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Relation between volatile composition, ellagitannin content and sensory

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DOI: 10.1007/s00217-013-1930-0

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Eur Food Res Technol (2013) 236:735–746
DOI 10.1007/s00217-013-1930-0
ORIGINAL PAPER
Relation between volatile composition, ellagitannin content
and sensory perception of oak wood chips representing
different toasting processes
Kleopatra Chira • Pierre-Louis Teissedre
Received: 19 November 2012 / Revised: 20 January 2013 / Accepted: 23 January 2013 / Published online: 28 February 2013
Ó Springer-Verlag Berlin Heidelberg 2013
Abstract The evolution of both volatile and nonvolatile
(ellagitannins) compounds extracted from oak wood chips
while being macerated for 3 months in wine model solution
with eight different commercial chips [Toasted LT (Light
Toast), LT? (Light plus Toast), MT (Medium Toast), MT?
(Medium plus Toast), HT (Heavy Toast), Noisette, Special)
and un-toasted (UN)] was studied. Sensory analysis con-
cerning vanilla, spicy, overall woody, astringency, bitterness
and sweetness descriptors was conducted in parallel. A
2-month time is needed for the maximum extraction of el-
lagitannins and of furfural compound. Relating to other
volatile compounds, their concentration increased progres-
sively over time. Spicy, woody and vanilla aromas as well as
sweetness perception increased during contact time with oak
wood. Additionally to pyrolytic toasting stage, watering
process during toasting influences significantly oak wood
composition (lactones, vanillin guaiacol compounds and
ellagitannins). Correlation analysis between chemical and
sensory data demonstrated significant correlations between
chemical and sensory parameters and provides some insight
into the implication of volatile and nonvolatile composition
on the final quality perception of astringency. A predictive
model between astringency intensity and ellagitannins, fur-
fural, guaiacol and methyl guaiacol contents was estab-
lished. Ellagitannins levels explained 45 %, guaiacol and
methyl guaiacol contents interpreted 13.20 and 8.86 %,
K. Chira  P.-L. Teissedre (&)
ISVV, EA 4577, Œnologie, Univ. Bordeaux,
210 Chemin de Leysotte, 33140 Villenave d’Ornon, France
e-mail: p.teissedre@u-bordeaux2.fr
K. Chira  P.-L. Teissedre
INRA, ISVV, USC 1366 Œnologie, 210 Chemin de Leysotte,
33140 Villenave d’Ornon, France
respectively, whereas furfural levels justified 5.66 % of the
total astringency variance.
Keywords Oak wood  Volatile compounds 
Ellagitannins  Astringency  Predictive model
Introduction
The wood from which a barrel is made contributes to the
characteristics of the alcoholic beverages stored in it. Oak
wood has commonly been used in wine aging, during oak
wood contact, red wine undergoes important modifications,
as spontaneous clarification, slow and continuous diffusion
of oxygen through the wood pores of the oak barrel, and the
extraction of many substances from the oak wood (e.g.,
aromatic compounds and ellagitannins) which modulate its
organoleptic quality and complexity such as aroma, struc-
ture, astringency, bitterness, persistence color and astrin-
gency. The ellagitannins (hydrolysable tannins) are among
these substances. In oak heartwood, they may represent
10 % of the dry weight and are responsible for the high
durability of this wood [1]. From a quantitative point of
view, castalagin and vescalagin are the most abundant el-
lagitannins in oak wood [2] but lyxose/xylose derivatives
(grandinin and roburin E) and dimeric forms (roburins A,
B, C and D) are also present [3, 4]. The hydroalcoholic
nature of wine allows the extraction of these compounds
from wood to wine, but due to their high reactivity, their
levels in wine are much lower than could be expected. The
total ellagitannins levels in wine, being in contact four
months with oak staves, may range from 0.8 to 3.49 mg/L
of released ellagic acid [5].
Human sensory experiments revealed that ellagitannins
have an impact on astringency and bitterness sensation [6, 7].
123
736
The oral sensation imparted by ellagitannins was described
as astringent at relatively low threshold concentrations
spanning from 0.2 to 6.3 lmol/L, whereas bitterness was
strongly depending on ellagitannin structure, a bitter taste
was perceived at threshold concentrations between 410 and
1650 lmol/L. Recently, Stark et al. [8] observed that all
ellagitannin derivatives induce a smooth and velvety
astringent oral sensation at rather low threshold concen-
trations ranging from 0.9 to 2.8 lmol/L.
Other important wood chemicals, which might be
impact molecules, include the naturally present cis- and
trans-methyl-octalactone (whiskey lactones, with a coco-
nut flavor in their pure state), trans-2-nonenal (sawdust
smell), volatile phenols released via toasting such as
guaiacol, 4-methylguaiacol and eugenol (spicy and smoky
smells) and vanillin (vanilla smell). All of these com-
