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Kurucz 1995
Kurucz 1995
1995
Copyright ‘C 1994 El&er Saence Ltd
Pergamon 0969-806X(94)00075-1 Printed in Great Britain. All rights reserved
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(Rrwirrd 2 July, 1992; crcceptctl 28 December 1992; receiord fir publication 16 May 1994)
Abstract- The Electron Beam Research Facility (EBRF) located in Miami, Florida houses a 1.5 MV,
50 mA electron accelerator. Extensive large scale (460 I min-‘) research on the use of electron beams for
the treatment of water and wastewater has been conducted at this facility over the last several years. Initial
research focused on determining the disinfection kinetics of bacteria in different wastewater streams at
large scale. Our most recent experiments have focused on evaluating the effectiveness of electron beam
irradiation in treating industrial wastes and contaminated groundwaters. The latter has been accomplished
by dissolving toxic organic compounds of interest in large quantities of potable water (groundwater). The
contaminated groundwater simulant is then treated with the electron beam. This paper provides a detailed
description of the EBRF, including equipment and layout, experimental protocols used for the research,
reliability and maintenance performance estimates based on our operational experience, and treatment
cost estimates
299
300 CHAKLt.5 N. KUKW~ L’/ (I/.
then treated with the electron beam. As shown in scale electron beam system can be operated reliably
Table I, removal efficiencies have been determined and maintained with reasonable cost for treating
for various halogenated methanes. ethanes, cthenes either water or wastewater. We have shown that
and propanes. phenols, and polynuclear aromatic electron beam irradiation is efficient and effective for
compounds. Bench scale studies have also shown that destroying toxic organics in aqueous streams of
irradiation may be effective at removing various widely varying quality, and can be a viable treatment
explosives and chemical warfare agents such as TNT. alternative for disinfection of raw sewage (Kurucz
GB and VX. ct trl.. I99 I ). The purpose of this paper is to provide
Disinfection and removal of organic compounds in a detailed description of the EBRF. including equip-
the irradiated waters is primarily due to the for- ment and layout, experimental protocols used for the
mation of electronically excited states, ions and/or research. reliability and maintenance performance
free radicals along the path of incident high energy estimates based on our operational experience. and
electrons. IO ’ s after an electron has passed through treatment cost cstimatcs.
a solution of pure water, the products that are present
arc: F-\C‘II.ITY DESCRIPTION
Radiation Mewing
Water Window
Fig. I. Floor plan of the Electron Beam Research Facihty. Miami. Florida
onto the scanner face which is protected by a sec- Total power consumption, including pumps, chillers
ondary titanium window. The minimum flow is ap- and other auxiliary equipment is about 125 kW. The
proximately 230 I/min (60 gal/min). Below this flow EBRF has been instrumented to continuously moni-
the falling sheet of water tends to become irregular tor and record various operating parameters (voltage,
and ultimately breaks up. In addition to the three current, flow) and estimated absorbed dose. The total
flow streams described above, we have the capacity to absorbed dose is estimated using five high precision
conduct large-scale batch experiments with ground- resistance temperature devices (RTDs) made by Tem-
water simulants and any other source of contami- perature Specialists Inc. The five RTDs are mounted
nated water for which treatability studies are desired in the influent (2 sensors) and effluent (3 sensors)
by connecting 23,000 I (6000 gal) tank trucks to the streams immediately before and after the beam. They
influent pumps. Batch experiments are run at are connected via a Strawberry Tree interface to a
383 I/min (100 gal;min) because of pumping limi- Compaq portable computer which continuously
tations. During experiments to determine the removal reads and records temperatures. The temperature
efficiency of parent compounds and reaction by-prod- difference between influcnt and effluent streams is
ucts. samples are taken in the control room from related to absorbed dose by the fact that a change of
continuously running sample streams prior to and I C is equivalent to I cal gal -’ of absorbed energy in
after irradiation. pure water. and this energy is equivalent to a dose of
approximately 418 krads. Although this relationship
can be altered by the presence of other material in the
PROCESS MONITORING AND ABSORBED DOSE
MEASUREMENT
waste stream. heat losses, and heat defect due to
chemical reactions, observed values have been within
Since the maximum penetration in water is ap- approximately 4% of calculated dose values.
