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Abstract—Hybrid gas–liquid electrical discharge has been in- conventional oxidants and disinfectants [3]. However, the en-
vestigated in recent years as an innovative technology for conta- ergy consumption of the electrical discharges generated in wa-
minated water treatment. A high-voltage pulsed-power supply is ter is many times higher than that generated in gas. Techniques
commonly needed for the generation of electrical discharges. This
paper aims, in lieu of cost effectiveness, to evaluate the degradation of direct discharges in close proximity to water surfaces are
efficiency of electrical discharges with an alternating-current (ac) therefore being rapidly developed and tested on the industrial
power since it is generally cheaper than a pulsed one. An ac power scale for water and wastewater treatments [4], for example the
supply with a fixed voltage of 13 kV and a fixed frequency of hybrid gas–liquid electrical discharges. Locke’s research team
60 Hz is therefore adopted in this paper for the inactivation of [3] developed a hybrid gas–liquid electrical-discharge reactor
aquatic microorganism. The energies required for one log order
of reduction of E. coli, S. aureus, and Yeast were 23, 34, and 31 J/ml, so that the electrical discharges took place in close proximity
respectively. The energy efficiencies achieved with an ac power in to water surfaces, i.e., just above the water level, to ensure that
this paper are comparable with other studies that achieved with a the chemically active species generated can get into the water
pulsed-power. easily and then to inactivate the microorganisms.
Index Terms—Biological treatment, disinfection, environmenta- High-voltage pulsed-power supplies are widely used for
ladaptation ability, mutation, nonthermal plasma (NTP), waste- the generation of electrical discharges, and high degradation
water treatment. efficiencies can be achieved. However, a high-voltage pulsed-
power supply is more expensive compared with an alternating
I. I NTRODUCTION current (ac) one. In lieu of cost effectiveness, this paper aims to
evaluate the degradation efficiency of electrical discharges by
Fig. 2. Illustration of the electrical-discharge reactors with (a) needle and (b) brush electrodes.
Fig. 6. Time variation of pH with the brush-plate electrode discharge (: with
discharge and : without discharge).
C. Influence of pH
Fig. 6 shows the change of pH of liquid (from 7.2 to 3.4)
during the electric discharges. Many factors could lead to the
decrease of pH. For instance, H2 O2 generated in air or liquid
could lead to the formation of H3 O+ ions in liquid phase,
consequentially decreasing the pH. Parts of H3 O+ ions might
be formed through the electron and ion bombardments to the
Fig. 4. Voltage waveforms with two different electrodes (needle and brush). water surface [14]. The other possibility for decreasing pH
might result from NO− −
3 and NO2 ions by dissolution of HNO2
and HNO3 , which were easily formed during the discharges in
the gas of nitrogen/oxygen/steam mixture.
E. coli is neutrophile and suitable living in pH = 5 − 7.
Low pH might harm them by disrupting the plasma membrane
or inhibiting the activity of enzymes and membrane transport
proteins. Therefore, it is difficult to distinguish whether the
bacterial was killed by plasma discharges directly or by an acid
environment indirectly.
In order to better understand how the pH value affects the
disinfection efficiency, the plasma was turned off, and the
inactivation of E. coli was tested in acid solutions with pH = 3
adjusted by either HNO3 or HCl. The D values achieved with
Fig. 5. Influence of the brush-plate electrode discharge on the inactivation of HNO3 and HCl solutions were 177 and 240 min, respectively
three microorganisms (: E. coli, : S. aureus, and : Yeast). (Fig. 7), which were one order of magnitude higher compared
218 IEEE TRANSACTIONS ON PLASMA SCIENCE, VOL. 36, NO. 1, FEBRUARY 2008
Fig. 7. Kill rate of E. coli in pure water and in two acid solutions without different sequences to migrate at different positions in the gel.
discharge (: HCl, : HNO3 , and : pure water with discharge). This provides the information necessary to distinguish between
the mutated- and wild-type sequences without prior knowledge
of what these sequences are, justifying why this method is
used to detect mutations within closely related organisms. The
DGGE is a rapid and efficient separation technique of same
length DNA sequences (amplified by PCR), which may vary
as little as a single base pair modification [15]. The DGGE
results of E. coli are shown in Fig. 9. Each lane represents a 16S
amplified product migrating to a unique position in the gel. The
16s rDNA fragments were in different positions before and after
the discharges. That means the mutation or the DNA damage
might take place during the electrical discharges. For example,
UV or H2 O2 , formed in plasmas, might damage the DNA and
result in the death, mutation, or carcinogenesis of cells [16].