pounds can be present in barrel-aged wines in concentra-
tions above the sensory threshold; their concentrations
depend on the chemical composition of the barrel’s wood.
Some of them undergo modification in a wine medium.
The increasing demand for wood that is suitable for
barrel making and the rapid development of alternative
aging systems have led to the possibility of using wood
pieces. This practice recently was approved and legislated
by the European Community (CE 2165/2005 and CE
1507/2006), but in some countries such as Australia, South
Africa and Chile, this practice has been used for several
years. Different shapes of oak wood pieces can be found on
the market: chips, cubes or beans, powder, shavings or
granulates, dominoes, and blocks or segments. Factors such
as piece size, amount of added wood and contact time
between wood and wine affect the sensory and chemical
characteristics of wines [9–11], especially their wood-
related volatile composition [12].
There are several factors that determine the final char-
acteristics of wines macerated with chips, and some of
these factors have been studied in recent years. Some
papers have been written after studying the effect of chips
on the phenolic composition of different wines [9, 10, 13–
15], whereas others have focused on volatile compounds,
mainly on those extracted from wood. Thus, Guchu et al.
[16] evaluated the influence of the geographical origin of
the oak (American or Hungarian), the toasting degree
(toasted and nontoasted) and the time of contact on volatile
compounds in a white wine. Arapitsas et al. [12] also
studied the effect of the contact time, but only for 14 days,
and the size of the chips on red wines. Frangipane et al.
[11] studied four types of chips from four different French
forests, added to a red wine stored in 2-year-old barrels.
Campbell et al. [17] studied the origin of the wood and the
type of heating in model wines. An analysis of the results
discussed in these papers indicates a great variability in the
results, which is probably due to the fact that there are
123
Eur Food Res Technol (2013) 236:735–746
many factors that affect oak qualities used: origin; species
[18]; the method used to obtain the staves; the stave-drying
technique (natural or artificial) [19].
However, in order to know the compounds that oak
wood yields to the wine, the use of synthetic wine has the
advantage of ensuring the absence of any microbial activ-
ity. At the same time, by using synthetic wine, this ensures
that no fermenting compounds, and which could also come
from the barrels, will exist. The bibliography consulted
reveals few studies on the characterization of oak wood in a
synthetic medium [20].
Therefore, to clarify the impact of oak wood on wine
composition, a model wine was used. This approach mini-
mized any effect which may have arisen due to compounds
naturally present in wines, and microbial activity was kept to
a minimum. The accumulation of oak volatiles and non-
volatiles compounds was monitored over a 3-month time. In
parallel, sensory evaluation of wine model solution over a
3-month time was realized. The toasting level impact on
both volatile, nonvolatile compounds and sensory perception
was studied in parallel. The relationship between the
chemical composition and the sensory assessment of oak
wood extract was also investigated.
Materials and methods
Wood origin and drying conditions
The wood samples were constituted from two oak species
(Quercus robur and Quercus petraea) from the same forest
located in center in France. The oak wood was stored for
natural seasoning during 24 months in the Tonnellerie
Nadalié (Ludon-Medoc, France) seasoning park. Then,
they were crushed to oak chips dimensions (L = 1–2 cm,
h = 0.2–0.8 cm) and submitted to different toasting pro-
cedures according to the desired final product using oak
fire. Each time 150 kg of chips is put into a stainless drum
(1 m3) and this drum turns above an oak fire. The intensity
levels used are as follows: light (LT), 1 h and 30 min at
165°C; light plus (LT ?), 2 h at 170°C; medium (MT), 2 h
at 180°C; medium plus (MT ?), 2 h and 25 min at 190°C;
Noisette, 3 h at 175°C; Special 2 h at 180°C and heavy
toast (HT), 2 h and 30 min at 200°C. In the case of Special,
a watering process takes place. After 2 h of toasting, 30 L
of water is put to the drum, and afterward the drum is
placed above the fire in order to be heated for 30 min more.
Sample preparation
Each experiment was carried out in triplicate in hermeti-
cally closed 5-L glass jars. Different model wines were
prepared for this experiment, all in triplicate. Model wines
Eur Food Res Technol (2013) 236:735–746
were prepared with deionized water, HPLC grade ethanol
(Prolabo-VWR, Fontenay-sous-Bois, France) and tartaric
acid (Prolabo-VWR, Fontenay-sous-Bois, France). Titrat-
able acidity was adjusted to 4.5 g tartaric acid/L, and
ethanol level was 12 % (v/v).
Small pieces of French oak wood (L = 1–2 cm,
