Food

Chemistry
Food Chemistry 92 (2005) 337–342
www.elsevier.com/locate/foodchem

Study of ultrasonic wave treatments for accelerating the

aging process in a rice alcoholic beverage
Audrey Chingzu Chang *

Department of Food Science, National Ilan University, 1, Section I, Shun Lung Road, Ilan City 260, Taiwan

Received 7 March 2003; received in revised form 28 July 2004; accepted 28 July 2004

Abstract

This research focussed on the accelerated aging of a rice alcoholic beverage by applying two different levels of ultrasonic power.
The rice alcoholic beverage was fermented with Saccharomyces sake. The control treatment was aged for one year in fired clay con-
tainers (standard aging) while two other treatments simulated aging by using 20 kHz and 1.6 MHz ultrasonic waves, respectively
(accelerated aging). Comparisons were made of alcohol content, titratable acidity value, gas chromatography measurements of vol-
atile aroma compounds, sensory evaluation and time of aging. Results showed that the 20 kHz treatment influences rice alcoholic
beverage aging better than the 1.6 MHz treatment. The 20 kHz ultrasonic wave treatment has potential as a good alternative method
for aging the alcoholic beverage. Further studies are needed to elucidate the best power range of ultrasonic waves for aging alcoholic
beverages made of various materials.
Ó 2004 Elsevier Ltd. All rights reserved.

Keywords: Rice alcoholic beverage; 1.6 MHz and 20 kHz Ultrasonic waves; Aging

1. Introduction techniques (Chang, 2003; Chang & Chen, 2002; Cocito,

Gaetano, & Delfini, 1995; Ho, Hogg, & Silva, 1999;
Moderate consumption of alcoholic beverages plays a Huang, 1987; Maduagwu, 1982; Masuda, Yamamota,
role in life, inducing a mild euphoria and increasing lon- & Asakura, 1985; Simpson & Miller, 1983). There have
gevity. Alcoholic beverages can be made from various been studies of alcoholic beverages aging using different
materials, using several processes. Alcoholic beverage chemical methods (Castellari, Matricardi, Arfelli, &
making, however, takes time, for fermenting and for Amati, 2000; Huang, 1980; Jan & Hsu, 1984; Mad-
aging. Fermenting produces alcohol, flavor, and taste; uagwu, 1982), but very little work was found (and/or
aging improves the sensory properties that make alco- was not written in English) dealing with accelerating
holic beverages pleasurable (Sato, 1984). Alcoholic bev- alcoholic beverage aging by applying physical methods.
erages usually have many flavors and other properties There is a lack of verifiable data in this field. Therefore,
which each play a subtle, intertwined, yet important role a research study of ultrasonic wave treatments for
in the tastes that humans prefer. Much research is pub- reducing the time of the aging process is an important
lished on the flavors, physical properties, chemical prop- new contribution to the field.
erties and constituents of alcoholic beverages made from In an ultrasonic wave process, high temperature and
various materials using different processes and aging high pressure can be generated from circulated ultra-
sonic waves, causing chemical polymers to be broken
into numerous mist particles (subparticles) and then
*
Fax: +886 3 5724176. recombined. In a review of sonoelectroanalysis, Saterlay
E-mail address: czchang@niu.edu.tw. and Compton (2000) concluded that ultrasonic

0308-8146/$ - see front matter Ó 2004 Elsevier Ltd. All rights reserved.
doi:10.1016/j.foodchem.2004.07.027
338 A.C. Chang / Food Chemistry 92 (2005) 337–342

