1098 IEEE TRANSACTIONS ON INDUSTRY APPLICATIONS, VOL. 49, NO.
3, MAY/JUNE 2013
Effects of the Voltage and Current Waveforms and
Discharge Power on Hydrogen Peroxide Formation
in Water-Spray Gliding Arc Reactors
Radu Burlica, Member, IEEE, Wright C. Finney, and Bruce R. Locke, Senior Member, IEEE
Abstract—This paper deals with the effects of discharge power
and voltage and current waveforms on the formation of hydrogen
peroxide (H2 O2 ) from liquid water sprayed as a fine aerosol
into a plasma formed by a gliding arc discharge. The formation
rates of H2 O2 were determined for different values of the power
injected into the reactor (1–7 W), as well as for different means of
applying the power [pulsed, alternating current (ac), and direct
current (dc)], with argon carrier. For the same power injected
into the plasma, the pulsed power was more efficient than the ac
power which was, in turn, more effective than the dc power for the
generation of H2 O2 . Energy yield increased with water flow up to
10 mL/min and thereafter was constant with a maximum of about
6 g/kWh.
Index Terms—Atmospheric-pressure plasmas, chemical reac-
tors, hydrogen peroxide, liquid water, plasma devices, power
supplies.
I. I NTRODUCTION
T HE COMBINATION and interaction of nonthermal
plasma technologies (e.g., direct current (dc) corona,
pulsed corona, gliding arc, and dielectric barrier discharges)
with liquid water are of great interest for a variety of ap-
plications, including the destruction of various pollutants and
the synthesis of various compounds [1]–[5]. While gas-phase
nonthermal plasma with water vapor [6]–[8] has been studied
(particularly for H2 generation), the combination of low-power
pulsed gliding arc plasma with water aerosol droplets has been
shown to be highly efficient for H2 and H2 O2 generation [9]–
[11]. A key feature of the gliding arc discharge is that the
flowing gas stabilizes the discharge that forms between two
knife edge electrodes [6], [12].
Hydrogen is commonly produced from the reforming of
natural gas, methanol, and gasoline via catalytic conversion
Manuscript received June 23, 2011; revised January 13, 2012, May 7, 2012,
and July 17, 2012; accepted August 8, 2012. Date of publication March 15,
2013; date of current version May 15, 2013. Paper 2011-EPC-260.R3, pre-
sented at the 2011 IEEE Industry Applications Society Annual Meeting,
Orlando, FL, USA, October 9–13, and approved for publication in the IEEE
T RANSACTIONS ON I NDUSTRY A PPLICATIONS by the Electrostatic Processes
Committee of the IEEE Industry Applications Society. This work was sup-
ported by the National Science Foundation under Grant CBET-0932481.
R. Burlica is with the Department of Electrical Engineering, “Gh. Asachi”
Technical University of Iasi, 700050 Iasi, Romania (e-mail: rburlica@ee.
tuiasi.ro).
W. C. Finney and B. R. Locke are with the Department of Chemical
and Biomedical Engineering, Florida Agricultural and Mechanical University
(FAMU)–Florida State University (FSU), College of Engineering, Tallahassee,
FL 32310-6046 USA (e-mail: finney@eng.fsu.edu; locke@eng.fsu.edu).
Digital Object Identifier 10.1109/TIA.2013.2253080
0093-9994/$31.00 © 2013 IEEE
[13], and nonthermal plasma technologies have been demon-
strated to effectively produce H2 from a variety of organic
compounds [14], [15]. The generation of H2 O2 from water is
of interest for chemical and biological applications [9], [16].
Simultaneous production of both of these species may also be
of interest in promoting chemical reactions with heterogeneous
catalysts [17].
Nonthermal plasma generates highly energetic species (e.g.,
electrons, ions, radicals, excited species, and molecules) in the
gas phase at ambient temperature and atmospheric pressure.
Direct and indirect interactions of the plasma-generated species
with water molecules lead to the formation of OH (and other)
radicals and ultimately to molecular products such as H2 O2 ,
H2 , O2 , and nitrates (nitrates in the case when air or nitrogen is
used as the carrier gas) [1]–[5], [7], [9].