proximately 0.74 cm (0.29”) for I.5 MeV electrons Plots of the various operating parameters and
(see Fig. 3). some electrons pass through the stream estimated dose for a typical experimental run are
and not all of the beam energy is transferred to the presented in Fig. 4. lnfluent and effluent temperature
water. With the addition of over-scanning the waste are shown in part (a). When zero beam current is
stream to insure that the edges of the stream are present the influent and effluent temperatures are
irradiated, more energy is lost with the result that the virtually identical cvcn though the overall tempera-
efficiency of energy transfer is approximately 65%. ture of both the influent and effluent increase or
Thus when the electron beam is operating at 50 mA decrease over time. As beam current is changed the
(75 kW) the waste stream is receiving an average dose effluent temperature increases in proportion to the
of approximately 650 krad. At the designed flowrate dose absorbed by the water. Beam current and the
the water spends at most 0.1 s in front of the beam associated dose estimates obtained from the influ-
thus generating a dose rate of at lcast 6.5 Mrad/s. ent:effluent temperature differences arc shown in part
302 CHARLES N. KIJRUCZ et nl
(b). Since fluctuations in the accelerating voltage and The major activities that took place during the start-
the flow rate of the water affect absorbed dose, these up phase involved the inspection, refurbishment,
parameters are also monitored to explain anomalies testing and conditioning of the electron beam
in estimated dose values. Part (c) shows the drop facility. The following summary of these efforts is
in flowrate from 120 to 100 gal/min as the influent intended to be indicative of the problems which
stream was switched from piped to chlorinated can be encountered in a real application of
secondary wastewater to raw wastewater in a tank electron beam technology to wastewater treatment
truck. The large variation in flowrate after 35 min and to provide the basis for estimated maintenance
was due to air voids as the tank became almost costs.
empty. A facility inspection was conducted by HVE in
February, 1988. The purpose of this effort was to
MAINTENANCE. REPAIRS AND REI.IABII.ITY
“confirm the status of the machine, to identify as
many machine problems as necessary, and to rec-
During the initial phases of our research, a large ommend a course of action, timetable and cost for
effort was required to reactivate the EBRF. Because putting the equipment back into operation.” This was
the system had been left unattended for over two a necessary step given that the equipment had been
years, major repaits were required and approximately sitting idle in the corrosive environment of a sewage
one year passed before experimentation could begin. treatment plant for nearly three years without any
ii.iw
v=2.6 fps l’
Fig. 2. (Iross sectional view of an aqueous waste stream falling over the weir delivery system at 460 l/min
(120 galimin).
The Miami EBRF wastewater treatment application 303
5
al 2.0
Z
6 2.5
._
f 2.0
ZZ 1.5
maintenance. As a result of the inspection the accel- major objective of the reactivation effort was the
erator tube was shipped to HVE for rebuilding and training of project personnel in the maintenance and
the reactivation effort scheduled for summer 1988. In operation.
addition to making the facility fully operational, a The major activities which took place during this
phase included installing the rebuilt accelerator tube,
replacing the vacuum ion pump, installing new pri-
mary and secondary windows, replacing the ICT tank
cover gasket, replacing the voltage stabilizer relay,
removing oil from the SF, gas transfer pipes, in-
stalling an additional gas line filter, overhauling the
g=y--+Jr-J
SF, gas compressor and compressor motor, fixing
major leaks in the gas handling system, adding 20
f bottles of SF, gas, replacing the ion pump PC
board and high voltage meter, repairing the voltage
0 5 10 15 20 25 30 35 40 45
and current ramp and stabilizer boards, restoring
Time (mins)
operation of the 22,000 kg (10,000 lb) steel door to
(b)
200
the ICT tank room, repairing the vault security
180 system lights, switches and interlocks, repairing the
z 700 - Dose - _
%
L
600 -
500 -
I E
120
control room air conditioner,
chiller, voltage regulator
air compressor,
cooling fans and vault
water
x,x’)
Extensive large scale research has been conducted
9,X9
at the EBRF. A total of 69 full days of experimen-
IO 89
11,x9 tation. not counting preparation and set-up, have
been performed. As mentioned previously, the initial
12’8’)
2 ‘90
research focused on disinfection of different waste-
5,‘90 water streams and the effects of electron beam ir-
IO,‘90 radiation on wastewater characteristics. These
I2 90 experiments typically involved filling tank trucks with
I YI cithcr raw or unchlorinated secondary wastewater
drawn from appropriate points in the treatment
?,91
3 Yl plant. and pumping the wastewaters through the
6,Yl electron beam. Subsequent research focused on the
X/91
IO’91
destruction of toxic organics when present as single
compounds in solution or present as mixtures. Water
Mean tlmc be~wecn Fdure\ (MTBF) quality effects were evaluated by injecting toxic or-
MTBF (Major) = 546’10 =X4 6 hour\
MTBF (All) :X46 23 = 36 X hour\ ganics into domestic raw sewage, secondary effluent
MTBF (Maxm~um”) = 3XOOO~10 = 3X00 hours and potable drinking water as they flowed through
,‘4.75 years of operation at X000 hour\ year the influent line. The chemical solutions of known
The Miami EBRF wastewater treatment application 305
concentration were injected under pressure using a The 3% clay concentration level was chosen pri-
Cole-Parmer Master Flex positive displacement in- marily on the basis of cost and the considerable effort
jection pump. Since the secondary effluent and required to obtain higher levels. For example, a
potable water are hard plumbed to the system, these concentration of 3% requires that approximately
experiments were usually carried out at the design 345 kg (760 lb) of clay be added to 11,500 I (3000 gal)
flowrate of 460 l/min (120 gal/min). Injection rates of water. This was accomplished by measuring the
were varied as necessary to obtain desired concen- amount of water after filling a tank truck and adding
trations. the appropriate amount of clay using a fork lift truck.