The aforementioned fact can be further proved by the ex-
perimental test of the environmental-adaptation ability. The
environmental adaptation of E. coli to the electrical discharges
was tested by ten-time recycle experimental tests. An average D
Fig. 8. Kill rate of E. coli with two kinds of buffer solutions and pure water
with the brush-plate electrode discharge (: phosphate buffer, : carbonate value of 44 ± 31 min was achieved in retreatment tests, which
buffer, and : pure water). is ∼360% higher than the D value (12 min) obtained in the first
test. In other words, the kill rate of E. coli was greatly reduced
with the D value achieved with plasma discharges (12 min,
after a ten-time retreatment under the electrical discharges.
Fig. 5). As a result, the pH should not be a key factor for
In short, the DGGE results indicate that mutation of
inactivation.
microorganism could take place in the electrical discharges.
To further understand the pH effect, a series of experiments
Microorganisms could be consequentially with stronger
was tested under buffer solutions. All pH values almost re-
environmental-adaptation ability and might result in a lower
mained unchanged after 60-min plasma discharges. Thus, the
inactivation rate (higher D value). If the phenomenon is true,
pH effect on inactivation can be excluded. Fig. 8 shows that
in a long-term viewpoint, it will affect the inactivation appli-
the D values were 299 and 209 min when the phosphate and
cation of the electrical discharges. Further studies are deemed
carbonate buffer solutions were added, respectively. In other
necessary to elucidate this issue.
words, the inactivation efficiency was seriously inhibited by
buffers. It is speculated that great parts of chemically active
species might react with the carbonate/phosphate or their elec- IV. C ONCLUSION
trolytes and, thus, reduce the kill rate.
The brush electrode achieves a higher energy efficiency than
the needle one for the disinfection process. The energy efficien-
D. Mutation of E. coli in Electrical-Discharge Environment
cies achieved with ac power in this paper are compared with the
In the DGGE, any variation of DNA sequences within these other studies with pulsed-power. Hence, this paper successfully
domains results in different melting temperatures, thus causing shows that the ac discharges can achieve high disinfection
CHEN et al.: INACTIVATION OF AQUATIC MICROORGANISMS BY LOW-FREQUENCY AC DISCHARGES 219
efficiency by reasonable energy consumption. However, the [15] D. Ercolini, “PCR-DGGE fingerprinting: Novel strategies for detection of
mutation and the low pH need to be further concerned. microbes in food,” J. Microbiol. Methods, vol. 56, no. 3, pp. 297–314,
Mar. 2004.
[16] K. P. Talaro and A. Talaro, Foundations in Microbiology Basic Principles,
R EFERENCES 4th ed. New York: McGraw-Hill, 2002, p. 273.
[1] M. A. Malik, A. Ghaffar, and S. A. Malik, “Water purification by electri-
cal discharges,” Plasma Source Sci. Technol., vol. 10, no. 1, pp. 82–91,
Feb. 2001.
[2] B. Sun, M. Sato, and J. S. Clement, “Use of a pulsed high-voltage dis-
charge for removal of organic compounds in aqueous solution,” J. Phys. Chih Wei Chen is currently working toward the
D, Appl. Phys., vol. 32, no. 15, pp. 1908–1915, Aug. 1999. Ph.D. degree in the Graduate Institute of Envi-
[3] D. R. Grymonpre, W. C. Finney, R. J. Clark, and B. R. Locke, “Hybrid ronmental Engineering, National Central University,
gas–liquid electrical discharge reactors for organic compound degrada- Chung-Li, Taiwan, R.O.C.
tion,” Ind. Eng. Chem. Res., vol. 43, no. 9, pp. 1975–1989, 2004. Since 1999, he has been a Lecturer with the
[4] M. Sato, B. Sun, T. Ohshima, and Y. Sagi, “Characteristics of active Department of Biochemical Engineering, Hwa Hsia
species and removal of organic compound by a pulsed corona discharge Institute of Technology, Chung-Ho, Taiwan.
in water,” J. Adv. Oxid. Technol., vol. 4, no. 3, pp. 339–342, 1999.
