, 0 mL (control wine, ARW_E_C), 50 mL (ARW_E_50), 100 mL (ARW_E_100), 200 mL (ARW_E_200), and 400 mL (ARW_E_400). The AWTBs were mixed well, bottled, and stored at 18 ± 1 °C in the dark.
The second variants (series ARW_M) were prepared as follows: the preliminarily prepared rosé wine (25 L) was divided into five parts (5 L each), and solid rose oil industry byproducts were added at different amounts to each batch, namely, 0 g (control wine, ARW_M_C), 12.5 g (ARW_M_12.5), 25 g (ARW_M_25), 50 g (ARW_M_50), and 100 g (ARW_M_100). The postfermentative maceration was allowed to proceed for 35 days at 18 ± 1 °C in the dark. After that, the mixtures were filtered, bottled, and stored at 18 ± 1 °C in the dark.
The third variants (series ARW_CoF) were prepared as follows: the 25 L grape must was divided into five aliquots (5 L each), and solid rose oil industry byproducts were added at different amounts to each batch, namely, 0 g (control wine, ARW_CoF_C), 12.5 g (ARW_CoF_12.5), 25 g (ARW_CoF_25), 50 g (ARW_CoF_50), and 100 g (ARW_CoF_100). The temperature of the mixtures was raised to 16 ± 1 °C, and each of them was inoculated with the rehydrated Saccharomyces cerevisiae yeast strain (0.25 g/L). The cofermentation of the grape must and the solid rose oil industry byproducts took place for 11 days at 16 ± 1 °C. The mixture was filtered to remove the precipitations and solid materials, sulfited with sulfurous acid to reach a final concentration of 50 mg/L SO2, and 25 g Polymust press (clarification agent for wine treatment) was added. The beverages were kept for two weeks, filtered, bottled, and stored at 18 ± 1 °C in the dark.
2.3. Analytical Methods
The relative density (specific gravity) of the grape must was measured hydrometrically according to the OIV-MA-AS2-01B: R2009 type IV method [18]. The content of ethanol in the control rosé wine and the AWTBs was determined according to Cioch-Skoneczny et al. [19], employing the pycnometric method. The amounts of sugars, titratable, and volatile acids in the wines were determined according to Tchobanova [20].
Total polyphenol compounds were determined with Folin–Ciocalteu’s reagent [21]. Gallic acid was used for standard curve preparation, and the values were presented as gallic acid equivalent (GAE) per liter of beverage. The antioxidant activities of the beverages were evaluated by the oxygen radical absorbance capacity (ORAC) assay [22] and the hydroxyl radical averting capacity (HORAC) assay [23], as described in detail by Slavov et al. [16]. The pH-differential method [24] was employed for the determination of the amount of total monomeric anthocyanins, and the results were expressed as equivalents of cyanidin-3-glucoside (CG) per liter.
Phenolic compounds were determined, according to Terzieva et al. [25], with an HPLC system ELITE LaChrome (Hitachi, Japan) equipped with a diode array detector Elite LaChrome L-2455 and Supelco Discovery HS C18 column (5 μm × 25 cm × 4.6 mm).
Gas chromatography with flame ionization detector (GC–FID) and gas chromatography with mass selective detector (GC–MS) were employed for the determination of aromatized wine-type beverage composition. The important volatile low-molecular aldehydes and alcohols were investigated by GC–FID using a Shimadzu GC-17A (Shimadzu, Kyoto, Japan) gas chromatographer and software GC Solution version 2.3 (Shimadzu, Japan). The separation was performed on a TEKNOKROMA TRB-WAX column (30 m × 0.32 mm × 0.25 µm) injecting 1 µL from the sample. The injector temperature was set at 229 °C, and the detector temperature at 250 °C. The carrier gas was nitrogen at a pressure of 32 kPa and at flow of 1 mL/min. The starting temperature of the column was 40 °C, held for 1 min, then increased with an increment of 5 °C/min until 100 °C, held for 10 min, and finally increased with an increment of 15 °C/min until a temperature of 220 °C was reached.
The nonvolatile polar substances were determined by GC–MS as follows: To 200 µL lyophilized sample, 50 μL pyridine and 50 μL BSTFA were added. The sample was incubated at 70 °C for 40 min. For analysis, 1.0 μL from the solution was injected on a gas chromatograph Agilent GC 7890 (Agilent Technologies, Palo Alto, CA, USA) with mass-selective detector Agilent MD 5975 and column HP-5ms (30 m × 0.32 mm × 0.25 μm thicknesses). The following temperature regimen was used: initial temperature 100 °C (hold for 2 min) then increased to 180 °C with an increment of 15 °C/min (hold for 1 min) and increase of the temperature to 300 °C with an increment of 5 °C/min (hold for 10 min); injector and detector temperatures were 250 °C, helium was used as the carrier gas at a flow rate of 1.0 mL/min. The scanning range of the mass-selective detector was m/z = 50–550 in split-split mode (10:1). All mass spectra were acquired in electron impact ionization with 70 eV.
The aroma (volatile) substances were extracted from the AWTBs (1 mL) three times with 1 mL dichloromethane. The organic layers were dried (under vacuum) and the residue was dissolved with 100 µL CH2Cl2. A volume of 1 µL of the solution was used for the analyses, which were performed using Agilent GC 7890 with mass-selective detector Agilent MD 5975 and Agilent DB-5ms (30 m × 0.25 mm × 0.25 μm) column. The temperature regimen used was: the initial temperature was 40 °C and then increased to 300 °C with 5 °C/min (hold for 10 min); injector and detector temperatures were 250 °C, helium was used as the carrier gas at 1.0 mL/min. The scanning range of the mass-selective detector was m/z = 40–400 in splitless mode. All mass spectra were acquired in electron impact ionization with 70 eV.
The individual compounds were identified by comparing the retention times and the relative index (RI) with those of standard normal alkanes (C8–C40) injected under the same conditions, and mass spectral data from libraries of The Golm Metabolome Database (
Sensory evaluation was performed according to [26] ISO 13299:2016 with the following indicators: color, aroma intensity, aroma pureness, fruity notes, flowery notes, grassy notes, flavor intensity, beverage balance, acidity, bitterness, aftertaste, and overall score. Briefly, the bottles (14 ± 0.5 °C) were opened, the drink was poured in glasses and served unknown to 9 (27–50 years old) trained panelists from the Department of Wine and Beer Technology at the University of Food Technologies, Plovdiv, Bulgaria. The degree of liking was based on a 0–10 range (0: absence of the specified parameter, 10: extremely sensing the specified indicator). The organoleptic evaluation was performed in three repetitions, and the values of each indicator were averaged.
2.4. Statistical Analysis
The experiments were performed in triplicate and data values are expressed as mean ± SD (standard deviation). Statistical analysis was carried out by one-way ANOVA (Tukey’s post hoc test; p < 0.05) using Microsoft Excel 2013 with added XL Toolbox NG application.
3. Results and Discussion
3.1. Preparation and Characterization of Ethanol–Water Extracts of Rose Oil Industry Byproducts
The byproducts of the rose essential oil industry retain biologically active substances (polyphenols, aroma compounds, glycosides) because the industrial distillation process does not result in complete exhaustion of the valuable substances present in the initial fresh material. These compounds can be further extracted with organic or water/organic reagents, which leads to further valorization of the byproducts [16].
The results, presented in Table 1, suggested that 70% ethanol–water solutions extracted the highest amount of polyphenolic compounds, which approximated 6.5 g/L. Since the antioxidant activity is strongly related to the presence of polyphenols [27], the highest antioxidant capacities for this extract as measured by ORAC and HORAC were not unexpected.
The most important phenolic compounds in the extracts were investigated by liquid chromatography (Table 2).
The results of the analyses (Table 1 and Table 2) suggested that 70% and 30% ethanol solutions extract phenolic compounds to a greater extent, with the amount of naringenin, quercetin-3-β-glucoside (including quercetin), and catechin prevailing. Since the amounts of polyphenols present in the extracts are related to the quenching of free radicals, the 70% ethanolic extract exhibited the highest antioxidant activity determined by ORAC and HORAC assays [16].
The profile of polar volatile components in the three ethanol-water extracts was determined by GC–MS (Table 3). The highest amounts of aroma compounds in the extracts were observed for β-phenethyl alcohol (14.11 ± 0.16% of total ion current (TIC)), β-citronellol (10.18 ± 0.12% of TIC), nerol (6.15 ± 0.11% of TIC), geraniol (4.67 ± 0.12% of TIC), β-cubebene (5.95 ± 0.15% of TIC), β-caryophyllene (3.84 ± 0.10% of TIC), trans-nerolidol (7.37 ± 0.08% of TIC), and geranyl acetate (2.99 ± 0.11% of TIC). Β-Phenethyl alcohol, cis- and trans-rose oxide, β-citronellol, nerol, and geraniol are characteristic of a specific dry, green, and flowery rose-like aroma. Their presence in the byproducts and, subsequently in the extracts, could contribute to the final aroma bouquet of the aromatized beverages, and enhance customer satisfaction with the final product.
The higher alkanes present in the extracts, n-nonadecane (8.28 ± 0.12% TIC) and n-tricosane (4.50 ± 0.06% TIC), have a significant contribution as odor fixators leading to stabilization of the perception of other volatile compounds found in the byproducts.
3.2. Grape Must Fermentation
The relative density during fermentation of the grape must of the rosé wine (control) and the AWTB series ARW_CoF was monitored for 11 days (Figure 1).
The typical relative density of the freshly obtained grape must is in the 1.080–1.090 g/mL range. In the course of fermentation, the amount of sugars in the must decreases due to their conversion into ethanol, and as a consequence, the relative density of the mixture diminishes. At the end of the fermentation, the relative density of the rosé wines was between 0.996 and 0.998 g/mL. The must fermentation time for white and rosé wine production is usually 10–12 days [1]. In our experiments, during the first 3–4 days of fermentation, the relative density decrease was negligible, which could be explained by the adaptation of the yeasts. After the fourth day of inoculation, the fermentation rate increased, and the process practically ended on day 11, based on the values of the relative density achieved. The experimental data suggested that the added rose byproducts did not affect the yeast growth and subsequently, the dynamics of the fermentation.
3.3. Aromatized Wine-Type Beverages Characteristics
The simplest method for the production of AWTBs is a direct addition of individual aroma substances, extracts, or flavoring plant materials. Preliminary experiments with the direct addition of essential oils in wines revealed phase separation during storage due to a lower degree of miscibility. Cold maceration of plant materials in prepared wines led to the preparation of products with dominating grassy notes, which masked the pleasant rose aroma. Another possibility is the addition of plant material or byproducts during the grape must fermentation, which resembles the preparation of resinated wines [6]. By following this approach, two effects could be achieved, namely, an influence of the added plant material/byproduct on the fermentation course, and slow extraction of volatile (aroma) and nonvolatile substances during maceration due to the production of ethanol by the yeasts. Cofermentation of the plant material/byproduct with the grape must has both advantages and drawbacks. The advantages include no pretreatment of the plant material obtaining new aromas and/or enhancing flavors during cofermentation. The major drawbacks are related to standardization issues of the added material due to differences in the composition (by region, climate conditions, crop year, and so on), difficulties in the control during the fermentation process, possible hampering of the fermentation, or obtaining off-flavors during storage. The isolation of individual aroma compounds or obtaining extracts from byproducts of the essential oil industry due to the lower content of the aroma substances in industrially processed material is often complicated and, for this reason, a direct addition of the waste rose biomass into the fermenting grape must was chosen. The three approaches followed in the present work are similar to the main methods for the preparation of Vermouth [6].
For the preparation of the AWTBs using an extract-additive approach (series ARW_E), 70% ethanol extract was preferred after performing preliminary experiments. In addition, the results (Table 1, Table 2 and Table 3) of the analyses of extract composition showed that the 70% ethanol solution extracted polyphenolic and aromatic compounds from the rose byproducts to the maximum extent. The composition of the tested AWTBs from this series did not differ in most of the parameters determined from the samples from the other series (ARW_CoF) and (ARW_M) (Table 4). Significant differences were found in the alcohol content and antioxidant activity (Table 4). The alcohol content increased with the increase of the amount of 70% ethanolic extract added to the wine, and in sample ARW_E_100, and especially in ARW_E_200 and ARW_E_400, the values were above the typical values for wines (15% v/v). In the samples ARW_E_400, ARW_CoF_100, and ARW_M_100, the concentration of total polyphenols also increased, which was expected due to the highest added amounts of extract or solid byproducts. In sample ARW_CoF_100, the concentration of total polyphenols was 32% more than the control rosé wine, and 6% more than sample ARW_CoF_12.5. The highest amount of total monomeric anthocyanins was exhibited by the control rosé wine and the samples with the lowest amount of added ethanol-water extracts or solid rose byproduct, although the values did not differ significantly (Table 4). This reflects the red color spectrum due to flavilium cations of anthocyanins (CI, dA %). The highest amount was observed for the control rosé wine and the samples with the lowest amount of added ethanol-water extracts or solid rose byproduct. This might be due to the substantial degradation of anthocyanins by the steam water distillation of rose flowers, which is performed under high temperatures for two hours. No significant difference between the values for the acidity (titratable and volatile) was observed (Table 4).