h = 0.2–0.8 cm) from the same forest located in the center
of France were supplied by Nadalié cooperage (Tonnellerie
Nadalié, Ludon-Medoc, France). Three grams of medium
size, UN (Untoast), LT (Light Toast), LT? (Light plus
Toast), MT (Medium Toast), MT? (Medium plus Toast),
HT (Heavy Toast), Noisette, Special chips were added to
the model wine solution. The jars were shaken once a day
to facilitate the extraction of oak compounds. Sampling
was carried out at 15 days, 1, 2 and 3 months from the
initiation of contact between the oak wood and the syn-
thetic wine. Afterward, elagitannins and aromatic com-
pounds quantification were performed by HPLC–UV and
GC–MS analysis, respectively. Sensory analysis was also
conducted.
Extraction of volatile compounds
Model wine solutions were extracted with dichlorometh-
ane; 200 lL of a solution of dodecan-1-ol as internal
standard was added to 50 mL of samples. Three extractions
were then carried out using 4, 2 and 2 mL of dichloro-
methane. The organic fractions were combined and dried
on sodium sulfate anhydrous and then concentrated to
500 lL under a nitrogen stream. In all cases, the samples
were analyzed in duplicate.
Gas-chromatography analysis
A simple and reliable GC method for quantitative deter-
mination of the volatile compounds arising from oak wood
was used according to an adaptation of a previous method
[21]. An Agilent HP 5890 GC (Hewlett–Packard, Wil-
mington, DE, USA) was coupled with a mass spectrometer
(HP 5972, electronic impact 70 eV, eMV = 2 kV). One
lL samples of organic extract were injected in splitless
mode. The column was BP21 (SGE) (50 m 9 0.32 mm,
0.25 lm); carrier gas was helium (pressure: 70 kPa);
temperatures were injector, 250 °C; detector, 280 °C;
oven, 60 °C for 1 min programmed at a rate of 3 °C/min to
240 °C, the final step lasting 40 min; the splitless time was
30 s with a split flow of 30 mL/min.
The compounds were identified by comparing their
retention times and mass spectra with those of the pure
reference standards. Working in the SIM mode, the fol-
lowing ions were used: syringaldehyde, m/z 182; vanillin,
m/z 151; eugenol, m/z 164; guaiacol, m/z 124; b-methyl-c-
octalactone, m/z 99; 5-methyl-2-furfuraldehyde, m/z 110;
737
furfuryl alcohol, m/z 98 and m/z 83 for the internal stan-
dard (dodecan-1-ol). The concentrations of each substance
were measured by comparison with calibrations made with
pure reference compounds analyzed under the same con-
ditions. The corresponding calibration was made for each
compound, and linear regression coefficients between 0.98
and 0.999 were obtained.
Sample preparation prior to total ellagitannin level
determination
Model wine solution (50 mL) was evaporated under
reduced pressure, and the resulting residue was dissolved in
methanol (20 mL); then, 4 mL of this mixture was loaded
in the hydrolysis tubes for the determination of the total
ellagitannin level.
Total ellagitannin level determination HPLC–UV
analysis
The total ellagitannin concentration was determined by the
quantification of ellagic acid released during acidic
hydrolysis (2 h at 100 °C, 2NHCl in MeOH) as previously
described [22]. Each sample was analyzed in triplicate, and
each reaction mixture was subjected to HPLC–UV using a
LiChrospher 100 RP-18 column, 250 9 4.6 mm, 5 lm.
The equipment used for the HPLC analysis consisted of a
Finnigan Surveyor UV–Vis detector (UV–Vis 200), a
Finnigan autosampler and a Finnigan ternary pump. The
mobile phases used were solvent A [H2O/H3PO4 (99.9/1)]
and solvent B [methanol/H3PO4 (99.9/1)], and the gradient
elution was 0–35 % of B in 5 min, 35–45 % of B in 25 min
and 45–100 % of B in 5 min. The flow rate was set at
1 mL/min with detection set at 370 nm.
Sensory analysis
The sensory assessment was done by a committee of 20
expert judges from the Oenology faculty of Bordeaux. The
judges were specially trained in the employment of scales
and aroma descriptors according to ISO 8586-1 [23]. The
attributes selected were grouped in two families: olfactive
descriptors related to wood–wine interaction (vanilla, spicy,
overall woody) and gustative descriptors (sweetness astrin-
gency and bitterness). The ‘‘overall woody’’ descriptor was
chosen by tasters to describe all olfactory sensations brought
about by the wood.
Panellists attended 16 training sessions over a period of
2 months. The training period included a first general phase
a second and a third, product-specific training phase. The
general phase was dedicated to the recognition of sensa-
tions and aromas perceived. Aqueous solutions of vanillin
(20 lg/L), eugenol (60 lg/L), furfurylthiol (0.8 ng/L) and
123
738
oak wood chip (5 g/L medium toast) were proposed for
vanilla, spicy and overall woody character, respectively.
Aqueous solutions of quinine sulfate (0.25 g/L), aluminum
sulfate (3 g/L) and sucrose (4 g/L) were proposed to set
bitterness, astringency and sweetness. During this session,
the discriminative ability of participants was assessed.