equipment, working in the range of 20–100 kHz, is rela- 2. Materials and methods
tively inexpensive, readily available and is an enabling
technology for electroanalysis. Lindley and Mason 2.1. General
(1987) reported the types of ultrasound which are used
in chemistry for effecting chemical reactivity, which were In this research, there were two ultrasonic wave aging
broadly divided in power between 20 and 100 kHz. They treatments, one conventional aging group and one un-
concluded that chemists are interested in ultrasound aged (untreated) group. The two ultrasonic wave treat-
power because it provides a form of energy for the mod- ments on rice alcoholic beverages were: 20 kHz
ification of chemical reactivity which is different from ultrasonic wave-treated, and 1.6 MHz ultrasonic wave-
those normally used, such as heat, light and pressure. treated. The conventionally aged group was aged for
Furthermore, they indicated that ultrasound power pro- one year.
duces its effects via cavitation bubbles. These bubbles
are generated during the rarefaction cycle of the wave 2.2. Sample preparation of rice alcoholic beverage for
when the liquid structure is literally torn apart to form ultrasonic wave treatments, for one year conventionally
microbubbles which collapse in the compression cycle. aged treatment and for unaged treatment
Lindley and Mason (1987) further noted that pressures
of hundreds of atmospheres and temperatures of thou- All the rice alcoholic beverage was made with a 1:1
sands of degrees are generated during the collapse of ratio (by volume) of whole dry grain rice (Taiwanese
the bubbles. Aroma extraction (Cocito et al., 1995), cell PonLai, 14% water, dry basis) and water. Four litres
growth and ester formation (Matsuura, Hirotsune, of a 1:1 rice/water mixture were cooked at 125 °C for
Nunokawa, Satoh, & Honda, 1994), associated with about 1 h and cooled to room temperature (25 °C).
ultrasound treatment, have been previously studied. When this cooked rice was cooled to room temperature,
We hypothesized that the high temperature and high four extra litres of water (pre-boiled and cooled to room
pressure generated from circulated ultrasonic waves temperature) were added and mixed well into the rice to
might help speed up the aging process and give more fla- liquefy the rice. This process was repeated 9 times in our
vor and/or taste to wine. By applying this physical accel- experiment for accelerating the aging process and was
eration aging method using ultrasonic waves, aging repeated 3 times for the conventional aging process.
would be fulfilled within a shortened time and space Aspergillus awamori (CCRC 30891) was then inoculated
would be saved as well. Our paper reports the effects into the rice in order to produce amyloglucosidase,
of different powers (20 kHz and 1.6 MHz) of ultrasonic glucoamylase, a-amylase, and b-glucuronidase to break
wave treatments on rice alcoholic beverage aging. The down the starch polymers into smaller starch oligo-
power range of 20 kHz, selected, was based on previ- carbohydrate polymers and sugar monomers and also
ously published data (Lindley & Mason, 1987; Saterlay to liquefy the rice for further yet more complete, fermen-
& Compton, 2000) and a 1.6 MHz treatment as an addi- tation. About 1 h later, with the temperature remaining
tional variant with higher energy. We also hypothesized around 25 °C, Saccharomyces sake (CCRC 20262) was
that ultrasound treatments by a power higher than 20 inoculated into the liquefied rice and kept at 25 °C for
kHz would shorten the process of aging alcoholic bever- fermentation. The fermentation took place in six closed
age more than a lower power. Rice was chosen because fired clay containers; three of the six were 30 l containers
it is relatively inexpensive, rich in starch (essential for for the accelerated aging process and the other three
alcohol fermentation techniques) and has fewer complex were 10 l containers for the conventional one year aging
flavors and other properties than alcoholic beverages process, which were vibrated 2–3 times a day. After the
made from other materials which would complicate fermentation was completed (14–16 days, depending on
experimental analysis. In addition to sonication, rice the alcohol content, 18–20% alcohol in our experiment),
alcoholic beverage was also aged for one year in fired the rice alcoholic beverage was collected using the 80 °C
clay containers as the comparative standard aging method distillation method and was ready for the ultrasonic
or control. In this study, the length of time used for the wave treatments of the accelerated aging process or for
standard aging method was set at one year because one the one year standard aging process.
year is the aging time for the market product of grain
alcoholic beverage. In Asia, most grain alcoholic bever- 2.3. Additional sample preparation of one year conven-
ages sold in the market are conventionally aged only for tionally aged rice alcoholic beverage
one year (or less). This study should indicate whether
the ultrasonic waves aging process has potential to pro- The standard, or conventionally aged, rice alcoholic
duce an alcoholic beverage from rice comparable in beverage was aged by placing it in three 3-l fired clay
quality to a conventionally aged alcoholic beverage containers for one year prior to conducting the acceler-
from rice and whether a higher power is better than a ated aging. An aging time of one year is the standard for
lower power in accelerating aging. conventional aging of Asian market grain alcoholic
 A.C. Chang / Food Chemistry 92 (2005) 337–342 339