The GC–FID analyses revealed that no significant increase in methanol content was observed, although in samples ARW_E_400, ARW_CoF_100, and ARW_M_100 the amount was slightly higher than the control wine (Table 5). The amounts determined were far below the permissible limits (250 mg/L for rosé type wines) [18]. The quantity of ethyl acetate determined in the control wine was 23.57 ± 1.62 mg/L and in the range from 23.15 ± 1.48 to 28.67 ± 2.01 mg/L for the aromatized wine-type samples. Ethyl acetate is among the esters dominantly present in wines, and is the main reason in certain cases for the changed sensory characteristics. In higher amounts of ethyl acetate (more than 100–150 mg/L), an acetone aroma is perceived [28], but concentrations below the threshold are favorable. In the range of 30 to 80 mg/L, the ethyl acetate increases the depth of the wine body, richness, and sweetness, and can contribute positively to the wine character and the pleasant wine bouquet [29]. The amounts of higher alcohols were slightly increased in the aromatized wines compared to the control rosé wine (Table 5). Higher alcohols (fusels) are an important factor in the overall enological characteristics of wines, and in concentrations lower than 300 mg/L have a beneficial effect on the aroma bouquet [30,31]. In higher concentrations, they negatively affect the proper and pleasant wine aroma. The AWTBs and the control rosé had total amounts of higher alcohols lower than 65 mg/L (Table 5). Therefore, the addition of extracts and solid rose byproducts (during grape must fermentation or by maceration in the prepared rosé) did not significantly alter the formation of higher alcohols. It should also be noted that the amounts of fusels, propanol, and butanol were below concentrations which can pose a danger to human health [31].
To achieve a better characterization of the AWTBs, the total component composition was also investigated (Table 6 and Table 7). Of the polar nonvolatile metabolites, the presence of low-molecular weight carbohydrates (glucose, fructose, galactose, and some disaccharides) was observed to the greatest extent (Table 6). However, no increase in their amounts was observed in all variants of the AWTBs compared to the control rosé wine. Of the amino acids, L-homoserine was found in the largest quantities.
The primary acids in grapes found in higher amounts were tartaric acid, malic acid, and, depending on the grapes but usually in small amounts, citric acid [32]. These acids were also found in the wines during the maceration, extraction, and fermentation. The highest amounts of tartaric acid were observed in the ARW_E_400, ARW_E_200, and ARW_CoF_50, although the values were closer to the control wine (Table 6). Syringic acid, also a characteristic compound of wines, was found in higher amounts, with a certain increase in its concentration observed in the variants obtained by all three methods used for AWTBs compared to the control. This may be due, to some extent, to the breakdown of malvidin in the course of obtaining the wine. Syringic acid and its naturally occurring derivatives have a beneficial effect on human health [33]. Ogut et al. [33] suggested potential therapeutic applications of syringic acid because of its antioxidant, anti-inflammatory, anticancer, antidiabetic, antiendotoxic, neuroprotective, cardioprotective, and hepatoprotective properties. In the course of fermentation, other acids, such as lactic, succinic, acetic, and so on, were formed, and their role in the final aroma of the wine may also be considered.
Overall, fifty-four volatile (aroma) compounds belonging to the alcohols, acids, aldehydes, hydrocarbons, and terpenes groups were determined (Table 7). Significant effects on the aroma substances formation/extraction in the AWTBs compared to the control were observed (Table 7) for β-citronellol, phenethyl alcohol, rose oxides, and geraniol. These substances were absent or present in the control wine in low amounts, and appeared in the AWTBs due to the addition of rose byproducts (solids or extracts). Phenethyl alcohol is among the compounds that contribute significantly to the favorable aroma of white and rosé wines [4,34]. Compared to the control rosé, the amount of phenethyl alcohol increased significantly from 1.07 ± 0.15 mg/L to 4.08 ± 0.30, 4.96 ± 0.24, and 5.77 ± 0.28 mg/L for the ARW_E_400, ARW_M_100, and ARW_CoF_100 (the samples with the highest amounts of added rose byproducts), respectively. The same trend was observed for the concentrations of β-caryophyllene, β-citronellol, rose oxides, and geraniol. They increased significantly, and a distinctive rose aroma in all the variants was sensed (Table 7; Figure 2). The amounts of higher alcohols increased in the AWTBs compared to control rosé wine, but this increase was insignificant and did not disrupt the overall balance and quality of the products. The amount of acetaldehyde increased significantly for ARW_E_400, ARW_M_100, and ARW_CoF_100 variants (the samples with the highest amounts of added rose byproducts), which confirmed the GC–FID analysis results. However, the amount of acetaldehyde is below the acceptable limits for acetaldehyde content [35]. The other aldehyde found in the AWTBs which significantly increased compared to the control was decanal. However, its amount in the ARW_CoF series was comparable to the control rosé (1.43 ± 0.11 mg/L). A slight increase in the concentration of decanal was observed in the ARW_CoF_400 samples only (Table 7). From the hydrocarbons (important aroma fixators), alkanes with more than 14 carbon atom chains predominated in the wines (control and aromatized) (Table 7).
3.4. Sensory Analyses
The creation of new food systems/products always needs to be finally tested by consumers, and their perception be taken into account. In the current study, all degustation analyses were carried out according to the main characteristics method with the participation of nine experienced tasters. The control rosé wine had a relatively clean, weak intensity, somewhat impersonal aroma, with fruity and partial mineral notes, weak floral, and very weak vegetal nuances. The control had a light-bodied aroma and quite fresh acidic nuances. It was balanced with a slightly sharp finish, the taste perception was for a weak, gentle, light rosé wine (Figure 2).
The tested AWTBs of the series differed in their organoleptic profile, with no defects or drastic deviations in the sensorium found anywhere (Figure 2). The influence of the addition of solid rose byproducts was expressed to varying degrees in terms of the colors, flowery nuances, harmony, and combination of the gentle taste with the rose-like and fruity wine aroma. Sample ARW_CoF_12.5 had a more intense, pure aroma, with well-developed delicate fruity and floral nuances, without harshness in the aroma bouquet. The taste was very harmonious, with playful acid notes, without bitterness, with a delicate taste aroma and a fresh aftertaste. In this sample, the fruity wine characteristics were very well-sensed with delicate floral nuances of roses.
Table 7Polar aroma (volatile) metabolites in the control wine and the AWTBs determined by GC–MS (mg/L).
| Compound | RIexp | RIcalc | Control | ARW_CoF | ARW_M | ARW_E | |||||||||
|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|
| 12.5 | 25 | 50 | 100 | 12.5 | 25 | 50 | 100 | 50 | 100 | 200 | 400 | ||||
| Organic acids | |||||||||||||||
| Butanoic acid | 785 | 770 | 0.43 ± 0.10 a | 0.45 ± 0.08 a | 0.42 ± 0.11 a | 0.44 ± 0.08 a | 0.41 ± 0.07 a | 0.47 ± 0.09 a | 0.44 ± 0.10 a | 0.46 ± 0.12 a | 0.43 ± 0.08 a | 0.48 ± 0.10 a | 0.45 ± 0.06 a | 0.48 ± 0.07 a | 0.44 ± 0.11 a |
| 2,3-Dihydroxy-butanedioic acid | 973 | 975 | 5.46 ± 0.23 a | 5.65 ± 0.30 a | 5.33 ± 0.25 a | 5.59 ± 0.19 a | 5.20 ± 0.21 a | 5.93 ± 0.30 a | 5.59 ± 0.24 a | 5.87 ± 0.23 a | 5.46 ± 0.25 a | 6.10 ± 0.09 a | 5.75 ± 0.27 a | 6.04 ± 0.16 a | 5.61 ± 0.21 a |
| Octanoic acid | 1192 | 1168 | 7.92 ± 0.32 a | 6.20 ± 0.25 b | 7.73 ± 0.31 a | 5.11 ± 0.19 c | 7.54 ± 0.22 a | 6.50 ± 0.24 b | 8.11 ± 0.30 a | 5.36 ± 0.26 c | 7.91 ± 0.19 a | 6.69 ± 0.21 a | 8.34 ± 0.24 a | 5.52 ± 0.31 c | 8.14 ± 0.26 a |
| Nonanoic acid | 1281 | 1269 | 6.55 ± 0.22 a | 6.77 ± 0.30 a | 6.39 ± 0.18 a | 6.70 ± 0.24 a | 6.23 ± 0.32 a | 7.11 ± 0.25 a | 6.71 ± 0.32 a | 7.04 ± 0.26 a | 6.54 ± 0.21 a | 7.31 ± 0.20 a | 6.90 ± 0.32 a | 7.24 ± 0.27 a | 6.73 ± 0.23 a |