Our most recent experiments have focused on The clay was kept in suspension by mixing with a
evaluating the effectiveness of electron beam ir- 767 l/min (200 gal/min) gasoline pump.
radiation in treating contaminated groundwaters. The maximum target concentration of 5500 pg I-’
This has been accomplished by dissolving toxic or- was chosen on the basis of preliminary tests to
ganic compounds of interest in large quantities determine the maximum concentration of TCE which
11,50&23,000 I (300&6000 gal) of potable ground- could be produced in a tank truck by adding TCE
water in tank trucks. Thorough mixing is obtained by and mixing overnight (approximately 24 h). The var-
using a combination of three submersible electric ious target concentrations were actually obtained by
pumps and a 767 I/min (200 gal/min) gasoline pump adding TCE at higher concentrations to compensate
to continuously circulate the contents of the tanker. for losses due to volatilization. Calculated concen-
Depending on the solubility of the compounds it is trations of 130, 1300 and 10,000 pg I-’ were used to
sometimes necessary to add chemicals the previous obtain the target levels. Since mixing of clay with the
day. The contaminated groundwater simulant is then 767 l/min (200 gal/min) gasoline pump caused ad-
pumped through 4-6” lines to the electron beam. ditional losses, the pump was run along with the three
recirculating pumps even during 0% clay runs to
ExperimentaI designs generate more consistent concentrations.
The major thrust of our research effort is to Since the pH of our potable water varies in the
estimate the relationships between electron beam range of 8.5-9, the nominal high target value was
dose and the destruction of undesirable compounds selected to be 9. Adding 3% clay to the potable water
(or amount of disinfection) in various waters and lowered the pH to the 6.8-7.5 range, so a middle
wastewaters at large scale. Such information is target value of 7 was used. A pH adjustment using
necessary to determine the minimum dose required to acid was made after the clay was added, if necessary,
obtain a given amount of destruction of selected to bring the value down to 7. If the value was slightly
chemical pollutants. The minimum dose is in turn below 7 no adjustment was made.
required to evaluate the economics of the process in Because of time limitations, especially when pump-
particular treatment applications. ing from tankers. changes in concentration for only
The measured response variable in almost all of 3 electron dose levels and a control of 0 are observed
our experiments is the change in concentration be- for each experimental condition described above. The
tween the flow into and the flow out of the electron order in which the 4 dose levels are set is randomized
beam process, expressed either in absolute units or in order to average out any systematic variation
percent reduction, as required for various analyses. which might be present from variables not being
Since the relationship between change in concen- specifically controlled. The 3 nonzero dose levels are
tration and electron dose for a given compound can obtained by setting beam current at appropriate
be affected by water quality, initial concentration of values. The IS treatment combinations in the TCE
chemical, and the presence or absence of other com- example were run in random order to average out the
pounds or substances (e.g. various solids such as effects of uncontrolled for Factors which might vary
clay), these are usually considered as independent from day to day. Whenever resources allow. most of
variables in experiments and the existence of their our experiments arc replicated at least once in their
effect determined. entirety. In this example, 2 replicates would require
As an example, consider a recent experiment on that 2 x IX = 36 individual experiments bc made for
TCE destruction designed to examine the effects of a particular compound.