Samples were presented, and participants were instructed
to identify the solutions as sweet, bitter, astringent, spicy,
overall woody or vanilla. All participants correctly identi-
fied all solutions.
During the second phase (8 sessions), the judges have
been trained to evaluate the descriptors: sweet, bitter,
astringent, spicy, woody or vanilla in various concentra-
tions [23]. In order to improve panel performance, scaling
training (ranking of solution according to concentration of
descriptor) was used. Fourth sessions were used for the
olfactory attributes and four for the sensory gustative
attributes. Wine model solutions containing different con-
centrations of table sugar (0–24 g /L) for sweetness [24],
quinine sulfate (0–15 mg/ L) for bitterness, aluminum
sulfate (0–4 g /L) for astringency, vanillin (0–320 lg/L)
for vanilla, eugenol (0–500 lg/L) for spicy and medium
toast oak wood chip (0–10 g/L) for woody were presented
to the panel to aid them to discriminate between the dif-
ferent concentrations. After this second phase, the dis-
criminative ability of participants was assessed.
The third phase (7 sessions) was allocated to familiarize
the judges with the intensity scale used (0–7). The first two
sessions have been dedicated to the overall assessment of
the descriptors of interest. Oak wood chips of different
concentrations (0–8 g/L) and of different toast (light,
medium and heavy) were added in model wine solutions in
order to determine the repeatability of judges from one
session to another. For the last five sessions, oak wood
chips of different concentrations (0–8 g/L) and of different
toast (light, medium, high) were added in red wine. After
these last sessions, the judges became familiar with
intensity rating of spicy, woody, vanilla, sweetness, bit-
terness and astringency using a 0–7 point scale.
In the formal sessions, the panelists were provided with
30 mL of wine in coded standard clear wine glasses [25],
covered with a watch glass to minimize the escape of vol-
atile components and coded with random three-digit num-
bers. Assessment took place in a standard sensory-analysis
chamber [26], equipped with separate booths, and with a
uniform source of lighting, absence of noise and distracting
stimuli, and ambient temperature between 19 and 22 °C.
Wines were sniffed and tasted. In every session, the
expert judges had to start with evaluation of the orthonasal
odor (first without moving the glass, then moving it
gently), and then, after a short break, they evaluated the
taste (sweetness, bitterness) and tactile sensation (astrin-
gency). The experiment was carried out in duplicate.
123
Eur Food Res Technol (2013) 236:735–746
Data analysis
Statistical data analysis was performed using the analysis
of variance (ANOVA) of Statistica V.7 software (Statsoft
Inc., Tulsa, OK). Tukey’s HSD and Duncan’s tests were
used as comparison tests when samples were significantly
different after ANOVA (p \ 0.05) for chemical and sen-
sory analysis, respectively. Principal component analysis
(PCA) was performed on the correlation matrix using the
attributes that differed significantly by ANOVA. Pearson’s
correlation analysis was used to investigate relationships
between chemical composition and sensory, perception.
Once correlations established, multiple regression analysis
was used to determine the extent to which the variance in
the sensory measures (astringency) could be predicted by
the remaining variables.
Results and discussion
Oak wood volatile composition
The following wood volatile compounds were studied:
furanic aldehydes, furfural and 5-methylfurfural, the two
isomers of methyl-c-octalactone, cis and trans (commonly
known as oak lactones or whiskey lactones); the volatile
phenols guaiacol, eugenol and cis- and trans-isoeugenol;
and the aldehyde phenols, vanillin and syringaldehyde.
Furfuryl compounds
The evolution of furfural and 5-methylfurfural concentra-
tions during aging was different and dependent on the
toasting (Fig. 1). Globally, furfural concentration was much
higher than that of 5-methylfurfural and was extracted
rapidly, reaching a maximum level at 60 days (2 months).
Using two pieces of oak wood (12 9 2 9 2 cm) in two
liters of model wine solution, an 105-day assay period was
needed to extract the maximum of furfural in model wine
solutions [27]. Using 10 grams of medium size in one liter
model wine solution [20], an 120-day assay period was
required for extracting the maximum of furfural. In the
current experiment, less time was demanded for the maxi-
mum extraction, probably due to the lower concentration of
oak chips used or even due to the toasting method used, oak
chips are toasted in oak fire.
cis- and trans-b-methyl-c-octalactones
cis-b-Methyl-c-octalactone was detected in bigger con-
centrations than trans-b-methyl-c-octalactone (Fig. 1). The
cis isomer is regarded as among the most important of oak
wood volatile components and is generally found at above
Eur Food Res Technol (2013) 236:735–746 739