| Decanoic acid | 1388 | 1367 | 5.61 ± 0.31 a | 5.80 ± 0.25 a | 5.47 ± 0.19 a | 5.74 ± 0.40 a | 5.33 ± 0.32 a | 6.09 ± 0.27 a | 5.74 ± 0.26 a | 6.03 ± 0.32 a | 5.60 ± 0.21 a | 6.26 ± 0.23 a | 5.91 ± 0.30 a | 6.20 ± 0.36 a | 5.76 ± 0.21 a |
| Dodecanoic acid | 1573 | 1566 | 2.00 ± 0.22 a | 2.27 ± 0.19 a | 2.50 ± 0.21 a | 2.15 ± 0.25 a | 2.69 ± 0.31 a | 2.38 ± 0.24 a | 2.62 ± 0.25 a | 2.25 ± 0.26 a | 2.82 ± 0.20 a | 2.45 ± 0.21 a | 2.69 ± 0.27 a | 2.32 ± 0.23 a | 2.91 ± 0.30 a |
| Tetradecanoic acid | 1774 | 1765 | 4.08 ± 0.26 a | 4.23 ± 0.31 a | 3.98 ± 0.27 a | 4.18 ± 0.30 a | 3.89 ± 0.32 a | 4.44 ± 0.44 | 4.18 ± 0.32 a | 4.39 ± 0.23 a | 4.08 ± 0.27 a | 4.56 ± 0.32 a | 4.30 ± 0.35 a | 4.51 ± 0.26 a | 4.20 ± 0.30 a |
| Aldehydes | |||||||||||||||
| Acetaldehyde | 400 | 402 | 16.32 ± 0.95 c | 18.24 ± 1.04 a,b | 19.58 ± 0.96 a,b | 20.04 ± 0.95 a | 20.15 ± 1.01 a | 17.05 ± 0.88 b,c | 17.39 ± 1.11 b,c | 18.84 ± 1.04 a,b | 19.28 ± 0.90 a | 17.78 ± 1.11 b,c | 18.98 ± 1.01 a,b | 19.64 ± 1.09 a,b | 20.63 ± 0.89 a |
| Hexanal | 800 | 801 | 2.31 ± 0.21 a | 2.39 ± 0.1 a | 2.25 ± 0.30 a | 2.37 ± 0.22 a | 2.20 ± 0.23 a | 2.51 ± 0.19 a | 2.37 ± 0.24 a | 2.48 ± 0.30 a | 2.31 ± 0.22 a | 2.58 ± 0.27 a | 2.44 ± 0.32 a | 2.56 ± 0.19 a | 2.38 ± 0.25 a |
| Octanal | 997 | 998 | 0.43 ± 0.11 a | 0.37 ± 0.10 a | 0.40 ± 0.08 a | 0.41 ± 0.07 a | 0.41 ± 0.12 a | 0.43 ± 0.14 a | 0.37 ± 0.10 a | 0.40 ± 0.12 a | 0.41 ± 0.13 a | 0.45 ± 0.11 a | 0.38 ± 0.10 a | 0.34 ± 0.09 a | 0.37 ± 0.08 a |
| Decanal | 1205 | 1201 | 1.43 ± 0.11 a | 1.37 ± 0.15 a | 1.40 ± 0.20 a | 1.41 ± 0.13 a | 1.87 ± 0.21 b | 3.27 ± 0.20 c | 3.09 ± 0.21 c | 3.24 ± 0.14 c | 3.01 ± 0.23 c | 3.37 ± 0.21 c | 3.18 ± 0.18 c | 3.33 ± 0.20 c | 3.10 ± 0.14 c |
| Alcohols | |||||||||||||||
| Propan-1-ol | 599 | 577 | 0.48 ± 0.10 a | 0.50 ± 0.08 a | 0.47 ± 0.07 a | 0.50 ± 0.11 a | 0.46 ± 0.09 a | 0.53 ± 0.08 a | 0.50 ± 0.11 a | 0.52 ± 0.14 a | 0.48 ± 0.11 a | 0.54 ± 0.09 a | 0.51 ± 0.07 a | 0.53 ± 0.11 a | 0.47 ± 0.10 a |
| Butan-1-ol | 660 | 664 | 0.40 ± 0.08 a | 0.41 ± 0.10 a | 0.39 ± 0.06 a | 0.41 ± 0.07 a | 0.38 ± 0.11 a | 0.44 ± 0.09 a | 0.41 ± 0.10 a | 0.43 ± 0.08 a | 0.40 ± 0.06 a | 0.45 ± 0.11 a | 0.42 ± 0.07 a | 0.44 ± 0.09 a | 0.42 ± 0.06 a |
| Pentan-1-ol | 768 | 762 | 0.52 ± 0.11 a | 0.54 ± 0.09 a | 0.51 ± 0.10 a | 0.54 ± 0.12 a | 0.50 ± 0.08 a | 0.57 ± 0.11 a | 0.54 ± 0.14 a | 0.56 ± 0.12 a | 0.52 ± 0.10 a | 0.59 ± 0.11 a | 0.55 ± 0.07 a | 0.58 ± 0.11 a | 0.55 ± 0.10 a |
| Hexan-1-ol | 867 | 863 | 2.41 ± 0.21 a | 2.50 ± 0.19 a | 2.35 ± 0.24 a | 2.47 ± 0.28 a | 2.30 ± 0.17 a | 2.62 ± 0.22 a | 2.47 ± 0.19 a | 2.59 ± 0.20 a | 2.41 ± 0.23 a | 2.70 ± 0.30 a | 2.54 ± 0.17 a | 2.67 ± 0.18 a | 2.35 ± 0.25 a |
| Heptan-1-ol | 952 | 959 | 0.65 ± 0.10 a | 0.67 ± 0.09 a | 0.63 ± 0.11 a | 0.66 ± 0.08 a | 0.62 ± 0.10 a | 0.70 ± 0.14 a | 0.66 ± 0.12 a | 0.70 ± 0.10 a | 0.65 ± 0.09 a | 0.72 ± 0.11 a | 0.68 ± 0.12 a | 0.72 ± 0.09 a | 0.64 ± 0.16 a |
| Octan-1-ol | 1073 | 1063 | 0.80 ± 0.20 a | 0.83 ± 0.18 a | 0.78 ± 0.21 a | 0.82 ± 0.17 a | 0.76 ± 0.22 a | 0.87 ± 0.13 a | 0.82 ± 0.15 a | 0.86 ± 0.19 a | 0.80 ± 0.20 a | 0.90 ± 0.17 a | 0.84 ± 0.16 a | 0.89 ± 0.18 a | 0.80 ± 0.19 a |
| Nonan-1-ol | 1170 | 1165 | 2.12 ± 0.22 a | 2.19 ± 0.18 a | 2.07 ± 0.30 a | 2.17 ± 0.19 a | 2.02 ± 0.22 a | 2.30 ± 0.17 a | 2.17 ± 0.20 a | 2.28 ± 0.24 a | 2.12 ± 0.19 a | 2.37 ± 0.24 a | 2.23 ± 0.22 a | 2.34 ± 0.18 a | 2.02 ± 0.19 a |
| Decan-1-ol | 1272 | 1267 | 0.34 ± 0.06 a | 0.35 ± 0.07 a | 0.33 ± 0.10 a | 0.35 ± 0.05 a | 0.32 ± 0.07 a | 0.37 ± 0.06 a | 0.35 ± 0.09 a | 0.36 ± 0.08 a | 0.34 ± 0.11 a | 0.38 ± 0.07 a | 0.36 ± 0.10 a | 0.37 ± 0.06 a | 0.31 ± 0.08 a |
| Hydrocarbons | |||||||||||||||
| n-Octane | 796 | 800 | 0.45 ± 0.07 a | 0.43 ± 0.06 a | 0.45 ± 0.08 a | 0.42 ± 0.05 a | 0.47 ± 0.04 a | 0.45 ± 0.08 a | 0.43 ± 0.09 a | 0.45 ± 0.07 a | 0.42 ± 0.06 a | 0.47 ± 0.08 a | 0.44 ± 0.10 a | 0.46 ± 0.07 a | 0.41 ± 0.08 a |
| n-Decane | 999 | 1000 | 0.38 ± 0.04 a | 0.35 ± 0.06 a | 0.37 ± 0.05 a | 0.35 ± 0.07 a | 0.39 ± 0.08 a | 0.38 ± 0.06 a | 0.35 ± 0.08 a | 0.37 ± 0.04 a | 0.35 ± 0.08 a | 0.39 ± 0.04 a | 0.36 ± 0.08 a | 0.38 ± 0.07 a | 0.36 ± 0.05 a |
| n-Dodecane | 1201 | 1200 | 0.49 ± 0.07 a | 0.46 ± 0.03 a | 0.49 ± 0.06 a | 0.45 ± 0.01 a | 0.51 ± 0.04 a | 0.49 ± 0.07 a | 0.46 ± 0.08 a | 0.49 ± 0.05 a | 0.45 ± 0.10 a | 0.51 ± 0.06 a | 0.48 ± 0.07 a | 0.50 ± 0.05 a | 0.48 ± 0.06 a |
| n-Tetradecane | 1400 | 1400 | 2.27 ± 0.31 a | 2.14 ± 0.29 a | 2.24 ± 0.17 a | 2.08 ± 0.25 a | 2.33 ± 0.19 a | 2.27 ± 0.20 a | 2.14 ± 0.24 a | 2.24 ± 0.27 a | 2.08 ± 0.19 a | 2.33 ± 0.22 a | 2.20 ± 0.26 a | 2.30 ± 0.18 a | 2.03 ± 0.24 a |
| n-Hexadecane | 1600 | 1600 | 2.59 ± 0.21 a | 2.68 ± 0.19 a | 2.53 ± 0.31 a | 2.65 ± 0.17 a | 2.46 ± 0.25 a | 2.81 ± 0.24 a | 2.65 ± 0.27 a | 2.78 ± 0.18 a | 2.59 ± 0.30 a | 2.89 ± 0.24 a | 2.73 ± 0.23 a | 2.86 ± 0.27 a | 2.66 ± 0.29 a |
| n-Octadecane | 1800 | 1800 | 3.79 ± 0.31 a | 3.92 ± 0.19 a | 3.70 ± 0.26 a | 3.88 ± 0.41 a | 4.26 ± 0.27 a | 4.12 ± 0.22 a | 3.88 ± 0.34 a | 4.07 ± 0.18 a | 4.47 ± 0.26 a | 4.24 ± 0.32 a | 3.99 ± 0.28 a | 4.19 ± 0.23 a | 4.60 ± 0.33 a |
| n-Nonadecane | 1900 | 1900 | 4.50 ± 0.46 a | 4.66 ± 0.29 a | 4.39 ± 0.25 a | 4.61 ± 0.27 a | 5.03 ± 0.36 a | 4.89 ± 0.42 a | 4.61 ± 0.28 a | 4.84 ± 0.26 a | 5.28 ± 0.33 a | 5.03 ± 0.29 a | 4.74 ± 0.27 a | 4.97 ± 0.34 a | 5.43 ± 0.19 a |
| n-Eicosane | 2000 | 2000 | 3.61 ± 0.18 a | 3.73 ± 0.22 a | 3.52 ± 0.27 a | 3.69 ± 0.35 a | 3.93 ± 0.26 a | 3.92 ± 0.34 a | 3.69 ± 0.27 a | 3.88 ± 0.25 a | 4.13 ± 0.22 a | 4.03 ± 0.36 a | 3.80 ± 0.44 a | 3.99 ± 0.29 a | 4.25 ± 0.41 a |
| n-Heneicosane | 2100 | 2100 | 2.71 ± 0.15 a | 2.81 ± 0.24 a | 2.65 ± 0.30 a | 2.78 ± 0.22 a | 2.58 ± 0.27 a | 2.95 ± 0.31 a | 2.78 ± 0.26 a | 2.91 ± 0.23 a | 2.71 ± 0.28 a | 3.03 ± 0.34 a | 2.86 ± 0.27 a | 3.00 ± 0.33 a | 2.79 ± 0.26 a |
| n-Docosane | 2200 | 2200 | 2.84 ± 0.16 a | 2.93 ± 0.22 a | 2.77 ± 0.34 a | 2.90 ± 0.23 a | 2.70 ± 0.26 a | 3.08 ± 0.31 a | 2.90 ± 0.19 a | 3.05 ± 0.27 a | 2.83 ± 0.35 a | 3.17 ± 0.22 a | 2.99 ± 0.18 a | 3.13 ± 0.31 a | 2.91 ± 0.24 a |
| Terpenes | |||||||||||||||
| Terpinolene | 1087 | 1086 | 0.76 ± 0.10 a | 0.78 ± 0.11 a | 0.74 ± 0.09 a | 0.77 ± 0.21 a | 0.72 ± 0.14 a | 0.82 ± 0.08 a | 0.78 ± 0.11 a | 0.81 ± 0.15 a | 0.76 ± 0.12 a | 0.85 ± 0.09 a | 0.80 ± 0.21 a | 0.84 ± 0.12 a | 0.78 ± 0.16 a |
| β-Linalool | 1097 | 1095 | 1.17 ± 0.21 b | 1.52 ± 0.15 a | 1.43 ± 0.15 a | 1.50 ± 0.20 a | 1.40 ± 0.17 a | 1.59 ± 0.18 a | 1.50 ± 0.12 a | 1.58 ± 0.20 a | 1.47 ± 0.16 a | 1.64 ± 0.14 a | 1.55 ± 0.17 a | 1.62 ± 0.16 a | 1.51 ± 0.13 a |
| Phenethyl alcohol | 1110 | 1106 | 1.07 ± 0.15 e | 3.10 ± 0.22 d | 3.87 ± 0.31 c | 4.06 ± 0.40 c | 5.77 ± 0.28 a | 3.31 ± 0.25 c,d | 3.56 ± 0.31 c,d | 4.01 ± 0.26 c | 4.96 ± 0.24 b | 3.43 ± 0.32 c,d | 3.18 ± 0.27 d | 3.58 ± 0.23 c,d | 4.08 ± 0.30 c |
| cis-Rose oxide | 1112 | 1107 | 0.09 ± 0.04 d | 0.20 ± 0.12 c,d | 0.37 ± 0.10 b | 0.57 ± 0.08 a | 0.71 ± 0.09 a | 0.23 ± 0.12 c,d | 0.40 ± 0.07 b | 0.49 ± 0.11 a,b | 0.64 ± 0.08 a | 0.21 ± 0.10 c,d | 0.39 ± 0.06 b | 0.51 ± 0.08 a,b | 0.69 ± 0.11 a |
| trans-Rose oxide | 1127 | 1122 | 0.05 ± 0.01 c | 0.19 ± 0.01 b | 0.23 ± 0.01 b | 0.28 ± 0.02 a | 0.36 ± 0.04 a | 0.17 ± 0.02 a | 0.25 ± 0.03 a | 0.30 ± 0.01 a | 0.35 ± 0.02 a | 0.17 ± 0.04 b | 0.29 ± 0.01 a | 0.31 ± 0.02 a | 0.33 ± 0.01 a |
| β-Citronellol | 1228 | 1223 | 0.31 ± 0.04 e | 0.95 ± 0.08 d | 1.31 ± 0.11 b,c | 1.56 ± 0.08 b | 1.94 ± 0.12 a | 1.01 ± 0.21 c,d | 1.47 ± 0.15 b,c | 1.64 ± 0.12 a,b | 1.83 ± 0.14 a | 0.86 ± 0.16 d | 1.21 ± 0.17 c | 1.49 ± 0.20 b,c | 1.70 ± 0.12 a |
| Nerol | 1230 | 1227 | 0.35 ± 0.05 a | 0.36 ± 0.06 a | 0.34 ± 0.02 a | 0.35 ± 0.07 a | 0.33 ± 0.10 a | 0.38 ± 0.06 a | 0.35 ± 0.08 a | 0.37 ± 0.02 a | 0.35 ± 0.04 a | 0.39 ± 0.08 a | 0.36 ± 0.06 a | 0.38 ± 0.07 a | 0.36 ± 0.05 a |
| Geraniol | 1255 | 1249 | 0.13 ± 0.01 d | 0.65 ± 0.11 c | 0.72 ± 0.04 b,c | 0.81 ± 0.03 a,b | 0.95 ± 0.05 a | 0.68 ± 0.02 c | 0.73 ± 0.04 b,c | 0.88 ± 0.06 a | 0.99 ± 0.03 a | 0.58 ± 0.02 c | 0.66 ± 0.05 c | 0.80 ± 0.07 a,b | 0.94 ± 0.05 a |
| Citronellyl acetate | 1354 | 1350 | 0.51 ± 0.01 b | 0.79 ± 0.04 a | 0.75 ± 0.04 a | 0.78 ± 0.07 a | 0.73 ± 0.03 a | 0.83 ± 0.08 a | 0.78 ± 0.06 a | 0.82 ± 0.04 a | 0.76 ± 0.03 a | 0.85 ± 0.02 a | 0.81 ± 0.07 a | 0.84 ± 0.06 a | 0.79 ± 0.04 a |
| Eugenol | 1356 | 1356 | 0.22 ± 0.01 a | 0.22 ± 0.01 a | 0.21 ± 0.01 a | 0.22 ± 0.02 a | 0.20 ± 0.02 a | 0.23 ± 0.01 a | 0.22 ± 0.01 a | 0.23 ± 0.01 a | 0.21 ± 0.02 a | 0.24 ± 0.01 a | 0.23 ± 0.01 a | 0.24 ± 0.01 a | 0.22 ± 0.01 a |