The efficiency of chemical production in gliding arc re-
actors with water spray has been shown to be dependent
upon the gas composition and the delivered power, and it
is possibly dependent upon the water aerosol particle size
[10], [11], [18]–[20]. Previous works with alternating cur-
rent (ac) power utilized comparatively much higher power
(400–500 W) [18], [19] than was utilized in previous works
with pulsed power at low power (ca. 300 mW) [10], [11]. At
very high power (400–500 W), all the water is vaporized, and
thermal effects and reactions become important [6], [20]. In the
cases with lower power (below 10 W), the water droplets do
not significantly vaporize within the reactor (i.e., the measured
value of the temperature at the outlet of the reactor does not
exceed 30 ◦ C), and it is conjectured that these condensed water
droplets enhance the energy yield for H2 O2 due to suppression
of radical quenching reactions [9]. Since previous works with
the different ac and pulsed power supplies were not conducted
under the same discharge power, it is therefore necessary to
make a comparison of these two methods (as well as dc) of
power delivery at the same power.
The present work focuses on H2 O2 formation from water
spray exposed to plasma generated by a gliding arc with argon
carrier gas for different voltage waveforms, electrical discharge
power levels, and power injection modes (ac, dc, and pulsed)
and for different water flow rates.
II. E XPERIMENT
The gliding arc reactor is the same as that previously reported
[10], [11], and briefly, it utilizes two stainless steel divergent
electrodes attached to a ceramic support placed between two
BURLICA et al.: EFFECTS OF THE VOLTAGE AND CURRENT WAVEFORMS AND DISCHARGE POWER 1099

Fig. 1. Pulsed gliding arc reactor configuration. (P) Pump, (Rsh) shunt resistor
(100 Ω), (OSC) oscilloscope, (HEI) high-efficiency ignition coil, (IGBT)
switch transistor, and (HVP) high-voltage probe (1/1000). Fig. 2. Voltage and current waveforms for the pulsed discharge.

rectangular glass sheets leading to confined plasma in a narrow

chamber. In the first experimental setup, a pulsed power supply
as shown in Fig. 1 was utilized. The pulsed high voltage is pro-
duced by a high-efficiency ignition coil made for automobiles
and driven by a pulse generator with pulsewidth and frequency
control. The power is controlled by variation of the pulse
frequency. Examples of the voltage and current waveforms for
this power supply are given in Fig. 2.
In the second experimental setup (Fig. 3), the electrodes are
connected to an ac power supply (7 kV/50 mA/60 Hz), utilizing
an ac high-voltage transformer with a magnetic shunt. The
voltage is controlled by a variable transformer (TR-VAR), and
the current is controlled by a variable power resistor (VAR).
Examples of the voltage and current waveforms for this power
supply are shown in Fig. 4. The dc power supply used for the
experiments was a Hipotronics 30-kV/5-mA system.
Deionized water is sprayed directly into the plasma formed
between the electrodes through an injection nozzle equipped
with one port for the gas injection and one port for the liquid,
attached to a Swagelok tee (1/16 in) (see Fig. 1). The water
droplets are carried with the gas flow through the outlet port of
Fig. 3. AC—Experimental setup. (P) Pump, (SH) shunt, (OSC) oscilloscope,
the nozzle and are atomized by the high velocity of the carrier (TRA) ac high-voltage transformer, (VAR) variable resistor, (TR-VAR) variable
gas. The very small exit diameter of the nozzle (∅ = 0.15 mm) transformer, and (HVP) high-voltage probe.
leads to a high exit velocity of the gas and a high droplet density
formation in the axial flow, thereby increasing the stability of A gas cylinder was connected to the straight port of the
the discharge while reducing the consumption of the carrier gas Swagelok tee, providing gas flow through the inner tube of the
(Qg = 2 L/min) compared with the system used in the previous nozzle, and the water was delivered by a high-pressure injection
study [10]. pump through the perpendicular port of the tee.