UN (not toasted), LT (Light Toast), LT+ (Light plus Toast), MT (Medium Toast), MT+ (Medium Plus Toast), HT (Heavy Toast), Noisette, Special (toast with watering)

6000 450

Furfural 400 Methyl-Furfural

5000
Concentration in µg/L

350

Concentration in µg/L
4000 300

250
3000
200

150
2000
100

1000 50

0
0 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4
T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4
UN LT LT+ MT MT+ HT Noisette Special
UN LT LT+ MT MT+ HT Noisette Special

200 200

180 180 cis b methyl -γ -octalactone

Trans b methyl -γ -octalactone
160 160

Concentration in µg/L
Concentration in µg/L

140 140

120 120

100 100

80 80

60 60

40 40

20 20

0 0
T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4
UN LT LT+ MT MT+ HT Noisette Special UN LT LT+ MT MT+ HT Noisette Special

60
60
Guaiacol Methyl -Guaiacol
50
50
Concentration in µg/L

Concentration in µg/L

40
40

30
30

20
20

10
10

0
0
T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4
T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4
UN LT LT+ MT MT+ HT Noisette Special
UN LT LT+ MT MT+ HT Noisette Special

20
20

18 Syringol
Eugenol+Isoeugenol 18
16
16
Concentration in µg/L

Concentration in µg/L

14
14
12
12
10
10
8
8
6
6
4
4
2
2
0
T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4
0
UN LT LT+ MT MT+ HT Noisette Special T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4
UN LT LT+ MT MT+ HT Noisette Special

4500
1600
Synrigaldehyde
4000
1400 Vanillin
Concentration in µg/L

3500
Concentration in µg/L

1200
3000
1000
2500
800
2000

600
1500

1000 400

500 200

0 0
T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4 T1 T2 T3 T4
UN LT LT+ MT MT+ HT Noisette Special UN LT LT+ MT MT+ HT Noisette Special

Fig. 1 Evolution of volatile oak compounds during different contact times (T1 = 15 days, T2 = 1 month, T3 = 2 months, T4 = 3 months)

123
740
its perception threshold [28]. The profile obtained for lac-
tone extraction from the wood is depending on their
toasting level. For almost all the samples, concentration
increases during the maceration time. Samples with UN
oak chips presented more important concentrations than
these with MT. This is due to the fact that b-methyl-c-
octalactone can be found naturally in oak wood [29, 30].
Moreover, light-toasted chips released more oak lactones to
wines than heavy toasted, probably due to the thermo-
degradation of these heat-sensitive compounds or their loss
by volatilization when the oak wood is subjected to very
high temperatures or even charring [31]. Noisette toast
showed the highest concentrations of lactones, and this
observation could be attributed to the fact that for Noisette,
the temperature used was lower and lasted more time than
this of MT. Comparing Special to MT oak chips, it is
observed that samples with Special extract more lactones,
implying that watering process during toasting enhance
lactones extraction.
Volatile phenols
Guaiacol and 4-methylguaiacol have smoky aromas and
indicate the wood toasting level [32] since they are formed
almost exclusively by the degradation of lignin during the
toasting process. The rate of extraction in model solutions
has been shown as consistent with their generation by
toasting, with the largest concentration presented at the end
of maceration time in samples with heavy toast oak chips
(Fig. 1). It is interesting to note that samples treated with
Noisette and Special extract less guaiacol compounds than
samples with MT, even if the toasting temperature used is
the same. Suggesting that the prolongation in toasting time
along with the watering during toasting is factors that
decrease guaiacol levels.
Eugenol increased its concentration from the beginning,
its concentration ranged from 2.72 lg/L (15 days for LT)
to 17.16 lg/L (after 3 months for Noisette) (Fig. 1). In
samples treated with HT oak, it was detected only after
1 month in a slight concentration of 0.74 lg/L, whereas in
samples with UN oak, it was presented from the beginning
to the end of maceration time (3.5–4.61 lg/L).
Phenolic aldehydes
Vanillin, which is very important to wine flavor, is present
in green wood but is also associated with the heating
process, so higher concentrations are to be expected in the
first few millimeters of the toasted wood. Its concentration
increased progressively over time, with the highest values
reached in the model solution with Noisette oak chip
(1431.08 lg/L after 3 months). Samples with MT and
MT ? oak chips extract more vanillin (1048.45 and
123
Eur Food Res Technol (2013) 236:735–746
970.88 lg/L, respectively) than samples with Special oak
(940.45 lg/L) at the end of 12-week period. This finding
suggests that watering during toasting process may
decrease significantly vanillin. Thus, except of alcohol
content and acidity [20], watering process during toasting
may modulate the extraction of lactones and vanillin.
In all samples, syringaldehyde content, like vanillin,
increased during maceration time, independently of the oak
type used. The samples with medium toast (Noisette, MT,
Special, MT?) presented the most important concentra-
tions, following by light (LT, LT?) and heavy toast (HT).
Indeed, toasting increases the quantities of aromatic
compounds and also leads to the formation of other new
compounds. Furanic aldehydes caused by carbohydrate
degradation and responsible for the ‘‘toasty’’ aromas, and
lignin degradation compounds (vanillin, syringaldehyde
and guaiacol) tend to be formed during the toasting pro-
cess. However, HT chips presented a low potential of
extracting volatile compounds, showing that toasting
increased concentrations of volatile compounds up to cer-
tain level of toasting and then decreases afterward [33]. In
general, it is observed that Noisette oak wood extracts
more volatile compounds following by MT, MT? and
Special oak wood extracts. These observations indicate that
1-hour prolongation in toasting process along with a 5 °C
decrease in toasting temperature enhance oak volatile
extraction.
Oak wood total ellagitannin concentration
The ellagitannin level and composition in each oak stave
were determined by HPLC–UV. In a first approach, the
total ellagitannin level was estimated by the determination
of the amount of ellagic acid released after acidic hydro-
lysis. During this reaction, each ellagitannin monomer or
dimer released one molecule of ellagic acid. The total el-
lagitannin level, expressed as mg/L of released ellagic acid
in wine model solution, revealed a large diversity of con-
centrations ranging from 0.95 to 13.72 mg of released
ellagic acid/L of wine model solution (Fig. 2). The UN and
the HT presented the highest and the less important
ellagitannins concentrations. Fig. 2 reveals the drastic
changes in wood chemical composition that occur during
toasting. Such differences were expected since ellagitan-
nins undergo thermolytic degradation during the toasting
process [34, 35]. UN oak chips presented the highest values
in mg of released ellagic acid/L of wine model solution
(from 8.96 (T1) to 13.72 (T4)), following by LT (from 7.87
(T1) to 9.52 (T4)), LT? (from 6.75 (T1) to 7.92 (T4)), MT
(from 3.10 (T1) to 6.23 (T4)), MT? (from 6.75 (T1) to 7.92
(T4)), Noisette (from 2.16 (T1) to 5.71 (T4)), Special (from
2.06 (T1) to 4.01 (T4)) and finally by HT (from 0.95 (T1)
to 1.21 (T4)). Moreover, the Fig. 2 demonstrates that
Eur Food Res Technol (2013) 236:735–746 741