| Neryl acetate | 1364 | 1359 | 2.33 ± 0.21 a | 2.42 ± 0.14 a | 2.28 ± 0.20 a | 2.39 ± 0.15 a | 2.52 ± 0.17 a | 2.54 ± 0.12 a | 2.39 ± 0.18 a | 2.51 ± 0.30 a | 2.53 ± 0.21 a | 2.61 ± 0.20 a | 2.46 ± 0.22 a | 2.58 ± 0.17 a | 2.60 ± 0.18 a |
| Geranyl acetate | 1383 | 1379 | 1.63 ± 0.20 a | 1.69 ± 0.15 a | 1.59 ± 0.18 a | 1.67 ± 0.20 a | 1.55 ± 0.16 a | 1.77 ± 0.21 a | 1.67 ± 0.12 a | 1.75 ± 0.17 a | 1.63 ± 0.22 a | 1.82 ± 0.21 a | 1.72 ± 0.16 a | 1.80 ± 0.20 a | 1.67 ± 0.24 a |
| β-Bourbonene | 1383 | 1387 | 3.53 ± 0.22 a | 3.66 ± 0.18 a | 3.45 ± 0.30 a | 3.62 ± 0.26 a | 3.36 ± 0.33 a | 3.84 ± 0.17 a | 3.62 ± 0.22 a | 3.80 ± 0.23 a | 3.53 ± 0.32 a | 3.95 ± 0.30 a | 3.72 ± 0.24 a | 3.91 ± 0.27 a | 3.63 ± 0.22 a |
| β-Cubebene | 1389 | 1388 | 0.43 ± 0.05 a | 0.44 ± 0.07 a | 0.41 ± 0.05 a | 0.44 ± 0.06 a | 0.40 ± 0.02 a | 0.46 ± 0.04 a | 0.44 ± 0.06 a | 0.46 ± 0.07 a | 0.42 ± 0.05 a | 0.48 ± 0.03 a | 0.45 ± 0.02 a | 0.47 ± 0.06 a | 0.44 ± 0.04 a |
| β-Elemene | 1390 | 1389 | 0.57 ± 0.06 a | 0.59 ± 0.08 a | 0.55 ± 0.05 a | 0.58 ± 0.04 a | 0.54 ± 0.02 a | 0.62 ± 0.06 a | 0.58 ± 0.04 a | 0.61 ± 0.03 a | 0.57 ± 0.05 a | 0.63 ± 0.05 a | 0.60 ± 0.04 a | 0.63 ± 0.06 a | 0.58 ± 0.03 a |
| β-Caryophyllene | 1419 | 1417 | 1.85 ± 0.28 b | 3.82 ± 0.23 a | 3.96 ± 0.27 a | 4.15 ± 0.32 a | 3.86 ± 0.31 a | 4.01 ± 0.33 a | 4.15 ± 0.28 a | 4.36 ± 0.33 a | 4.05 ± 0.25 a | 4.13 ± 0.31 a | 4.27 ± 0.29 a | 4.48 ± 0.32 a | 4.17 ± 0.27 a |
| α-Caryophyllene | 1454 | 1452 | 0.38 ± 0.01 a | 0.39 ± 0.01 a | 0.37 ± 0.02 a | 0.39 ± 0.03 a | 0.36 ± 0.01 a | 0.41 ± 0.02 a | 0.39 ± 0.04 a | 0.41 ± 0.02 a | 0.38 ± 0.03 a | 0.42 ± 0.02 a | 0.40 ± 0.04 a | 0.42 ± 0.03 a | 0.39 ± 0.02 a |
| Germacrene D | 1479 | 1484 | 0.44 ± 0.02 a | 0.46 ± 0.01 a | 0.43 ± 0.04 a | 0.45 ± 0.02 a | 0.42 ± 0.03 a | 0.48 ± 0.02 a | 0.45 ± 0.01 a | 0.47 ± 0.02 a | 0.44 ± 0.03 a | 0.49 ± 0.02 a | 0.46 ± 0.04 a | 0.49 ± 0.02 a | 0.45 ± 0.03 a |
| α-Farnesene | 1508 | 1505 | 0.63 ± 0.02 a | 0.65 ± 0.05 a | 0.61 ± 0.04 a | 0.64 ± 0.02 a | 0.60 ± 0.07 a | 0.68 ± 0.06 a | 0.64 ± 0.04 a | 0.68 ± 0.02 a | 0.63 ± 0.03 a | 0.70 ± 0.05 a | 0.66 ± 0.02 a | 0.70 ± 0.02 a | 0.65 ± 0.05 a |
| β-Bisabolene | 1510 | 1506 | 0.20 ± 0.01 a | 0.21 ± 0.01 a | 0.20 ± 0.01 a | 0.21 ± 0.01 a | 0.19 ± 0.01 a | 0.22 ± 0.02 a | 0.21 ± 0.01 a | 0.22 ± 0.02 a | 0.20 ± 0.01 a | 0.23 ± 0.01 a | 0.22 ± 0.2 a | 0.23 ± 0.02 a | 0.21 ± 0.01 a |
| trans-Nerolidol | 1564 | 1561 | 1.53 ± 0.22 a | 1.58 ± 0.14 a | 1.49 ± 0.20 a | 1.57 ± 0.16 a | 1.46 ± 0.17 a | 1.66 ± 0.22 a | 1.57 ± 0.21 a | 1.65 ± 0.20 a | 1.53 ± 0.15 a | 1.71 ± 0.24 a | 1.61 ± 0.18 a | 1.69 ± 0.21 a | 1.57 ± 0.19 a |
| Spathulenol | 1575 | 1577 | 1.83 ± 0.16 a | 1.89 ± 0.21 a | 1.78 ± 0.18 a | 1.87 ± 0.21 a | 1.74 ± 0.24 a | 1.98 ± 0.22 a | 1.87 ± 0.22 a | 1.96 ± 0.24 a | 1.82 ± 0.18 a | 2.04 ± 0.30 a | 1.92 ± 0.25 a | 2.02 ± 0.22 a | 1.88 ± 0.17 a |
| Caryophyllene oxide | 1580 | 1582 | 0.36 ± 0.02 a | 0.37 ± 0.01 a | 0.35 ± 0.01 a | 0.37 ± 0.2 a | 0.34 ± 0.02 a | 0.39 ± 0.01 a | 0.37 ± 0.01 a | 0.39 ± 0.03 a | 0.36 ± 0.02 a | 0.40 ± 0.01 a | 0.38 ± 0.02 a | 0.40 ± 0.01 a | 0.37 ± 0.03 a |
| γ-Eudesmol | 1631 | 1630 | 0.33 ± 0.01 a | 0.34 ± 0.01 a | 0.32 ± 0.01 a | 0.34 ± 0.01 a | 0.31 ± 0.01 a | 0.36 ± 0.02 a | 0.34 ± 0.01 a | 0.36 ± 0.01 a | 0.33 ± 0.02 a | 0.37 ± 0.01 a | 0.35 ± 0.01 a | 0.37 ± 0.01 a | 0.34 ± 0.01 a |
| β-Eudesmol | 1649 | 1649 | 0.28 ± 0.01 a | 0.29 ± 0.01 a | 0.28 ± 0.01 a | 0.29 ± 0.01 a | 0.27 ± 0.01 a | 0.31 ± 0.01 a | 0.29 ± 0.01 a | 0.30 ± 0.01 a | 0.28 ± 0.01 a | 0.32 ± 0.01 a | 0.30 ± 0.01 a | 0.31 ± 0.01 a | 0.29 ± 0.01 a |
| α-Eudesmol | 1651 | 1652 | 0.99 ± 0.05 a | 1.03 ± 0.02 a | 0.97 ± 0.07 a | 1.01 ± 0.06 a | 0.94 ± 0.08 | 1.08 ± 0.10 a | 1.02 ± 0.05 a | 1.07 ± 0.06 a | 0.99 ± 0.07 a | 1.11 ± 0.06 a | 1.04 ± 0.08 a | 1.10 ± 0.03 a | 1.02 ± 0.08 a |
RIexp—Experimentally determined retention index (Kovats retention index); RIcalc—calculated retention index; a–e The experiments were performed in triplicate and given as mean ± SD. Values with different superscript letters in a row are significantly different (p < 0.05).
The sample ARW_CoF_25 had a relatively intense aroma, clean, with tangible notes of rose, the fruity nuances still dominated, but the harmony with the florals was not positive, the taste of the wine slightly sharpens, the acids were more irritating and somehow dry, bitterness appears and the aftertaste was sharper.
In the aromatized wine-type beverage ARW_CoF_50, the harmony between wine and floral notes was very well expressed. The aroma was strong and clean, with a pronounced dominance of elegant floral nuances. The fruitiness was weakly expressed, but it blended well into the general flavor perception. The taste of the sample was balanced, the acids were softened and embedded in the body with a soft and elegant finish. The flavor was strongly floral with scents of rose, but fine, clean, and light.
The sample with the highest amount of added solid rose byproducts ARW_CoF_100 (25 g per litter) had the strongest expression of floral nuances, but lost a lot of harmony in the aroma and somewhat in the taste. The notes were strong, but coarse, together with the pronounced, intrusive notes of rose, “green” grassy nuances were sensed, the taste of the sample was dense, with a weaker feeling of acidity, quite soft, but the notes of raw, green, grassy mass intruded in the aroma. Here, the addition of rose byproducts negatively influenced the overall appearance and perception of the aromatized wine-type beverage, despite the distinguished floral expression.
The general impression of the ARW_M series (Figure 2) was that in postfermentative maceration of the rose byproducts in the preliminarily prepared rosé wine, the influence of the rose byproducts was coarser than in cofermentative maceration during alcoholic fermentation of the grape must (series ARW_CoF). The tested beverages of the series differed in their organoleptic profile, and in samples ARW_M_50 and ARW_M_100, a strong negative influence of the added solid rose byproducts was perceived. The harmony in the first two samples of the series was better expressed, while in the second, the wine notes were interwoven in the most balanced way with distinct floral nuances. The ARW_M_12.5 sample had a more intense, clean aroma, with well-woven delicate fruit and floral nuances, without harshness in the aroma. The taste was very harmonious, with a playful juicy acidic sense, without bitterness, with a delicate taste aroma and a fresh aftertaste. In this sample, the fruity wine characteristics are very well combined with the delicate floral rose aroma. Sample ARW_M_25 has the same character as ARW_M_12.5, but the floral nuances are more pronounced and dominating without compromising the complex character of the wine drink. In sample ARW_M_50, and especially in ARW_M_100, the harmony between the wine notes and florals is strongly disturbed, along with the floral rose notes, rough green-grassy vegetal nuances appear, notes of stork’s-bills (Pelargonium roseum), geranium (Geranium macrorrhizum), and sweet-scented geranium (Pelargonium graveolens). They are particularly noticeable in the aftertaste aroma, changing the character of the drinks and making them intrusive and inharmonious. An irritating acidic taste appeared as the bitterness increased and became more persistent.
The sensory profile of the AWTBs of the series ARW_E suggested that their flavor is the most disharmonious of the three series of products. There were problems with the clarity of the samples, which was most probably due to insoluble essential oils. Slight grayish nuances in the color of the wines were observed, which were especially noticeable in samples ARW_E_200 and ARW_E_400. In the beverage’s aroma, atypical fruit and boiled fruits were felt. With the increase of ethanol-water extract amounts added, the aroma became sharper, fiery, and alcoholic. The flavor of the first two samples was soft, and the acidic taste was melted, but the feeling of mild heat turned into flames in the last samples of the series. The aroma was sharply alcoholic, and the grassy and green notes were strongly felt in ARW_E_200 and ARW_E_400. They could be associated with drinks having added ethanol. Of this series, ARW_E_50 was the most preferred sample. Despite the strong influence of the floral notes and high ethanol, the drink was harmonious, with well-balanced wine and floral notes. There was no coarsening of the aroma and the appearance of green plant intrusive nuances.