1100 IEEE TRANSACTIONS ON INDUSTRY APPLICATIONS, VOL. 49, NO. 3, MAY/JUNE 2013
Fig. 4. Voltage and current waveforms of the ac discharge.
In both cases, the input energy is not sufficient to vaporize
the water droplets. The temperature of the treated water was
also measured at the outlet of the reactor and was found, at
most, to be 5 ◦ C–10 ◦ C higher than the initial ambient water
temperature injected into the reactor, depending on the power
of the discharge. The electrical discharge forms at the minimum
distance between the electrodes and “glides” along their edges
in a gas containing the very fine droplets of water to be treated
(approximately 25 μm). In the present study, the gas flow
(argon) rate Qg is approximately 2 L/min, and the water flow
rate Qw varies for different experimental situations between 4
and 20 mL/min.
The power of the ac discharge was about 6 W for a cur-
rent of approximately 5 mA. Measurements of H2 O2 were
conducted for different values of the electrical power injected
into the discharge (approximately 1–6 W) and water flow rates
(4–20 mL/min). The liquid-phase water is collected in a glass
vessel at the bottom of the reactor after passing through the
plasma, and the gas is directed to another sampling vessel.
The H2 O2 formed in the liquid phase is measured us-
ing a colorimetric test with a PerkinElmer Lambda 3A UV
spectrophotometer [21]. The voltage and current waveforms
of the discharge were measured with a Tektronix DPO3014
oscilloscope. The power was calculated from averages of five
measurements of the voltage and the current. The sampling rate
of the oscilloscope was 104 points for the acquisition window.
The discharge voltage was measured with a high-voltage probe
(Tektronix; 1/1000) connected to the electrodes. The current
Fig. 5. Hydrogen peroxide concentrations for different types of applied power
and water flow rates for 2.8-W discharge power.
Fig. 6. Hydrogen peroxide concentration versus discharge power for Qw =
4 mL/min.
was measured on a shunt to the ground of 10 Ω in the secondary
of the ignition coil of the ac high-voltage transformer.
Three repeated measurements for H2 O2 were taken after
5 min of reactor operation for each water flow rate from 4, 6,
10, 15, to 20 mL/min. The averages of the three repeated values
are reported.
The H2 O2 energy yield is calculated by
m(H2 O2 )MH2 O2 3.6
EER(H2 O2 ) = [g/kWh] (1)
P
where m(H2 O2 ) is the hydrogen peroxide production rate (in
micromoles per second), MH2 O2 is the hydrogen peroxide
molecular mass (in grams per mole), and P is the power (in
watts).
III. R ESULTS AND D ISCUSSION
As in previous work [11], the H2 O2 concentration decreases
with increasing liquid flow rate; however, as shown in Fig. 5, the
pulsed discharge shows significantly higher concentrations than
either the ac or dc discharge. The H2 O2 concentration generally
increases with power as shown in Fig. 6, again with the highest
concentration for the pulsed power followed by the ac power
and then the dc power.
BURLICA et al.: EFFECTS OF THE VOLTAGE AND CURRENT WAVEFORMS AND DISCHARGE POWER
Fig. 7. Hydrogen peroxide production energy yield with water flow rates for
the pulsed, ac, and dc discharges for 2.6–2.8 W.
H2 O2 may form in plasma through OH radical recombina-
tion by
OH + OH → H2 O2 .
Reactions between hydrogen peroxide and OH radicals can
also occur, leading to H2 O2 destruction and water formation
through reaction
H2 O2 + OH → HO2 + H2 O.
The highest concentration of hydrogen peroxide, about
1.5 mM for the pulsed power supply (4-mL/min water flow
rate), is likely due to the fact that the low-power pulsed
discharge requires less energy, therefore leading to lower gas
and liquid temperatures and rapid quenching of the plasma.
The rapid quenching may reduce degradation of H2 O2 due to
the reaction with OH radicals [reaction (3)] or other reactive
species from gas phase.