16 16
UN LT
mg eq.released ellagic acid/L of model
14 14

mg eq.released ellagic acid/L of model

wine solution 12 12
10 10

wine solution
8 8
6 6
4 4
2 2
0 0
T1 T2 T3 T4 T1 T2 T3 T4
mg eq.released ellagic acid/L of model

16
16

LT+ 14 MT

mg eq.released ellagic acid/L of model

14

12 12
wine solution

10

wine solution
10

8 8

6 6

4 4

2 2

0 0
T1 T2 T3 T4 T1 T2 T3 T4
mg eq.released ellagic acid/L of model

16 16
MT+ HT
mgeq.releasedellagicacid/L of

14 14
model wine solution

12 12
wine solution

10 10
8 8
6 6
4 4
2 2
0 0
T1 T2 T3 T4
T1 T2 T3 T4
mg eq.released ellagic acid/L of model

mg eq.released ellagic acid/L of model

16
16
14
Noisette 14 Special
12
12
wine solution

wine solution

10
10
8
8
6
6
4
4
2 2
0 0
T1 T2 T3 T4 T1 T2 T3 T4

Fig. 2 Evolution of ellagitannins during different contact times (T1 = 15 days, T2 = 1 month, T3 = 2 months, T4 = 3 months)

independent toasting time and method, a maximum
extraction of ellagitannins is obtained after a 2-month time,
afterward a stabilization or even a decrease is observed.
During the first 2 months, wine model solution extracts
ellagitannins at a faster rate than between 2 and 3 months.
When most of the ellagitannins have been extracted from
the first millimeter of the wood, the solution needs to go
deeper in the wood to extract more ellagitannins, conse-
quently, at a slower rate. Samples with Special oak chips
not only presented less important ellagitannins concentra-
tions than samples with MT oak chips but they also showed
as well the greatest decrease in these compounds during

123
742 Eur Food Res Technol (2013) 236:735–746

Fig. 3 Sensory evaluation of UN Vanilla

model wine solution treated 5 LT Vanilla
5
with different oak chips during 4
4
different contact times Bitterness
3
Woody 3
Bitterness Woody
(T1 = 15 days, T2 = 1 month, 2
2
T3 = 2 months, 1
1
T4 = 3 months) 0
0

Astringency Spicy
UN T1 Astringency Spicy
LT T1
UN T2
LT T2
Sweetness UN T3 LT T3
Sweetness
UN T4 LT T4

LT+ Vanilla MT Vanilla

5 5
4
4
3
3 Bitterness Woody
Bitterness Woody 2
2
1
1
0
0

Astringency Spicy
LT+ T1
Astringenc MT T1
Spicy
y LT+ T2
MT T2
LT+ T3
Sweetness
MT T3
LT+ T4
Sweetness MT T4