Among all AWTBs, ARW_CoF_12.5 and ARW_CoF_50 were the most preferred samples, with the first sample tasting score being one unit higher, mostly due to the better harmony between the wine notes and the floral nuances (Table 8). ARW_CoF_100 was evaluated with the lowest score because the influence of the rose byproducts was strong and emphasized, but the harmony in the drink was greatly disturbed by the appearance of unpleasant green-grassy nuances in the aroma.
From the ARW_M series, samples ARW_M_25 and ARW_M_12.5 were the most appreciated by tasters, with the tasting score of sample ARW_M_25 being one unit higher than that of ARW_M_12.5, mainly due to the better harmony between the wine notes and the floral nuances. Sample ARW_M_100 was the least rated, the reason being the strong intrusive influence of the rose byproducts. The harmony in the drink was greatly disturbed, and there was an appearance of unpleasant green vegetal nuances in the nose and aftertaste in the mouth.
The AWTBs from the series ARW_E were the least preferred by the panelists. The best-rated and ranked first in preference from this series was sample ARW_E_100 (Table 8). Tasting rating scores were lower, the sense of harmony between the drink character and the floral grassy nuances was weak, and the influence of added ethanol from the extracts was strong and rather negative. Still in this series, the grassy, green nuances could be considered as the main problem. The results imply that the addition of ethanol-water extracts of rose byproducts in the range of 10 to 20 mL/L could potentially prevent unpleasant customer perception.
According to Noble et al. [36], the AWTBs from the ARW_CoF series could be classified as beverages with a floral aroma (rose), except the sample ARW_CoF_100, where some “green” nuances were sensed. The latter could be classified in the type of beverages of vegetative, green class. The samples ARW_M_50 and ARW_M_100 from series ARW_M had a strong negative influence from the added solid rose byproducts, and they belonged to the classes ‘vegetative’ and ‘chemical’. The other two samples, ARW_M_12.5 and ARW_M_25 (with the lower added solid rose byproducts), were distinctive, with a more balanced aroma, and could be classified as a ‘floral’ type of beverage. The variants from the ARW_E series lack a lot of harmony (except for sample ARW_E_50) and belonged to the ‘vegetative’ and ‘chemical’ classes, with a coarse and, to some extent, pungent taste and aftertaste.
4. Conclusions
Three approaches for the preparation of AWTBs using rose oil industry byproducts were investigated, namely, cofermentation of the solid byproducts with the grape must (ARW_CoF series), maceration of the solid byproducts in preliminarily prepared rosé wine (ARW_M series), and addition of ethanol-water extracts of solid rose byproducts to preliminarily prepared rosé wine (ARW_E series). The dynamics of the relative density during fermentation of the grape must (11 days) of the control rosé wine and the ARW_CoF were similar, which suggested that the addition of the rose byproducts did not hamper the growth of the yeasts. The amount of ethanol in the products did not differ significantly, except for ARW_E_200 and ARW_E_400 (ARW_E series), where the concentration of this compound was higher than 15% (v/v). The addition of solid rose byproducts/extracts during fermentation or in the preliminarily prepared rosé wine did not negatively affect the formation of higher alcohols. The polyphenol content increased significantly from 230.00 ± 5.21 (control) to 296.13 ± 3.57 (ARW_M_100), 295.50 ± 3.78 (ARW_CoF_100), and 293.73 ± 4.29 (ARW_E_400) µmol GAE/L, rendering the AWTBs with a higher antioxidant activity. The highest amounts of tartaric acid were observed in ARW_E400 (220.91 ± 3.10 mg/L), ARW_E200 (218.21 ± 2.53 mg/L), and ARW_CoF50 (218.65 ± 2.32 mg/L). In all variants, obtained by all three methods used for AWTB preparation, the syringic acid, also a characteristic compound of wines, was found in the range from 60.53 ± 0.72 to 81.17 ± 0.65 mg/L. The most positive sensory analyses evaluated the AWTBs from the ARW_CoF series, with the ARW_CoF_50 and ARW_CoF_12.5 variants scoring the highest results. The experimental data and sensory analyses suggested that the solid rose oil byproducts added to the grape must during its fermentation did not negatively influence the fermentation process. The results of the present study indicated that rose oil industry byproducts could be successfully valorized for the preparation of AWTBs, and contribute to the augmentation of the total polyphenol content, antioxidant capacity, and new aroma profile of the final products.
Conceptualization, A.S. and H.S.; methodology, A.S., P.D. and H.S.; validation, R.D., A.S., and V.C.; formal analysis, A.S. and P.D.; investigation, A.S., M.G.T., R.D., P.D. and I.D.; resources, H.S. and A.S.; data curation, A.S., H.S., V.C. and I.D.; writing—original draft preparation, A.S.; writing—review and editing, H.S., V.C., and A.S.; visualization, H.S., R.D., A.S. and P.D.; supervision, A.S.; project administration, H.S. and A.S.; funding acquisition, H.S., A.S. and V.C. All authors have read and agreed to the published version of the manuscript.
Not applicable.
Not applicable.
Data are available on request.
The authors would like to thank Vasil Georgiev, (Laboratory for Cell Biosystems—Plovdiv, Bulgaria, The Stephan Angelov Institute of Microbiology—Bulgarian Academy of Sciences) for the HPLC analyses.
The authors declare no conflict of interest.
Footnotes
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Enlarge this image.Figure 1. Dynamics of the relative density during fermentation of the grape must of the control rosé wine and the AWTB series ARW_CoF.
Polyphenol content and antioxidant activity of ethanol-water ethanol–water extracts of rose oil industry byproducts.
| Extract | Polyphenol Content, mg/L | Antioxidant Activity | |
|---|---|---|---|
| ORAC, µmol TE/L | HORAC, µmol GAE/L | ||
| 30% | 6029.0 ± 150.5 b | 97,845.6 ± 1058.6 b | 45,522.5 ± 863.4 b |
| 70% | 6506.1 ± 137.9 a | 108,674.9 ± 968.3 a | 63,219.3 ± 915.4 a |
| 90% | 3740.6 ± 148.3 c | 66,010.2 ± 1058.8 c | 40,448.8 ± 886.2 c |
a–c The experiments were performed in triplicate and given as mean ± SD. Values in a column with different superscripts differ significantly (p < 0.05). ORAC—oxygen radical absorbance capacity assay; HORAC—hydroxyl radical averting capacity assay; TE—Trolox equivalent; GAE: gallic acid equivalent.
Individual phenolic compounds in the ethanol-water extracts of rose oil industry byproducts.
| Compound | 30% Extract, |
70% Extract, |
90% Extract, |
|---|---|---|---|
| Neochlorogenic acid | 148.86 ± 2.38 a | 137.19 ± 3.24 b | 87.22 ± 1.99 c |
| Caffeic acid | 39.37 ± 1.24 a | 37.17 ± 1.16 a | nd * |
| p-Coumaric acid | 132.03 ± 3.57 a | 131.78 ± 2.68 a | 28.42 ± 2.89 b |
| Ellagic acid | 92.03 ± 3.15 b | 130.84 ± 3.08 a | 23.98 ± 2.84 c |
| Quercetin | 168.32 ± 2.67 b | 196.54 ± 3.04 a | 129.91 ± 2.54 c |
| Quercetin-3-β-glucoside | 721.25 ± 3.68 b | 888.04 ± 3.84 a | 629.64 ± 3.79 c |
| Myricetin | 281.99 ± 2.18 b | 333.63 ± 2.68 a | 151.77 ± 1.95 c |
| Kaempferol | 16.51 ± 1.06 b | 23.59 ± 1.17 a | 24.05 ± 1.35 a |
| Naringin | 1149.76 ± 2.96 a | 1153.55 ± 3.28 a | 778.10 ± 2.86 b |
| Catechin | 562.78 ± 2.79 b | 968.78 ± 3.05 a | 542.94 ± 2.69 c |
| Epicatechin | 212.56 ± 2.17 a | 165.94 ± 1.96 b | nd |
nd *—Not determined; a–c the experiments were performed in triplicate and given as mean ± SD. Values in a row with different superscripts differ significantly (p < 0.05).
Polar volatile compounds in the ethanol-water extracts of rose oil industry byproducts.
| Compound | RIexp | RIcalc | % of TIC | ||
|---|---|---|---|---|---|
| 30% | 70% | 90% | |||
| α-Pinene | 940 | 932 | 0.88 ± 0.12 a | 0.92 ± 0.10 a | 0.86 ± 0.10 a |
| β-pinene | 980 | 974 | 0.61 ± 0.06 a | 0.64 ± 0.07 a | 0.63 ± 0.07 a |
| β-Myrcene | 991 | 988 | 0.35 ± 0.05 a | 0.36 ± 0.04 a | 0.37 ± 0.04 a |
| γ-Terpinene | 1062 | 1054 | 0.92 ± 0.06 a | 0.96 ± 0.10 a | 0.95 ± 0.10 a |
| Terpinolene | 1087 | 1086 | 0.68 ± 0.06 a | 0.71 ± 0.06 a | 0.73 ± 0.06 a |
| β-Linalool | 1097 | 1095 | 2.72 ± 0.14 a | 2.84 ± 0.09 a | 2.81 ± 0.09 a |
| Phenethyl alkohol | 1110 | 1106 | 14.11 ± 0.16 a | 13.84 ± 0.20 a | 13.80 ± 0.20 a |
| cis-Rose oxide | 1112 | 1107 | 0.44 ± 0.06 a | 0.46 ± 0.06 a | 0.46 ± 0.06 a |
| trans-Rose oxide | 1127 | 1122 | 0.25 ± 0.05 a | 0.26 ± 0.04 a | 0.27 ± 0.04 a |
| Terpin-4-ol | 1178 | 1174 | 0.33 ± 0.06 a | 0.35 ± 0.08 a | 0.33 ± 0.08 a |
| α-Terpineol | 1189 | 1186 | 0.35 ± 0.04 a | 0.37 ± 0.06 a | 0.32 ± 0.06 a |
| β-Citronellol | 1228 | 1223 | 9.73 ± 0.12 a | 10.18 ± 0.12 b,c | 10.01 ± 0.12 c |
| Nerol | 1230 | 1227 | 5.88 ± 0.10 a,b | 6.15 ± 0.11 a | 5.45 ± 0.11 b |
| Geraniol | 1255 | 1249 | 4.47 ± 0.13 a | 4.67 ± 0.12 a | 4.07 ± 0.12 a |
| Citronellyl acetate | 1354 | 1350 | 0.69 ± 0.06 a | 0.72 ± 0.06 a | 0.73 ± 0.06 a |
| Eugenol | 1356 | 1356 | 0.19 ± 0.005 a | 0.20 ± 0.03 a | 0.21 ± 0.03 a |
| Neryl acetate | 1364 | 1359 | 2.11 ± 0.12 a | 2.20 ± 0.11 a | 2.15 ± 0.11 a |
| Geranyl acetate | 1383 | 1379 | 2.86 ± 0.09 a | 2.99 ± 0.11 a | 2.90 ± 0.11 a |
| Methyl eugenol | 1401 | 1403 | 0.44 ± 0.06 a | 0.47 ± 0.06 a | 0.48 ± 0.06 a |
| β-Bourbonene | 1383 | 1387 | 3.19 ± 0.10 a | 3.33 ± 0.12 a | 3.23 ± 0.12 a |
| β-Cubebene | 1389 | 1388 | 5.95 ± 0.15 a | 4.22 ± 0.12 b | 4.28 ± 0.12 b |
| β-Elemene | 1390 | 1389 | 0.51 ± 0.06 a | 0.53 ± 0.09 a | 0.50 ± 0.09 a |
| β-Caryophyllene | 1419 | 1417 | 3.66 ± 0.10 a | 3.83 ± 0.10 a | 3.84 ± 0.10 a |
| α-Humulene (α-Caryophyllene) | 1454 | 1452 | 0.34 ± 0.03 a | 0.36 ± 0.06 a | 0.35 ± 0.06 a |
| Germacrene D | 1479 | 1484 | 0.40 ± 0.05 a | 0.42 ± 0.08 a | 0.40 ± 0.08 a |
| α-Farnesene | 1508 | 1505 | 0.57 ± 0.05 a | 0.59 ± 0.05 a | 0.58 ± 0.05 a |
| β-Bisabolene | 1510 | 1506 | 0.18 ± 0.04 a | 0.19 ± 0.03 a | 0.20 ± 0.03 a |
| trans-Nerolidol | 1564 | 1561 | 4.95 ± 0.06 a | 7.27 ± 0.08 a | 7.37 ± 0.08 a |
| Spathulenol | 1575 | 1577 | 1.65 ± 0.10 a | 1.72 ± 0.06 a | 1.70 ± 0.06 a |
| Caryophyllene oxide | 1580 | 1582 | 0.33 ± 0.05 a | 0.34 ± 0.06 a | 0.33 ± 0.06 a |
| γ-Eudesmol | 1631 | 1630 | 0.30 ± 0.06 a | 0.31 ± 0.06 a | 0.30 ± 0.06 a |
| β-Eudesmol | 1649 | 1649 | 0.26 ± 0.06 a | 0.27 ± 0.04 a | 0.28 ± 0.04 a |
| α-Eudesmol | 1651 | 1652 | 0.89 ± 0.05 a | 0.94 ± 0.05 a | 0.90 ± 0.05 a |
| Farnesol | 1714 | 1714 | 0.34 ± 0.06 a | 0.36 ± 0.04 a | 0.35 ± 0.04 a |
| n-Nonadecane | 1901 | 1900 | 8.28 ± 0.12 a | 7.66 ± 0.15 a | 7.78 ± 0.15 a |
| n-Eicosane | 2000 | 2000 | 3.86 ± 0.10 a | 3.04 ± 0.09 b | 3.05 ± 0.09 b |
| n-Heneicosane | 2100 | 2100 | 2.80 ± 0.10 a | 2.93 ± 0.12 a | 2.90 ± 0.12 a |
| n-Docosane | 2200 | 2200 | 2.82 ± 0.10 a | 2.95 ± 0.10 a | 2.91 ± 0.10 a |
| n-Tricosane | 2300 | 2300 | 4.50 ± 0.06 a | 3.71 ± 0.11 a,b | 3.83 ± 0.11 a,b |
| n-Tetracosane | 2400 | 2400 | 1.61 ± 0.09 a | 1.69 ± 0.11 a | 1.65 ± 0.11 a |
| n-Pentacosane | 2500 | 2500 | 1.43 ± 0.09 a | 1.49 ± 0.10 a | 1.45 ± 0.10 a |
| n-Hexacosane | 2600 | 2600 | 1.42 ± 0.07 a | 1.48 ± 0.11 a | 1.43 ± 0.11 a |
RIexp—Experimentally determined retention index (Kovats retention index); RIcalc—calculated retention index; TIC—total ion current; a–c the experiments were performed in triplicate and given as mean ± SD. Values in a row with different superscripts differ statistically (p < 0.05).