Fig. 7 shows the effects of water flow rate on the hydrogen
peroxide energy production yield. The highest energy efficiency
for hydrogen peroxide production was obtained for the pulsed
power supply. The effect of water flow rate was more pro-
nounced with the pulsed power supply, particularly in the range
of 4–8 mL/min, while with the dc power supply, there was
almost no effect of water flow rate. The hydrogen peroxide
efficiency increases with the water flow rate up to 6 g/kWh
for the pulsed discharge, 3.5 g/kWh for the ac case, and about
1.2 g/kWh for the dc discharge.
As shown in Fig. 8, the maximum H2 O2 energy yield occurs
at about 1 W for the pulsed discharge and for 4-mL/min fixed
water flow rate. It can be noted that the H2 O2 energy yields
at 1 W are considerably lower than those previously reported
for the case of 300 mW [11]. While it is expected that the
higher power, and therefore the higher local temperature, may
lead to degradation reactions that lower the efficiency [9], [20],
the significantly lower H2 O2 energy yield in the present study
compared to that in the previous study (50–80 g/kWh), at input
power near 300 mW, suggests some other aspects that may be
different in the present reactor.
1101
Fig. 8. Hydrogen peroxide production energy yield with power for pulsed, ac,
and dc discharges (Qw = 4 mL/min).
(2)
(3)
Fig. 9. Effect of water flow rate on the discharge power in the cases of pulsed
and ac deliveries for P = 2.8 W.
Fig. 9 shows that there is no significant effect of water flow
rate on the discharge power for either the pulsed or ac power
supply. At high water flow rates, the dc discharge is fully
quenched.
For a fixed power of about 3 W, the water flow rates do not
have a significant influence on the power of the discharge in
both pulsed and ac gliding arc reactors. This may be due to the
fact that the reactive species in the plasma are generated in the
gas phase by electron collisions with gaseous species. Under
medium to low concentrations, the water droplets are therefore
less important for such gas-phase reactions. If the water droplet
concentration in the plasma zone is very high (for water flow
rates above 20 mL/min), the ionization process of the gas is
diminished, and the discharge decreases in intensity and finally
is extinguished at high-enough water flow.
Fig. 10 shows the influence of the gas flow rate on the
electrical discharge with the electrical parameters f = 200 Hz
and duty cycle = 40% (for the pulsed discharge).
In contrast to the liquid flow rate, the gas flow rate affects the
power injected into the discharge. The variation of the power
shows a maximum for 2-L/min Ar gas flow rate in the case
1102
Fig. 10. Effects of gas flow rate on discharge power for the pulsed and ac
discharges.
of the pulsed power supply. For higher gas flow rates, more
electrical charges are carried out with the gas (the equivalent
resistance decreases), and the power starts to decrease. That can
be due to the fact that the nominal power of the coil used to
generate pulses is much lower than the nominal power of the
ac and dc power supplies and therefore has a fast-drop output
characteristic. Therefore, the coil is working in an overloaded
regime and cannot provide the energy required by the electrical
conditions of the reactor. The higher capability in the electrical
power of the ac transformer is able to maintain a constant power
of 2 W even for high gas flow rates.
The experiments presented earlier show that the energy pro-
duction yield of hydrogen peroxide is higher with the pulsed
power discharge than with the ac and dc power injection modes.
We currently do not have a detailed comprehensive explanation
for this effect, and modeling of the reactor is under way to
address this issue. Nevertheless, dc discharges in the reactor are
unlikely to produce large spatial gradients and do not produce
temporal gradients in the plasma properties. It is known that
large gradients in space [20] and in time [7] can lead to
more efficient plasma production of stable species, including
hydrogen peroxide. Rapid quenching of the plasma prevents
degradation reactions by plasma-generated species, e.g., OH
radicals by reaction (3). Clearly, the pulsed discharge leads to
sharper temporal gradients in the plasma than the ac discharge
as shown in the current waveforms in Figs. 2 and 4, and this
may partially account for the higher efficiency of production by
the pulsed discharge.