beverages, and analysis at that aging time was done. evaporation), 1, 2, 3, and 4 treatments (repetitions) for
About one year later, the alcoholic beverage to be aged the 1.6 MHz level of ultrasonic waves.
by accelerated methods, was aged by the two ultrasonic
processes. Analysis was done immediately after the 2.5. Tests
accelerated aging processes was completed.
2.5.1. Types of tests
2.4. Accelerated aging process for the 20 kHz and 1.6 Each sample was analyzed for alcohol content, titrat-
MHz ultrasonic wave treatments able acidity, gas chromatography measurements of vol-
atile aroma compounds, sensory evaluation and the time
The accelerated-aged rice alcoholic beverage was of aging. Each of the experimental treatments was repli-
aged about one year after the standard aging rice alco- cated 3 times (e.g. three one year-aged alcoholic bever-
holic beverage, so that analysis of the conventionally age samples were obtained from three different
aged alcoholic beverage and accelerated-aged alcoholic containers) for analysis, and the results were the aver-
beverage could take place concurrently. Moreover, the ages of the three samples.
rice alcoholic beverage-making techniques for both con-
ventional standard aging and accelerated aging, were as 2.5.2. Titratable acidity
close to exactly the same as possible for all tested sam- The titratable acidity was represented as acetic acid
ples in our study in order to produce similar rice alco- due to its domination in the rice alcoholic beverage.
holic beverage sample quality and to minimize bias. The titratable acidity was measured by the AOAC
Analysis of the untreated rice alcoholic beverage (for (1995) from the 1 N NaOH used. The titratable acidities
accelerating aging process) was done immediately after of rice alcoholic beverage (fresh, immediately after dis-
the fermentations were completed, for which the rice tillation, for the accelerating aging process), one year
alcoholic beverage samples were collected by using the conventionally aged rice alcoholic beverage (similar to
80 °C distillation method. This test was used as a check the market aging technique) and each sample of all
index of the start quality of the two different aging proc- accelerated aging treatments (repetitions) were meas-
esses to assure the same quality level at commencement. ured. This gave an indication of acidity and the level
Both the 20 kHz and 1.6 MHz ultrasonic wave setups of sour taste of the alcoholic beverage; it was also an in-
were designed and self-made by a Professor of the dex of possible contamination throughout the entire
Mechanical Engineering Department in our school. study.
20 kHz and 1.6 MHz ultrasonic waves generators were
used to apply ultrasound energy to the rice alcoholic 2.5.3. Alcohol content
beverage. The two ultrasonic wave generators both Alcohol was measured by a KYOTO, DA-310, elec-
had piezoelectric chips, which generated electrons. tric specific gravity meter. Untreated rice alcoholic
When the electrons accumulated they vibrated in terms beverage (fresh, immediately after distillation, for accel-
of ultrasonic waves. The ultrasonic nozzle orifice for erating aging process), one year conventionally aged rice
20 kHz was 10 mm while that for 1.6 MHz was 4 mm. alcoholic beverage (similar to the market aging tech-
We chose 10 and 4 mm orifice nozzle because these noz- nique) and each sample of all accelerated aging treat-
zle amplitude energies were found, by trial, to fit our ments (repetitions) were measured. Alcohol was then
experimental needs in terms of atomizing the bulk alco- calculated from the gravity measurements by the AOAC
holic beverage liquids into a spray of smoke-like mist method (1995). The alcohol content check gave an indi-
droplets to fulfill the ultrasonic process. The rice alco- cation of possible alcohol loss in the process.
holic beverage volume for one ultrasonic treatment
run was 2 l and was triplicated. All the ultrasonic aging 2.5.4. Gas chromatography measurements of volatile
treatments were at 25 °C and were in a closed chamber aroma compounds
to prevent evaporation loss of the rice alcoholic bever- Flavor compounds were analyzed by a WHIRL-
age and to assure the best collection of the misted rice POOL 5790 gas chromatograph with a glass column
alcoholic beverage. The rice alcoholic beverage was that was 1.8 m long, 2 mm thick, packed with 6.6% car-
repeatedly treated, up to 16 times, for the 20 kHz proc- bowax and 20 M/80–120 mesh carbopack B Aw using a
ess and up to 4 times for the 1.6 MHz ultrasonic wave flame ionization detector (FID). The carrier gas was
process. The whole processing time of each was consid- nitrogen with 20 ml/min flow rate. The injection temper-
ered as the time of aging and was used for comparison ature was 150 °C and the FID temperature was 200 °C.
to conventional aging. Samples of the treated rice alco- The gas chromatograph temperature gradient started at
holic beverage were collected after 0 (untreated, immedi- 60 °C and remained at that level for 1 min. It then in-
ately after evaporation), 4, 8, 12, and 16 treatments creased at 5 °C/min and reached 160 °C in 20 min where
(repetitions) for the 20 kHz level of ultrasonic waves it stayed for 2 min. Each sample injection was 2 ll.
and were collected after 0 (untreated, immediately after Standards for the gas chromatograph were prepared as
340 A.C. Chang / Food Chemistry 92 (2005) 337–342