Physicochemical composition and characteristics of the AWTBs.
| Series | Sample | Parameters | ||||||||
| Sugars, (g/L) | Ethanol, (% v/v) | TA, (g/L) | VA, (g/L) | TPP, µmol GAE/L | TMA, mg CG/L | ORAC, µmol TE/L | HORAC, µmol GAE/L | CI, dA% | ||
| control | 1.26 ± 0.08 b,c | 12.30 ± 0.45 d | 5.65 ± 0.24 a | 0.30 ± 0.02 a | 230.00 ± 5.21 d | 9.22 ± 0.57 a | 3514 ± 169 d | 3045 ± 175 d | 66.44 ± 2.37 a | |
| ARW_E | 50 | 1.20 ± 0.05 c,d | 13.90 ± 0.32 c | 5.60 ± 0.31 a | 0.35 ± 0.04 a | 276.15 ± 6.57 b,c | 9.00 ± 0.69 a | 4057 ± 164 c | 3097 ± 164 d | 62.77 ± 1.99 b,c |
| 100 | 1.10 ± 0.07 d | 14.60 ± 0.58 c | 5.60 ± 0.27 a | 0.32 ± 0.01 a | 270.34 ± 4.69 c | 8.88 ± 0.43 a | 4268 ± 127 c | 3156 ± 170 d | 63.86 ± 2.03 a,b | |
| 200 | 1.60 ± 0.10 a | 16.90 ± 0.67 b | 5.45 ± 0.32 a | 0.38 ± 0.03 a | 286.79 ± 3.88 a,b | 8.87 ± 0.65 a | 4387 ± 138 b,c | 3284 ± 148 c,d | 61.29 ± 2.14 b,c | |
| 400 | 1.40 ± 0.06 b | 21.50 ± 0.72 a | 5.40 ± 0.20 a | 0.30 ± 0.05 a | 293.73 ± 4.29 a | 8.71 ± 0.71 a | 4461 ± 151 b,c | 3361 ± 163 c | 56.56 ± 1.86 c | |
| ARW_M | 12.5 | 1.30 ± 0.08 b,c | 12.30 ± 0.49 d | 5.60 ± 0.26 a | 0.35 ± 0.04 a | 277.47 ± 5.02 b,c | 9.03 ± 0.62 a | 4125 ± 164 c | 3124 ± 158 d | 60.37 ± 2.08 b,c |
| 25 | 1.16 ± 0.05 c,d | 12.35 ± 0.51 d | 5.60 ± 0.30 a | 0.32 ± 0.06 a | 270.24 ± 3.69 c | 8.96 ± 0.58 a | 4328 ± 147 b,c | 3267 ± 160 c,d | 62.47 ± 2.32 a,b | |
| 50 | 1.56 ± 0.08 a | 12.30 ± 0.37 d | 5.85 ± 0.28 a | 0.38 ± 0.02 a | 288.76 ± 4.87 a,b | 8.85 ± 0.39 a | 4462 ± 139 b,c | 3408 ± 159 b,c | 59.19 ± 2.11 c | |
| 100 | 1.60 ± 0.09 a | 12.40 ± 0.29 d | 5.90 ± 0.21 a | 0.39 ± 0.03 a | 296.13 ± 3.57 a | 8.66 ± 0.47 a | 4691 ± 154 b | 3565 ± 146 b | 58.41 ± 1.67 c | |
| ARW_CoF | 12.5 | 1.32 ± 0.04 b | 12.40 ± 0.35 d | 5.60 ± 0.34 a | 0.30 ± 0.05 a | 278.50 ± 5.71 b,c | 9.20 ± 0.56 a | 4502 ± 153 b | 3454 ± 163 b,c | 61.13 ± 1.93 b,c |
| 25 | 1.08 ± 0.07 d | 12.30 ± 0.32 d | 5.70 ± 0.26 a | 0.38 ± 0.07 a | 272.50 ± 4.28 c | 9.06 ± 0.64 a | 4618 ± 148 b | 3520 ± 154 b | 61.34 ± 2.37 b,c | |
| 50 | 1.57 ± 0.06 a | 12.35 ± 0.41 d | 5.80 ± 0.31 a | 0.32 ± 0.04 a | 289.67 ± 4.62 a,b | 8.84 ± 0.52 a | 5037 ± 160 a | 3677 ± 161 b | 60.48 ± 2.16 b,c | |
| 100 | 1.68 ± 0.09 a | 12.50 ± 0.48 d | 5.95 ± 0.24 a | 0.35 ± 0.06 a | 295.50 ± 3.78 a | 8.78 ± 0.81 a | 4921 ± 152 a | 3933 ± 157 a | 58.86 ± 2.34 c | |
TA—Titratable acids; VA—volatile acids; TMA—total monomeric anthocyanins; CG—cyanidin 3-glucoside; TPP—total polyphenolic content; GAE—gallic acid equivalents; ORAC—antioxidant activity measured by oxygen radical absorbance capacity assay; HORAC—antioxidant activity measured by hydroxyl radical averting capacity assay; TE—Trolox equivalents; CI, dA%—relative part of the red color due to flavilium cations of anthocyanins; a–d the experiments were performed in triplicate and given as mean ± SD. Values with different superscript letters in a column are significantly different (p < 0.05).
Content of low-molecular weight volatile compounds in the control and the AWTBs determined by GC–FID (mg/L).
| Compound | Control | ARW_CoF | ARW_M | ARW_E | |||||||||
|---|---|---|---|---|---|---|---|---|---|---|---|---|---|
| 12.5 | 25 | 50 | 100 | 12.5 | 25 | 50 | 100 | 50 | 100 | 200 | 400 | ||
| Acet-aldehyde | 15.00 ± 1.02 a | 17.15 ± 1.15 a,b | 19.01 ± 0.84 b | 19.89 ± 1.05 b | 20.15 ± 1.11 b | 15.01 ± 0.98 a | 15.39 ± 0.14 a | 19.21 ± 1.35 b | 16.35 ± 1.10 a | 17.64 ± 1.14 a,b | 15.88 ± 1.21 a | 18.64 ± 1.09 a,b | 17.49 ± 0.99 a,b |
| Ethyl acetate | 23.57 ± 1.62 a | 26.57 ± 1.30 a,b | 27.86 ± 1.48 b | 26.58 ± 1.67 a,b | 28.67 ± 2.01 b | 23.54 ± 1.67 a | 25.88 ± 1.36 a,b | 22.48 ± 1.09 a | 24.07 ± 2.03 a,b | 23.15 ± 1.48 a | 22.77 ± 1.74 a | 21.59 ± 1.14 a | 24.13 ± 1.15 a |
| Methanol | 20.47 ± 0.99 a | 19.87 ± 1.13 a | 21.69 ± 1.14 a | 21.47 ± 1.18 a | 22.05 ± 1.61 a | 19.05 ± 1.05 a | 22.73 ± 0.98 a | 20.34 ± 1.18 a | 21.75 ± 1.47 a | 20.35 ± 1.16 a | 19.68 ± 1.12 a | 21.64 ± 1.30 a | 20.97 ± 1.28 a |
| 2-Propanol | 13.36 ± 1.06 a | 11.08 ± 1.15 a | 14.28 ± 1.31 a | 13.64 ± 1.15 a | 14.95 ± 1.47 a | 11.04 ± 1.04 a | 12.46 ± 1.14 a | 12.24 ± 1.31 a | 11.08 ± 1.28 a | 10.38 ± 1.29 a | 10.83 ± 1.64 a | 11.53 ± 1.58 a | 12.72 ± 1.17 a |
| 1-Propanol | 35.49 ± 1.84 a | 38.84 ± 2.18 a | 38.61 ± 2.17 a | 39.67 ± 2.31 a,b | 41.27 ± 2.26 b | 37.73 ± 1.98 a | 40.22 ± 1.84 a,b | 42.77 ± 2.15 b | 40.69 ± 2.17 a | 41.87 ± 2.48 b | 40.01 ± 2.60 a | 39.24 ± 2.09 a | 38.64 ± 2.13 a |
| 2-Methyl-1-propanol | 33.58 ± 1.65 a | 34.59 ± 1.86 a | 33.61 ± 1.89 a | 37.84 ± 1.91 b | 36.64 ± 2.01 b | 38.80 ± 1.87 b | 37.82 ± 2.11 b | 35.88 ± 1.94 a,b | 33.51 ± 2.48 a | 37.28 ± 1.94 b | 37.79 ± 2.13 b | 43.95 ± 2.05 c | 33.77 ± 2.00 a |
| 1-Butanol | 10.48 ± 1.06 a | 7.28 ± 1.87 a | 7.67 ± 1.34 a | 8.78 ± 1.45 a | 9.61 ± 1.67 a | 10.59 ± 0.99 a | 11.45 ± 1.46 a | 11.21 ± 1.37 a | 10.33 ± 1.26 a | 9.93 ± 1.16 a | 9.31 ± 1.09 a | 10.11 ± 1.99 a | 10.81 ± 1.48 a |
| 3-Methyl-1-butanol (isoamyl alcohol) * | 53.30 ± 2.64 a | 60.51 ± 2.89 b | 57.13 ± 2.84 a,b | 61.21 ± 2.67 b | 65.20 ± 2.96 b | 59.48 ± 2.83 b | 60.17 ± 2.67 b | 62.58 ± 2.86 b | 61.69 ± 2.57 b | 58.32 ± 2.87 b | 60.15 ± 2.93 b | 61.59 ± 3.01 b | 63.94 ± 2.83 b,c |
a–c The experiments were performed in triplicate and given as mean ± SD. Values with different superscript letters in a row are significantly different (Tukey’s HSD test, p < 0.05); * 3-methyl-1-butanol plus other higher alcohols (alcohols with a C-chain of more than four carbon atoms).