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vol. 1, no. 16, Sep. 2001.
[6] A. Abou-Ghazala, S. Katsuki, K. H. Schoenbach, F. C. Dobbs, and
K. R. Moreira, “Bacterial decontamination of water by means of
pulsed-corona discharges,” IEEE Trans. Plasma Sci., vol. 30, no. 4,
pp. 1449–1453, Aug. 2002. How-Ming Lee was born in Kaohsiung, Taiwan,
[7] C. Wouter, A. Fiala, E. Bosch, and L. M. Creyghton, “Couple electrical- R.O.C., in 1971. He received the B.Sc. degree
fluid model of pulsed electric field treatment in a model food system,” in environmental science and/or engineering from
Innovative Food Sci. Emerging Technol., vol. 2, no. 4, pp. 229–238, Tunghai University, Taiwan, in 1994, and the M.S.
Dec. 2001. and Ph.D. degrees in environmental science and/or
[8] B. Qin, U. R. Pothakamury, H. Vega, O. Martin, G. V. Barbosa-Cánovas, engineering from the National Central University,
and B. G. Swanson, “Food pasteurization using high intensity pulsed Chung-Li, Taiwan, in 1996, and 2000, respectively.
electric fields,” J. Food Technol., vol. 49, no. 12, pp. 55–60, 1994. From 2001 to November 2005, he was a Postdoc-
[9] Q. H. Zhang, F. J. Chang, and G. V. Barbosa-Cánovas, “Inactivation of toral Researcher with the National Central Univer-
microorganisms in a semisolid model food using high voltage pulsed sity. He is currently a Researcher with the Physics
electric fields,” Lebensm. Wiss. Technol., vol. 27, no. 6, pp. 538–543, Division, Institute of Nuclear Energy Research,
Dec. 1994. Taoyuan, Taiwan. Currently, he is developing a novel plasma-assisted gasifier
[10] M. Pilar, L. Barsotti, and J. C. Cheftel, “Microbial inactivation by pulsed to the conversion of biomass into syngas. His research interests cover all
electric fields in a batch treatment chamber: effects of some electrical pa- environmental plasma applications, particularly in air pollution controls. He
rameters and food constituents,” Innovative Food Sci. Emerging Technol., also devotes into simulation and modeling of plasma chemistry as well as
vol. 2, no. 4, pp. 239–249, Dec. 2001. thermal/nonthermal plasma processes.
[11] L. Picart, E. Dumay, and J. C. Cheftel, “Inactivation of Listeria innocua in
dairy fluids by pulsed electric fields: Influence of electric parameters and
food composition,” Innovative Food Sci. Emerging Technol., vol. 3, no. 4,
pp. 357–369, Dec. 2002.
[12] B. Qin, G. V. Barbosa-Cánovas, G. Swanson, P. Pedrow, and R. Olsen,
Moo Been Chang received the Ph.D. degree in envi-
“Inactivating microorganisms using a pulsed electric field continuous
ronmental engineering from the University of Illinois
treatment system,” IEEE Trans. Ind. Appl., vol. 34, no. 1, pp. 43–50,
at Urbana–Champaign, Urbana, in 1991.
Jan./Feb. 1998.
He is a Professor with the Graduate Institute of
[13] M. A. Malik, Y. Minamitani, S. Xiao, J. F. Kolb, and K. H. Schoenbach,
Environmental Engineering, National Central Uni-
“Comparison of E. coli decontamination in water between coaxial elec-
versity, Chung-Li, Taiwan, R.O.C.
trodes in presence and absence of dielectric pellet,” in Proc. ISNTPT-4,
Panama City Beach, FL, 2004.
[14] R. Burlica, M. J. Kirkpatrick, and B. R. Locke, “Formation of reac-
tive species in gliding arc discharges,” J. Electrostat., vol. 64, no. 1,
pp. 35–43, Jan. 2006.