follows: 0.5 ml of 5.14% acetaldehyde, 0.4 ml of 5.01% evaluators (Table 3). The titratable acidity in 1.6 MHz
methanol, 2 ml of 5.0% ethyl acetate, 0.2 ml of 5% ultrasonic wave-treated rice alcoholic beverage re-
1-propanol, 0.4 ml of 5% 2-methyl-1-propanol, and 1 mained the same as that of the untreated rice alcoholic
ml of 2% 2,3,dimethyl-butanol were mixed with 40% beverage as the number of treatments (repetitions) in-
ethanol to reach 100 ml in total. creased (Table 2). The titratable acidity check of all
studied samples also showed that it was in the normal
2.5.5. Sensory evaluation range of rice alcoholic beverage, which indicated the
Sensory evaluations were done by 12 qualified and right fermentation process and no contamination in
experienced alcoholic beverage sensory tasters using our work over this entire study.
the Krammer preference priority organoleptic method
which has a statistical significance of a = 5% and had 3.2. Alcohol content
been applied widely for the purpose of alcoholic bever-
age tasting (Huang, 1984; Sato, 1988; Wang, 1980; Zhai, The alcohol content in the rice alcoholic beverage
2000). Each of the 12 tasters tasted the rice alcoholic aged with 20 kHz and 1.6 MHz ultrasonic waves de-
beverage before any treatments (repetitions) and after creased as treatment time increased, resulting in less
each of the 4 (for 1.6 MHz) and each of the 16 (for 20 burning flavor (Tables 1 and 2). The alcohol content
kHz) accelerated aging treatments (repetitions). The (52%) of the samples treated 16 times by 20 kHz ultra-
tasters ranked the treated rice alcoholic beverage against sonic waves was a little lower than the alcohol content
the rice alcoholic beverage conventionally aged for one (54%) of samples aged by the standard one-year process.
year. They gave the treated rice alcoholic beverage a The alcohol content (45%) of the samples treated 4 times
ranking of 1 (best) to 9 (worst). Generally, a quality con- by 1.6 MHz ultrasonic waves was much lower than the
ventionally aged rice alcoholic beverage would be alcohol content (52%) of the samples treated (repeated)
ranked 1 on this scale. The results were then calculated 16 times by 20 kHz ultrasonic waves and the alcohol
and analyzed from the preference priorities of each ta- content (54%) of samples aged by the standard one-year
ster and ranked from best to worst flavor. process. The large quantity of alcohol lost in the rice
alcoholic beverage aged by 1.6 MHz ultrasonic waves
2.5.6. Time of aging may be a problem.
Time of aging for the alcoholic beverages aged by the
accelerated process was counted as the time needed to 3.3. Gas chromatography measurements of volatile aroma
complete the whole ultrasonic waves aging process vs. compounds
the one year conventional aging process.
The gas chromatography analyses of volatile aroma
compounds showed that the evaporating flavor com-
3. Results and discussion pounds generally decreased slightly as the number of
20 kHz ultrasonic waves process treatments (repetitions)
3.1. Titratable acidity volume increased, but decreased to a lower level as the number
of 1.6 MHz ultrasonic waves process treatments (repeti-
The titratable acidity value in 20 kHz ultrasonic tions) increased (Tables 1 and 2). Acetaldehyde has the
wave-treated rice alcoholic beverage decreased slightly lowest boiling point of rice alcoholic beverage flavor
as the number of treatments increased, thus giving a less compounds and has an unpleasant offensive flavor.
sour taste (Table 1) and was preferred by the sensory Thus, by decreasing the amount of acetaldehyde of 20