Polar nonvolatile metabolites in the control wine and the AWTBs determined by GC–MS (mg/L).
| Compound | RIexp | RIcalc | Control | ARW_CoF | ARW_M | ARW_E | |||||||||
|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|
| 12.5 | 25 | 50 | 100 | 12.5 | 25 | 50 | 100 | 50 | 100 | 200 | 400 | ||||
| L-Valine | 1228 | 1224 | 0.76 ± 0.11 a | 0.89 ± 0.24 a | 0.83 ± 0.10 a | 0.75 ± 0.15 a | 0.79 ± 0.14 a | 1.00 ± 0.17 a | 0.94 ± 0.12 a | 0.84 ± 0.10 a | 0.89 ± 0.13 a | 0.97 ± 0.12 a | 0.90 ± 0.26 a | 0.81 ± 0.15 a | 0.85 ± 0.09 a |
| L-Leucine | 1272 | 1272 | 0.50 ± 0.20 a | 0.59 ± 0.12 a | 0.55 ± 0.14 a | 0.49 ± 0.10 a | 0.52 ± 0.16 a | 0.66 ± 0.13 a | 0.62 ± 0.17 a | 0.55 ± 0.12 a | 0.58 ± 0.11 a | 0.63 ± 0.13 a | 0.59 ± 0.15 a | 0.53 ± 0.17 a | 0.56 ± 0.13 a |
| Phosphoric acid | 1278 | 1272 | 8.60 ± 0.40 a | 10.14 ± 0.31 b | 9.46 ± 0.52 a,b | 8.49 ± 0.43 a | 8.94 ± 0.35 a | 11.39 ± 0.34 b | 10.63 ± 0.32 a,b | 9.54 ± 0.37 a,b | 10.04 ± 0.39 a,b | 10.94 ± 0.52 b | 10.21 ± 0.34 a,b | 9.16 ± 0.38 a,b | 9.65 ± 0.52 a,b |
| L-Isoleucine | 1299 | 1293 | 0.35 ± 0.11 a | 0.41 ± 0.10 a | 0.39 ± 0.12 a | 0.35 ± 0.15 a | 0.36 ± 0.13 a | 0.47 ± 0.09 a | 0.43 ± 0.11 a | 0.39 ± 0.08 a | 0.41 ± 0.09 a | 0.45 ± 0.11 a | 0.42 ± 0.14 a | 0.37 ± 0.13 a | 0.39 ± 0.12 a |
| L-Proline | 1307 | 1304 | 1.99 ± 0.31 a | 2.34 ± 0.28 a | 2.18 ± 0.26 a | 1.96 ± 0.25 a | 2.06 ± 0.22 a | 2.63 ± 0.27 a | 2.45 ± 0.22 a | 2.20 ± 0.23 a | 2.32 ± 0.18 a | 2.53 ± 0.20 a | 2.36 ± 0.19 a | 2.12 ± 0.17 a | 2.23 ± 0.21 a |
| Succinic acid | 1310 | 1307 | 5.72 ± 0.52 a | 6.74 ± 0.41 a | 6.29 ± 0.38 a | 5.65 ± 0.42 a | 5.94 ± 0.44 a | 7.57 ± 0.43 b | 7.07 ± 0.34 b | 6.34 ± 0.51 a | 6.68 ± 0.29 a,b | 7.27 ± 0.35 b | 6.79 ± 0.27 a,b | 6.09 ± 0.29 a,b | 6.41 ± 0.35 a,b |
| Glyceric acid | 1339 | 1335 | 1.27 ± 0.23 a | 1.49 ± 0.24 a,b | 1.39 ± 0.18 a | 1.25 ± 0.19 a | 1.32 ± 0.17 a | 1.68 ± 0.16 b | 1.56 ± 0.17 a,b | 1.40 ± 0.18 a,b | 1.48 ± 0.16 a,b | 1.61 ± 0.19 a,b | 1.50 ± 0.15 a,b | 1.35 ± 0.17 a | 1.42 ± 0.18 a,b |
| Fumaric acid | 1355 | 1349 | 0.92 ± 0.10 a | 1.09 ± 0.22 a | 1.02 ± 0.17 a | 0.91 ± 0.16 a | 0.96 ± 0.12 a | 1.22 ± 0.14 a | 1.14 ± 0.12 a | 1.03 ± 0.13 a | 1.08 ± 0.14 a | 1.18 ± 0.16 a | 1.10 ± 0.10 a | 0.98 ± 0.17 a | 1.04 ± 0.18 a |
| L-Serine | 1362 | 1365 | 0.43 ± 0.11 a | 0.50 ± 0.12 a | 0.47 ± 0.10 a | 0.42 ± 0.14 a | 0.44 ± 0.08 a | 0.56 ± 0.07 a | 0.53 ± 0.09 a | 0.47 ± 0.11 a | 0.50 ± 0.14 a | 0.54 ± 0.13 a | 0.50 ± 0.09 a | 0.45 ± 0.08 a | 0.48 ± 0.10 a |
| L-Threonine | 1390 | 1386 | 0.22 ± 0.05 a | 0.26 ± 0.07 a | 0.24 ± 0.10 a | 0.22 ± 0.06 a | 0.23 ± 0.08 a | 0.29 ± 0.11 a | 0.27 ± 0.09 a | 0.24 ± 0.07 a | 0.26 ± 0.06 a | 0.28 ± 0.11 a | 0.26 ± 0.10 a | 0.24 ± 0.08 a | 0.25 ± 0.09 a |
| L-Homoserine | 1446 | 1442 | 6.86 ± 0.60 a | 8.09 ± 0.54 b,c | 7.55 ± 0.48 a,b | 6.78 ± 0.39 a | 7.13 ± 0.37 a,b | 9.09 ± 0.35 c | 8.48 ± 0.40 a,b,c | 7.61 ± 0.34 a,b | 8.01 ± 0.42 a,b | 8.73 ± 0.36 a,b,c | 8.14 ± 0.38 a,b | 7.31 ± 0.42 a | 7.69 ± 0.38 a,b |
| Pyroglutamic acid | 1512 | 1515 | 0.72 ± 0.14 a | 0.85 ± 0.20 a | 0.79 ± 0.18 a | 0.71 ± 0.17 a | 0.75 ± 0.13 a | 0.95 ± 0.14 a | 0.90 ± 0.10 a | 0.80 ± 0.11 a | 0.84 ± 0.12 a | 0.92 ± 0.13 a | 0.86 ± 0.10 a | 0.77 ± 0.10 a | 0.81 ± 0.11 a |
| Salicylic acid | 1516 | 1519 | 0.79 ± 0.11 a | 0.93 ± 0.20 a | 0.86 ± 0.21 a | 0.78 ± 0.14 a | 0.82 ± 0.12 a | 1.04 ± 0.14 a | 0.97 ± 0.16 a | 0.87 ± 0.15 a | 0.92 ± 0.12 a | 1.00 ± 0.10 a | 0.93 ± 0.17 a | 0.84 ± 0.12 a | 0.88 ± 0.12 a |
| L-Aspartic acid | 1531 | 1527 | 0.38 ± 0.11 a | 0.44 ± 0.10 a | 0.41 ± 0.08 a | 0.37 ± 0.08 a | 0.39 ± 0.10 a | 0.50 ± 0.12 a | 0.47 ± 0.07 a | 0.42 ± 0.06 a | 0.44 ± 0.07 a | 0.48 ± 0.06 a | 0.45 ± 0.08 a | 0.40 ± 0.11 a | 0.42 ± 0.10 a |
| L-Threonic acid | 1528 | 1531 | 1.33 ± 0.21 a | 1.57 ± 0.32 a | 1.46 ± 0.27 a | 1.31 ± 0.32 a | 1.38 ± 0.26 a | 1.76 ± 0.19 a | 1.64 ± 0.22 a | 1.48 ± 0.19 a | 1.55 ± 0.20 a | 1.69 ± 0.24 a | 1.58 ± 0.18 a | 1.42 ± 0.17 a | 1.49 ± 0.19 a |
| L-(+)-Tartaric acid | 1612 | 1614 | 215.14 ± 2.20 b,c | 210.70 ± 1.91 c | 211.46 ± 2.57 c | 218.65 ± 2.32 a,b | 217.81 ± 2.81 a,b | 214.62 ± 1.86 b,c | 215.48 ± 2.33 b,c | 217.81 ± 2.10 a,b | 216.45 ± 2.08 b | 212.91 ± 2.52 c | 210.08 ± 1.98 c | 218.21 ± 2.53 a,b | 220.91 ± 3.10 a |
| L-Phenylalanine | 1646 | 1648 | 0.13 ± 0.02 a | 0.15 ± 0.05 a | 0.14 ± 0.04 a | 0.13 ± 0.02 a | 0.13 ± 0.03 a | 0.17 ± 0.01 a | 0.16 ± 0.01 a | 0.14 ± 0.01 a | 0.15 ± 0.02 a | 0.16 ± 0.04 a | 0.15 ± 0.04 a | 0.14 ± 0.01 a | 0.14 ± 0.01 a |
| L-Asparagine | 1682 | 1680 | 0.19 ± 0.01 a | 0.22 ± 0.02 a | 0.21 ± 0.03 a | 0.19 ± 0.04 a | 0.20 ± 0.01 a | 0.25 ± 0.02 a | 0.23 ± 0.01 a | 0.21 ± 0.05 a | 0.22 ± 0.02 a | 0.24 ± 0.01 a | 0.22 ± 0.03 a | 0.20 ± 0.02 a | 0.21 ± 0.01 a |
| L-Lysine | 1737 | 1738 | 0.81 ± 0.11 a | 0.95 ± 0.17 a | 0.89 ± 0.15 a | 0.80 ± 0.13 a | 0.84 ± 0.10 a | 0.96 ± 0.14 a | 0.91 ± 0.15 a | 0.95 ± 0.17 a | 0.93 ± 0.12 a | 0.88 ± 0.16 a | 0.87 ± 0.14 a | 0.86 ± 0.17 a | 0.84 ± 0.15 a |
| Ribonic acid | 1756 | 1753 | 0.60 ± 0.20 a | 0.71 ± 0.15 a | 0.66 ± 0.14 a | 0.59 ± 0.13 a | 0.62 ± 0.18 a | 0.79 ± 0.10 a | 0.74 ± 0.11 a | 0.67 ± 0.16 a | 0.70 ± 0.14 a | 0.76 ± 0.18 a | 0.71 ± 0.17 a | 0.64 ± 0.12 a | 0.67 ± 0.14 a |
| Vanillic acid | 1758 | 1760 | 0.74 ± 0.13 a | 0.87 ± 0.17 a | 0.81 ± 0.20 a | 0.73 ± 0.14 a | 0.76 ± 0.12 a | 0.97 ± 0.10 a | 0.91 ± 0.13 a | 0.82 ± 0.16 a | 0.86 ± 0.12 a | 0.93 ± 0.11 a | 0.87 ± 0.17 a | 0.78 ± 0.12 a | 0.82 ± 0.13 a |
| Protocatechuic acid | 1813 | 1812 | 0.38 ± 0.10 a | 0.45 ± 0.08 a | 0.42 ± 0.06 a | 0.38 ± 0.08 a | 0.40 ± 0.07 a | 0.51 ± 0.10 a | 0.47 ± 0.12 a | 0.42 ± 0.10 a | 0.45 ± 0.08 a | 0.49 ± 0.09 a | 0.45 ± 0.11 a | 0.41 ± 0.04 a | 0.43 ± 0.07 a |
| Quinic acid | 1843 | 1843 | 0.91 ± 0.11 a | 1.07 ± 0.10 a | 1.01 ± 0.18 a | 0.90 ± 0.17 a | 0.94 ± 0.12 a | 1.20 ± 0.20 a | 1.12 ± 0.19 a | 1.01 ± 0.14 a | 1.06 ± 0.12 a | 1.15 ± 0.15 a | 1.08 ± 0.17 a | 0.97 ± 0.12 a | 1.02 ± 0.16 a |
| Fructose isomer | 1862 | 1864 | 69.17 ± 0.52 a | 81.54 ± 0.67 b | 76.09 ± 0.59 c | 68.32 ± 0.58 a | 71.91 ± 0.32 a | 91.61 ± 0.50 d | 85.48 ± 0.47 e | 76.75 ± 0.39 c | 80.79 ± 0.52 b | 87.98 ± 0.65 e | 82.09 ± 0.68 b | 73.71 ± 0.67 f | 77.59 ± 0.52 c |
| Fructose isomer | 1868 | 1870 | 18.64 ± 0.73 a | 21.97 ± 0.48 b | 20.50 ± 0.67 a | 18.41 ± 0.42 a | 19.38 ± 0.51 a | 24.69 ± 0.36 c | 23.03 ± 0.57 c | 20.68 ± 0.49 a | 21.77 ± 0.48 b | 23.71 ± 0.43 c | 22.12 ± 0.48 d | 19.86 ± 0.55 a | 20.91 ± 0.66 a |
| Fructose isomer | 1875 | 1875 | 33.81 ± 0.49 a | 39.86 ± 0.54 b | 37.20 ± 0.58 c | 33.40 ± 0.63 a | 35.15 ± 0.78 a | 44.78 ± 0.64 d | 41.79 ± 0.67 e | 37.52 ± 0.86 c | 39.50 ± 0.53 b | 43.01 ± 0.68 d | 40.13 ± 0.64 b | 36.03 ± 0.49 c | 37.93 ± 0.56 c |
| Galactose isomer | 1884 | 1880 | 9.85 ± 0.68 a | 11.61 ± 0.58 b | 10.83 ± 0.63 a,b | 9.72 ± 0.65 a | 10.24 ± 0.57 a,b | 13.04 ± 0.49 c | 12.17 ± 0.45 c | 10.93 ± 0.63 a,b | 11.50 ± 0.58 b,c | 12.52 ± 0.52 c | 11.69 ± 0.23 b,c | 10.49 ± 0.55 a,b | 11.04 ± 0.38 a,b,c |