In addition to the temporal gradients, the liquid droplets
are distinct from the surrounding plasma phase. Therefore,
there may be spatial gradients between the plasma and the
condensed liquid which assist in the suppression of quenching
reactions near and on the liquid droplet. The OH radicals can
be generated by electron collisions with water molecules in
the vapor phase or directly with water molecules at the liquid
surface. Since the gas phase is likely very close to saturation
with water vapor, it may be more likely that the collisions
between water and plasma electrons occur in the gas phase to
produce OH radicals in the gas phase. Nevertheless, quantum
IEEE TRANSACTIONS ON INDUSTRY APPLICATIONS, VOL. 49, NO. 3, MAY/JUNE 2013
chemical calculations using density function theory suggest
that OH radicals (which can be formed in the gas phase or at
the gas–liquid interface) form caged structures by hydrogen
bonding to water molecules in aerosols and water clusters
[22]. The capture of the highly soluble hydrogen peroxide into
the liquid droplets can thus further protect the peroxide from
reactions in the gas phase that may lead to degradation and
lower efficiency.
IV. C ONCLUSION
The production of H2 O2 in gliding arc reactors with water
spray significantly depends on the water flow rate injected
into the plasma, the power of the discharge, and the mode
of discharge (pulsed, ac, or dc). The energy yields for H2 O2
production are dependent on power. The energy yield of H2 O2
is two times higher for the pulsed voltage power supply than for
the ac case at a power between 1 and 3 W.
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Radu Burlica (M’11) received the Ph.D. degree in
electrical machines, electrical apparatus, and actua-
tors from the “Gh. Asachi” Technical University of
Iasi, Iasi, Romania.
He was involved in postdoctoral studies in the field
of management of the environment, legislation, and
waste at the Ecole des Mines d’Ales, Ales, France,
and was a NATO/NSF Postdoctoral Research Fellow
with Florida State University, Tallahassee, FL, USA,
during 2002–2003. He is currently an Associate Pro-
fessor with the Department of Electrical Engineer-
ing, “Gh. Asachi” Technical University of Iasi. He has research interest in
gliding arc electrical discharges for pollution control.
1103
Wright C. Finney received the B.S. degree in
physics and the M.S. degree in biology from Florida
State University (FSU), Tallahassee, FL, USA, in
1975 and 1978, respectively.
He is currently a Research Associate with the
Department of Chemical and Biomedical Engineer-
ing, College of Engineering (COE), Florida Agri-
cultural and Mechanical University (FAMU)–FSU,
Tallahassee, FL, USA, where, prior to joining COE,
FAMU–FSU, he was with the Aerosol Physics Re-
search Group, Department of Physics, from 1978 to
1992. There, he codeveloped several aerosol and gas treatment techniques, such
as an electron beam particle precharger for enhanced electrostatic precipita-
tion and a pulsed-streamer-corona reactor for high-efficiency SO2 and NOx
removal. In addition to his research, he is involved in the development of new
undergraduate and graduate academic initiatives in the department. His general
research interests include environmental engineering, electrostatic processes,
aerosol science, and biomedical engineering. One of his continuing current
interests lies in the area of using a nonthermal plasma technology known
as pulsed streamer corona for the treatment and breakdown of airborne and
groundwater-containing organic contaminants.
Bruce R. Locke (M’99–SM’08) received the B.S.
degree in chemical engineering and environmental
and water resources engineering from Vanderbilt
University, Nashville, TN, USA, the M.S. degree
in chemical engineering from the University of
Houston, Houston, TX, USA, and the Ph.D. degree
from North Carolina State University, Raleigh, NC,
USA.
He is Associate Vice President for Academic
Affairs at Florida State University (FSU),
Tallahassee, FL, USA, and a Professor with the
Department of Chemical and Biomedical Engineering, Florida Agricultural
and Mechanical University (FAMU)–Florida State University (FSU), College
of Engineering, Tallahassee, FL, USA. He is also a Distinguished University
Research Professor with FSU. He has published over 120 peer-reviewed journal
papers. His research interests include the development and analysis of electrical
discharge plasma reactors for initiating chemical reactions in air and water
pollution control, green chemistry, and disinfection. He also studies networks
of chemical reactions coupled with diffusion and convection in bioreactors,
tissue engineering, and other bioengineering applications.
Dr. Locke is a member of the American Institute of Chemical Engineers and
the American Chemical Society.