MT+
Vanilla HT
5
Vanilla
4 5

3 4
Bitterness Woody
2 3
Bitterness Woody
1 2

0 1

0
MT+ T1
Astringenc
Spicy MT+ T2 HT T1
y Astringenc
Spicy
MT+ T3 y HT T2

MT+ T4 HT T3
Sweetness HT T4
Sweetness

Noisette Special
Vanilla Vanilla
5 5

4 4

3 3
Bitterness Woody Bitterness Woody
2 2

1
1
0
0

N T1 Astringenc S T1
Astringenc Spicy
Spicy y
y N T2 S T2

N T3 S T3

N T4 Sweetness S T4
Sweetness

123
Eur Food Res Technol (2013) 236:735–746
Fig. 4 Principal component
analysis (PCA) representation N
of chemical and sensory data for
model wine solution treated
with different oak chips during
different contact times
(T1 = 15 days, T2 = 1 month,
T3 = 2 months,
T4 = 3 months)
after 2 months. Thus, not only the pyrolytic toasting stages
diminish the quantity of these compounds but also the
watering procedure.
Sensory evaluation of oak chips
Figure 3 shows ‘‘spider web’’ diagrams for the average
scores of the olfactory attributes for all the trials. For all the
trials, it is observed that vanilla, smoky, grilled characters
along with sweetness build up, whereas astringency
intensity decreases slightly during the contact time. In
general, MT and MT? are perceived more woody, whereas
UN less woody; vanilla intensity varies from 1.9 (for UN
oak chips) to 4.4 (for Noisette oak chips), woody intensity
ranges from 0.4 (for UN oak chips) to 4.9 (for Noisette oak
chips); spicy character fluctuates from 1.1 (for HT oak
chips) to 3.3 (for Noisette oak chips); in parallel, samples
with Noisette after 3 months, presented the most important
levels of eugenol and vanillin contents, observation that
may justify their intense spicy and vanilla aroma. Samples
with Special were perceived less woody than samples with
MT oak chips which is accordance with the above results,
samples treated Special extract less guaiacol compounds
than samples with MT.
Sweetness perception goes from 2.0 (for UN oak chips)
to 3.2 (for MT oak chips); astringency perception varies
between 1.4 (for HT oak chips) and 4.3 (UN) and bitterness
varies between 2.0 (MT ?) and 4.2 (UN). Model wine
solutions treated with untoasted oak chips were generally
743
HT
LT
LT+
UN
more astringent and with stronger bitterness. This may be
attributed to their higher levels of ellagitannins.
Correlations between sensory and chemical results
The analysis of variance revealed that the toasting method
has a significant impact (p \ 0.05) on chemical composi-
tion and sensory perception of oak wood extracts. After-
ward correlations between sensory descriptors were
assessed. The PCA factor loading plot for the sensory
variables and the means for oak volatile compounds and
ellagitannins are shown in Fig. 4. This figure is comple-
mented by the Pearson’s correlation coefficient values
presented in Table 1. The first two principal components
captured 67.53 % of the sample variance. The first principal
component (PC) is strongly and negatively correlated with
both sensory descriptors (vanilla, smokey/grilled, spicy,
sweetness) and volatile compounds (furanic compounds
guaiacol, eugenol and vanillin), whereas it is strongly pos-
itively correlated with ellagitannins, astringency and bit-
terness. Concerning the second principal component, it
represents strongly and negatively the lactones. Apparently
oak chips can easily be discriminated according their
chemical composition and sensory parameters. There seem
to be six groups, namely HT, LT, LT?, UN, N (Noisette)
and S (Special). MT and MT? oak chips seem to have
similar behavior pattern, they show a good correlation with
guaiacol compound and smoky aroma. UN along with LT
and LT? oak chips has a good affinity with ellagitannins
123
744 Eur Food Res Technol (2013) 236:735–746

and both astringency and bitterness. Special oak chips
demonstrate a compatibility with lactones, whereas Noi-
sette oak chips are perceived to have more vanilla and
grilled flavor, and at the same time, they perceived sweeter.
Each sensory descriptor was correlated with the chem-
ical concentration of the oak wood compounds of interest
(Table 1). This procedure allowed us to measure the extent
to which sensory and chemical variables are correlated.
Based on the correlation analysis, it can be observed that
perceived astringency is positively and significantly cor-
related with elagitannins levels (R = 0.93) and negatively
with guaiacol (R = -0.65), methyl guaiacol (R = -0.46)
and furfural (R = -0.47). These are the variables con-
tributing the most to the predictive model of astringency.
When these three variables are used for a multiple linear
regression analysis (Fig. 5), they explained 72.6 % of the
perceptual astringency variance; ellagitannins levels
explained 45 %, guaiacol and methyl guaiacol contents
account 13.20 and 8.86 %, respectively, whereas furfural
levels justified 5.66 % of the total astringency variance
(Table 2). The importance of these variables can be also
seen in the predicted model:
Astringency ¼ 2:17 þ 1:57  ðellagitanninsÞ  2:06
 ðfurfuralÞ  5:37  ðguaiacolÞ þ 6:11
 ðmethyl guaiacolÞ
These results confirm ellagitannins importance in
astringency perception; it intensifies significantly with
ellagitannins concentration. It is also noteworthy that the
above model suggests that volatile compounds like guaia-
col and furfural contents play a relevant role in sensory
astringency, and the highest astringency was perceived for
UN oak wood extracts (4.3) containing 13.72 mg/L of
released ellagic acid, 47.14 lg/L of furfural and 2.46 lg/L
guaiacol.
The overall woody intensity is positively correlated with
guaiacol, methyl guaiacol and furfural contents which is
reasonable since oak wood sensation is complex and
influenced by the presence of various odor-active wood
extractives [18, 36, 37]. The negative correlation with
ellagitannins content may be attributed to the fact that
toasting up to a certain level decreases ellagitannins con-
centration. The perceived intensity of vanilla aroma is