Table 1
The titratable acidity, alcohol content, acetaldehyde content, ethyl acetate content, and alcohol contents and standard deviations of 20 kHz
ultrasonic wave-treated rice alcoholic beverage with different repetitions vs. one year conventionally aged rice alcoholic beverage, and fresh rice
alcoholic beverage (untreated)
Number of accelerated Titratable Alcohol (%) Acetaldehyde Ethyl Alcohols
aging repetitions acidity (mg/l) acetate
Methanol 1-Propanol 2,3- 2-Methyl-
(g/100 ml) (mg/l) (mg/l) (mg/l) Dimethyl-butanol 1-propanol
(mg/l) (mg/l)
0 (untreated) 0.012 56 ± 0.47 106 ± 12 103 ± 15 58 ± 3 161 ± 8 1130 ± 170 368 ± 27
4 0.011 54 ± 0.41 98 ± 11 104 ± 14 58 ± 3 155 ± 8 1088 ± 180 361 ± 23
8 0.011 53 ± 0.40 89 ± 13 105 ± 13 57 ± 3 150 ± 7 1019 ± 180 355 ± 25
12 0.010 53 ± 0.38 80 ± 9 109 ± 13 55 ± 2.5 147 ± 7 975 ± 176 344 ± 26
16 0.010 52 ± 0.53 70 ± 11 113 ± 13 54 ± 3 144 ± 7 913 ± 154 331 ± 22
One year conventionally 0.010 54 ± 0.41 90 ± 7 115 ± 11 54 ± 3 154 ± 6 933 ± 126 355 ± 24
aged rice alcoholic beverage
 A.C. Chang / Food Chemistry 92 (2005) 337–342 341

Table 2
The titratable acidity, alcohol content, acetaldehyde content, ethyl acetate content, and other alcohol contents and standard deviation of 1.6 MHz
ultrasonic wave-treated rice alcoholic beverage with different repetitions vs. one year conventionally aged rice alcoholic beverage and fresh rice
alcoholic beverage (untreated)
Number of accelerated Titratable Alcohol (%) Acetaldehyde Ethyl acetate Alcohols
aging treatments acidity (mg/l) (mg/l)
Methanol 1-Propanol 2,3-Dimethyl- 2-Methyl-1-
(g/100 ml) (mg/l) (mg/l) butanol propanol
(mg/l) (mg/l)
0 (untreated) 0.012 56 ± 0.47 106 ± 12 103 ± 15 58 ± 3 161 ± 8 1130 ± 170 368 ± 27
1 0.012 50 ± 0.61 88 ± 11 107 ± 14 54 ± 4 155 ± 9 1114 ± 187 358 ± 35
2 0.012 47 ± 0.78 77 ± 13 118 ± 14 51 ± 5 150 ± 8 1069 ± 176 350 ± 38
3 0.012 45 ± 0.56 65 ± 12 130 ± 12 50 ± 4 146 ± 9 1035 ± 190 344 ± 32
4 0.012 45 ± 0.44 54 ± 11 134 ± 12 50 ± 4 142 ± 9 990 ± 160 340 ± 35
One year conventionally 0.010 54 ± 0.41 90 ± 7 115 ± 11 54 ± 3 154 ± 6 933 ± 126 355 ± 24
aged rice alcoholic beverage