| Syringic acid | 1888 | 1886 | 61.28 ± 0.61 a | 72.25 ± 0.67 b | 67.41 ± 0.56 c | 60.53 ± 0.72 a | 63.71 ± 0.67 d | 81.17 ± 0.65 e | 75.73 ± 0.73 f | 68.00 ± 0.68 c | 71.58 ± 0.80 b | 77.95 ± 0.65 f | 72.73 ± 0.73 b | 65.30 ± 0.67 c,d | 68.74 ± 0.62 c |
| Glucose isomer | 1896 | 1890 | 18.94 ± 0.29 a | 22.33 ± 0.45 b | 20.84 ± 0.50 a,b | 18.71 ± 0.53 a | 19.69 ± 0.38 a,b | 25.09 ± 0.51 c | 23.41 ± 0.47 b | 21.02 ± 0.42 a,b | 22.13 ± 0.48 b | 24.09 ± 0.39 c | 22.48 ± 0.54 b | 20.19 ± 0.46 a,b | 21.25 ± 0.42 a,b |
| Galactose isomer | 1907 | 1895 | 18.17 ± 0.48 a | 21.42 ± 0.37 b | 19.98 ± 0.42 a,b | 17.94 ± 0.63 a | 18.89 ± 0.48 a | 24.06 ± 0.39 c | 22.45 ± 0.38 b | 20.16 ± 0.36 b | 21.22 ± 0.47 b | 23.12 ± 0.45 c | 21.56 ± 0.46 b | 19.36 ± 0.38 a,b | 20.38 ± 0.36 a |
| Glucose isomer | 1916 | 1911 | 97.36 ± 0.81 a | 114.78 ± 0.94 b | 107.10 ± 0.86 c | 96.16 ± 0.59 a | 101.22 ± 0.78 d | 128.95 ± 0.81 e | 120.32 ± 0.68 f | 108.03 ± 0.42 c | 113.72 ± 0.64 b | 123.84 ± 0.86 g | 115.55 ± 0.67 h | 103.75 ± 0.72 d | 109.21 ± 0.88 c |
| Glucitol | 1930 | 1926 | 40.94 ± 0.59 a | 48.26 ± 0.60 b | 45.03 ± 0.48 c | 40.43 ± 0.71 a | 42.56 ± 0.67 d | 54.23 ± 0.69 e | 50.59 ± 0.68 f | 45.42 ± 0.56 c | 47.81 ± 0.67 b | 52.07 ± 0.59 e | 48.58 ± 0.48 b | 43.62 ± 0.48 c | 45.92 ± 0.52 c |
| Gluconic acid | 1991 | 1990 | 30.25 ± 0.68 a | 35.66 ± 0.59 b | 33.27 ± 0.52 c | 29.88 ± 0.71 a | 31.45 ± 0.74 a,c | 40.06 ± 0.59 d | 37.38 ± 0.48 e | 33.56 ± 0.52 c | 35.33 ± 0.67 b | 38.47 ± 0.48 e | 35.90 ± 0.39 b | 32.23 ± 0.38 c | 33.93 ± 0.37 c |
| Palmitic acid | 2039 | 2040 | 3.85 ± 0.31 a | 4.54 ± 0.44 a,b | 4.24 ± 0.29 a | 3.80 ± 0.27 a | 4.00 ± 0.28 a | 5.10 ± 0.32 b | 4.76 ± 0.35 a,b | 4.27 ± 0.29 a | 4.50 ± 0.38 a,b | 4.90 ± 0.37 b | 4.57 ± 0.40 a,b | 4.10 ± 0.33 a | 4.32 ± 0.29 a |
| Glucaric acid | 2013 | 2046 | 12.04 ± 0.41 a | 14.20 ± 0.50 b | 13.25 ± 0.39 a,b | 11.90 ± 0.38 a | 12.52 ± 0.39 a | 15.95 ± 0.42 c | 14.88 ± 0.51 b,c | 13.36 ± 0.64 b | 14.07 ± 0.38 b | 15.32 ± 0.37 c | 14.29 ± 0.36 b | 12.83 ± 0.50 a | 13.51 ± 0.48 b |
| Myo-Inositol | 2090 | 2092 | 26.12 ± 0.81 a | 30.80 ± 0.60 b | 28.74 ± 0.54 c | 25.80 ± 0.48 a | 27.16 ± 0.44 a | 34.60 ± 0.67 d | 32.28 ± 0.65 b | 28.99 ± 0.39 c | 30.51 ± 0.46 b | 33.23 ± 0.52 d | 31.00 ± 0.57 b | 27.84 ± 0.53 c | 29.30 ± 0.61 b |
| Stearic acid | 2132 | 2137 | 1.13 ± 0.19 a | 1.33 ± 0.20 a | 1.24 ± 0.14 a | 1.11 ± 0.17 a | 1.17 ± 0.22 a | 1.49 ± 0.21 a | 1.39 ± 0.20 a | 1.25 ± 0.18 a | 1.32 ± 0.16 a | 1.43 ± 0.24 a | 1.34 ± 0.18 a | 1.20 ± 0.13 a | 1.26 ± 0.17 a |
| Caffeic acid | 2140 | 2144 | 5.25 ± 0.22 a | 6.19 ± 0.30 a,b | 5.77 ± 0.27 a | 5.18 ± 0.25 a | 5.45 ± 0.29 a | 6.95 ± 0.23 b | 6.48 ± 0.28 a,b | 5.82 ± 0.20 a,b | 6.13 ± 0.34 a,b | 6.67 ± 0.32 b | 6.23 ± 0.28 b | 5.59 ± 0.23 a | 5.89 ± 0.28 a |
| Linoleic acid | 2209 | 2212 | 8.30 ± 0.40 a | 9.79 ± 0.41 b | 9.13 ± 0.54 a,b | 8.20 ± 0.38 a | 8.63 ± 0.37 a | 11.00 ± 0.33 c | 10.26 ± 0.35 c | 9.21 ± 0.34 a,b | 9.70 ± 0.42 c | 10.56 ± 0.46 c | 9.85 ± 0.35 c | 8.85 ± 0.33 a | 9.31 ± 0.29 a,b |
| α-Linolenic acid | 2217 | 2219 | 6.39 ± 0.22 a | 7.54 ± 0.24 b | 7.03 ± 0.23 b | 6.31 ± 0.40 a | 6.64 ± 0.44 a,b | 8.47 ± 0.26 c | 7.90 ± 0.19 b,c | 7.09 ± 0.25 b | 7.47 ± 0.24 b | 8.13 ± 0.53 c | 7.59 ± 0.28 b | 6.81 ± 0.43 a,b | 7.17 ± 0.29 b |
| Sucrose isomer α-D-Glc-(1,2)-β-D-Fru | 2649 | 2651 | 3.97 ± 0.18 a | 4.68 ± 0.21 b | 4.37 ± 0.18 a,b | 3.92 ± 0.23 a | 4.13 ± 0.25 a,b | 5.26 ± 0.19 c | 4.91 ± 0.24 b,c | 4.41 ± 0.18 b | 4.64 ± 0.30 b | 5.05 ± 0.23 c | 4.71 ± 0.28 b,c | 4.23 ± 0.32 a,b | 4.46 ± 0.27 b |
| Sucrose isomer α-D-Glc-(1,2)-β-D-Fru | 2660 | 2660 | 6.57 ± 0.30 a | 7.74 ± 0.41 b | 7.22 ± 0.55 a,b | 6.49 ± 0.39 a | 6.83 ± 0.27 a,b | 8.70 ± 0.32 c | 8.12 ± 0.29 b,c | 7.29 ± 0.28 a,b | 7.67 ± 0.40 b | 8.35 ± 0.19 b,c | 7.79 ± 0.43 b | 6.99 ± 0.30 a,b | 7.37 ± 0.34 a,b |
| Sucrose isomer α-D-Glc-(1,2)-β-D-Fru | 2674 | 2670 | 1.89 ± 0.22 a | 2.23 ± 0.31 a | 2.08 ± 0.29 a | 1.87 ± 0.22 a | 1.97 ± 0.27 a | 2.51 ± 0.19 a | 2.34 ± 0.18 a | 2.10 ± 0.14 a | 2.21 ± 0.18 a | 2.41 ± 0.21 a | 2.25 ± 0.16 a | 2.02 ± 0.17 a | 2.12 ± 0.13 a |
| Catechine | 3221 | 3218 | 3.31 ± 0.21 a | 3.90 ± 0.03 a,b | 3.64 ± 0.18 a | 3.27 ± 0.17 a | 3.44 ± 0.21 a | 4.38 ± 0.22 b | 4.09 ± 0.18 b | 3.67 ± 0.17 a | 3.86 ± 0.20 a,b | 4.21 ± 0.16 b | 3.93 ± 0.18 a,b | 3.52 ± 0.22 a | 3.71 ± 0.21 a |
| Stigmasterol | 3315 | 3307 | 1.13 ± 0.10 a | 1.33 ± 0.11 a | 1.24 ± 0.14 a | 1.11 ± 0.10 a | 1.17 ± 0.21 a | 1.49 ± 0.17 a | 1.39 ± 0.16 a | 1.25 ± 0.12 a | 1.31 ± 0.11 a | 1.43 ± 0.13 a | 1.34 ± 0.14 a | 1.20 ± 0.12 a | 1.26 ± 0.13 a |
| β-Sitosterol | 3355 | 3344 | 1.30 ± 0.12 a | 1.53 ± 0.21 a | 1.43 ± 0.17 a | 1.28 ± 0.15 a | 1.35 ± 0.21 a | 1.72 ± 0.16 a | 1.61 ± 0.14 a | 1.44 ± 0.16 a | 1.52 ± 0.17 a | 1.65 ± 0.14 a | 1.54 ± 0.13 a | 1.39 ± 0.17 a | 1.46 ± 0.16 a |
RIexp—Experimentally determined retention index (Kovats retention index); RIcalc—calculated retention index; a–h The experiments were performed in triplicate and given as mean ± SD. Values with different superscript letters in a row are significantly different (Tukey’s HSD test, p < 0.05).
Overall sensory evaluation and ranking of the AWTBs.
| Series | Sample | Sensory Evaluation | Ranking |
|---|---|---|---|
| Control | 80.0 ± 1.5 | - | |
| ARW_CoF | ARW_CoF_12.5 | 84.2 ± 1.3 | I |
| ARW_CoF_25 | 80.9 ± 1.2 | III | |
| ARW_CoF_50 | 83.4 ± 1.6 | I | |
| ARW_CoF_100 | 78.4 ± 1.9 | IV | |
| ARW_M | ARW_M_12.5 | 81.0 ± 1.1 | II |
| ARW_M_25 | 82.3 ± 1.4 | I | |
| ARW_M_50 | 77.6 ± 1.6 | III | |
| ARW_M_100 | 73.7 ± 1.8 | V | |
| ARW_E | ARW_E_50 | 79.1 ± 1.2 | II |
| ARW_E_100 | 81.0 ± 1.0 | II | |
| ARW_E_200 | 74.9 ± 1.5 | V | |
| ARW_E_400 | 70.2 ± 1.3 | V |
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; Spasov, Hristo 2 ; Dinkova, Rada 3 ; Denev, Petko 4
; Dincheva, Ivayla 5
; Mariyana Georgieva Topuzova 1 ; Chalova, Vesela 6
1 Department of Organic and Inorganic Chemistry, Technological Faculty, University of Food Technologies, 26 Maritsa Blvd., 4002 Plovdiv, Bulgaria;
2 Department of Wine and Beer Technology, Technological Faculty, University of Food Technologies, 26 Maritsa Blvd., 4002 Plovdiv, Bulgaria;
3 Department Food Preservation and Refrigeration Technology, Technological Faculty, University of Food Technologies, 26 Maritsa Blvd., 4000 Plovdiv, Bulgaria;
4 Laboratory of Biologically Active Substances, Institute of Organic Chemistry with Centre of Phytochemistry, Bulgarian Academy of Sciences, 139 Ruski Blvd., 4000 Plovdiv, Bulgaria;
5 Department of Agrobiotechnologies, Agrobioinstitute, Agricultural Academy, 8 “Dragan Tsankov” Blvd., 1164 Sofia, Bulgaria;
6 Department of Biochemistry and Molecular Biology, University of Food Technologies, 26 Maritsa Blvd., 4002 Plovdiv, Bulgaria