Table 1 Pearson’s correlations between chemical and sensory data

Elagitannins Furfural Methyl Guaiacol Methyl trans-b methyl-c- cis-WL b methyl-c- Eugenol Vanillin
furfural guaiacol octalactone octalactone

Vanilla -0.27 NS 0.39* 0.25 NS 0.76*** 0.88*** -0.04 -0.10 0.40* 0.56**
Woody -0.46** 0.50** 0.29 NS 0.88*** 0.89*** -0.17 -0.26 0.35 0.45**
Spicy -0.01 NS 0.18 0.04 NS 0.26 NS 0.45** 0.02 0.04 0.11 0.28
Sweetness 0.03 NS 0.23 0.10 NS 0.47** 0.63*** -0.35 -0.34 0.06 0.30
Astringency 0.93*** -0.47** -0.25 NS -0.65*** -0.46** -0.06 0.15 -0.25 -0.22
Bitterness 0.35 NS -0.34 -0.33 NS -0.47** -0.54** 0.19 0.19 -0.08 -0.18
NS not significant ([5 %)
*, **, *** Significant at 5, 1 and 0.1 %, respectively

Fig. 5 Prediction of sensory

astringency from chemical
composition

123
Eur Food Res Technol (2013) 236:735–746
Table 2 Predictive model of astringency
Variable Astringency
Sum of squared errors p value
of prediction (SSE)
Ellagitannins 45.00 6.681 3.59e-07***
Furfural 5.66 0.02535*
Guaiacol 13.20 0.00121**
Methyl guaiacol 8.86 0.00510**
Residuals 27.27 8.832 1.90e-09***
*, **, *** Significant at 5, 1 and 0.1 %, respectively
correlated with vanillin, eugenol and furfural concentra-
tions. Thus, vanilla flavor is correlated with vanillin, a
marker of vanilla smell but it is also enhanced by the
presence of other odorous chemicals like eugenol, furfural
and methyl guaiacol. Overall woody aroma is positively
correlated with methyl guaiacol and furfural compounds,
which is logical since these molecules enhance oak woody
aromas. Surprisingly, the spicy flavor is not closely related
to eugenol content (pure eugenol is described as clove
like), but it is correlated with methyl guaiacol, it is likely
that this sensation is more complex and influenced by the
presence of other odor-active wood extractives. Sweetness
and bitterness perception are related to guaiacol com-
pounds, judges characterized samples with important
guaiacol levels sweeter and less bitter; implying that a
strong reduction in bitterness takes place, when samples
have important guaiacol levels. This may also indicate that
judges interpret less bitter the samples that they found
sweeter.
In summary, this work reveals that cooperage oak woods
from different toasting treatments differed in terms of their
principal chemical composition, and these differences were
reflected by perceived sensory differences. The oak chips,
representing different toasting methods (UN, LT, LT?,
MT, MT?, HT, Noisette and Special), were very well
discriminated according to their chemical composition and
sensory assessment. Independent of toasting, a 2-month
time is demanding for extracting the maximum of furfural
and ellagitannins compounds. Additionally to pyrolytic
toasting stage, watering process during toasting influences
significantly oak wood composition. Special extracts more
lactones, less vanillin and guaiacol compounds and at the
same time less ellagitannins.
The correlation analysis evidenced significant correla-
tions between chemical and sensory parameters and pro-
vides some insight into the implication of volatile and
nonvolatile composition on the final quality perception of
astringency. A predictive model between astringency
intensity and ellagitannins, furfural, guaiacol and methyl
guaiacol contents was established.
745
Acknowledgments The authors gratefully thank Dr. Tempère
Sophie for her essential advices in the training of the judges as well as
the judges who participated in the sensory analyses. We also thank
Dr. Warren Albertin for her suggestions in statistical analysis.
Conflict of interest None.
Compliance with Ethics Requirements This article does not
contain any studies with human or animal subjects.
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