Table 3
The results of sensory evaluation of ultrasonic wave treatments of rice alcoholic beverage vs. one year conventionally aged rice alcoholic beverage
and fresh rice alcoholic beverage (untreated); the smaller the preference number, the better the sensory evaluation
Untreated Ultrasonic waves treatments One year aged
20 kHz 1.6 MHz 20 kHz 1.6 MHz 20 kHz 1.6 MHz 20 kHz 1.6 MHz
4 times 1 time 8 times 2 times 12 times 3 times 16 times 4 times
Rank Summation of all 108 93 15 44 40 26 62 12 84 12
tasters
Preference 9 8 2 5 4 3 6 1 7 1

kHz ultrasonic wave-treated rice alcoholic beverage, taste smoother and less greasy in the mouth (Table 3).
other pleasant flavor compounds became more promi- When the polyol contents decreased to a lesser extent
nent and made the 20 kHz ultrasonic wave-treated rice with the number of 1.6 MHz ultrasonic wave treatments
alcoholic beverage taste better (Tables 1 and 3). But, (repetitions), in combination with the prominent in-
by decreasing the amount of acetaldehyde of the rice crease of the ethyl acetate and prominent decrease of
alcoholic beverage further than that 20 kHz ultrasonic the acetaldehyde, the rice alcoholic beverage tasted
wave-treated rice alcoholic beverage, both pleasant spicy, tart, and unsmooth in the mouth (Table 2). The
and unpleasant flavor compounds became more promi- acceptability decreased as the treatments (repetitions)
nent which made the 1.6 MHz ultrasonic wave-treated increased (Table 3).
rice alcoholic beverage have a more complicated taste
(Tables 2 and 3). Ethyl acetate, which is one of the fra- 3.4. Sensory evaluation
grant compounds in the alcoholic beverage, slightly in-
creased in 20 kHz ultrasonic wave-treated rice Human preference for certain alcoholic beverages is
alcoholic beverage but increased to a much higher level mostly based on odour, taste and tactile properties.
in the 1.6 MHz ultrasonic wave-treated rice alcoholic Some are not detectable by gas chromatography analy-
beverage (Tables 1 and 2), and thus made the 1.6 sis and thus human sensory evaluations are needed. Re-
MHz ultrasonic wave-treated rice alcoholic beverage sults of sensory evaluations showed that the taste of the
smell (not taste) much more fragrant than the 20 kHz 20 kHz ultrasonic wave-treated rice alcoholic beverage
ultrasonic wave-treated rice alcoholic beverage. The improved as the number of treatments (repetitions) in-
high alcohols (polyhydric alcohols) such as 1-propanol, creased (Table 3); while the taste of the 1.6 MHz ultra-
2-methyl-1-propanol, 2,3-dimethyl-butanol and metha- sonic wave-treated rice alcoholic beverage grew
nol, often have rice-oil flavors and cause a greasy feel progressively worse as the number of treatments (repeti-
in the mouth. When the levels of these decreased with tions) increased (Table 3). The rice alcoholic beverage
the number of 20 kHz ultrasonic wave treatments (rep- treated 16 times by 20 kHz ultrasonic waves had a taste
etitions), combined with the decreased unpleasant acet- equivalent to conventional one year-aged rice alcoholic
aldehyde (Table 1), the ethyl acetate contribution to beverage (Table 3) while the rice alcoholic beverage that
the taste was increased in the 20 kHz accelerated aging had one treatment by 1.6 MHz ultrasonic wave was
rice alcoholic beverage and made the alcoholic beverage rated nearly as good as the conventionally aged rice
342 A.C. Chang / Food Chemistry 92 (2005) 337–342

alcoholic beverage, though it was rated progressively tural Engineering of Texas A&M University, USA, for
worse as the number of treatments (repetitions) in- their help with this manuscript.
creased (Table 3). The rice alcoholic beverage that was
treated 4 times by 1.6 MHz ultrasonic waves had a taste
less preferred than the rice alcoholic beverage that was
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