pH, the presence of clay and initial concentration of The data collection and analysis effort is generally
TCE. This experiment was conducted at three target quite extensive. For the present example. a total of I8
concentrations (100. 1000 and 5500 pg I ’ ), three pH (experimental conditions) x 2 (replications) x 4
values (5, 7 and 9) and two clay concentrations (0 and (doses) x 2 (influcnt and effluent samples) = 288
3% by weight). These values were chosen on the basis samples would be processed. Since 4 determinations
of objectives of the experiment, the practical limi- are usually made on each sample. a total of
tations imposed by full scale experimentation and the 4 x 288 = II52 analyses would be performed.
characteristics of available groundwater (drinking Samples have been analyzed at the Florida Inter-
water). There are a total of 3 (initial concen- national University Drinking Water Research Center
trations) x 3 (pH values) x 2 (clay present or and the University of Miami Laboratories for
not) = 18 experimental conditions. Pollution Control Technologies.
306 CHARLES N. Ku~ucz et ul.
The effects of factors such as electron dose, water time before erratic flow occurs is usually about
quality and concentration, are analyzed using analy- 25 min.
sis of variance. Nonlinear regression analysis is used After the runs for the day are completed, operating
to fit curves relating change in concentrations to parameters and time data, which have been logged
electron dose for each treatment combination found into a computer file during the experiments, is pro-
to differ in the analysis of variance. The formal cessed along with the information on the experiment
experimental designs generally fall into the random- sheet. The data file is edited and plots of pertinent
ized block or split plot design categories. Similar operating parameters (e.g. Fig. 4) are prepared and
analyses are sometimes performed for reaction by- examined for anomalies which may affect the results
products if measured as part of a particular exper- or which may reveal problems with the treatment
imental effort. In addition, analyses of variance are system. Finally, the times on the experiment sheet are
sometimes run on the inflow concentrations of natu- used to estimate when each effluent sample water
rally occurring independent variables to determine passed through the beam. The data file is then
how the input streams vary in quality. searched to determine the doses that were actually
being delivered at those times. The results are
recorded for subsequent matching to the destruction
Data collection
or disinfection data determined from analysis of each
The large scale experiments performed at the influent/effluent sample pair.
EBRF are a team effort requiring at least five people
Experimental rrsults
to accomplish. Two people collect influent and efflu-
ent samples, one person operates the electron beam, Again, the removal percentages for most organic
one person operates the computer and one person compounds that we have investigated to date are
performs measurements of various water quality par- summarized in Table 1. Although experiments were
ameters such as pH and dissolved oxygen. In many run with varying water qualities and initial conccn-
experiments additional people are utilized to fill trations, doses of 5OG800 krads effectively removed
tankers, add chemicals and switch hoses and lines most of the compounds studied. To date we have not
between feed streams. Typically, five to eight people identified significant quantities of reaction by-prod-
will be present at the facility when experiments are ucts (e.g. sub-PM concentrations of aldehydes) when
being run. destruction of the parent compound is near complete.
During an experiment the beam operator is respon- When complete destruction does occur the com-
sible for ensuring proper performance of the beam pounds are reduced to CO,, Hz0 and salts. By-
and for changing beam current as necessary to obtain product studies have been undertaken, howcvcr, by
the planned doses. The computer operator monitors intentionally utilizing lower doses (Nickclsen, 1992).
the system operating parameters and verbally indi-
cates when influent and effluent samples arc to be TREATMENT COSTS
drawn and when beam current is to be changed. Dye
studies have been performed to estimate the transit The cost of treatment using electron beam technol-
time of water between the influent sample point, the ogy depends on many factors such as the dose
point at which the water flows over the weir and the required to obtain the desired destruction. the volume
effluent sample points. At a flow of 383 I/min of waste to be treated. the size of the treatment
(100 gal/min), the effluent samples arc drawn ap- facility, the time utilization of the facility and the
proximately 60 s after the influent samples to obtain manner in which capital recovery is handled. Fat
a “matched” set of unirradiatcd and irradiated example, the estimated current cost of the EBRF. a
samples. It is necessary to take repeated influent permanent full scale I.5 MeV treatment facility. is
samples because of variation in concentrations that $2,350 M which results from an approximate 5%
occur when working with the large scale, high flow annual inflation of the total price actually paid for the
system. Both the influent and effluent sampling points Miami facility (Kurucz ct c/l.. 1990). Note that this
are in the control room as indicated in Fig. I. estimate includes the building(s) necessary to house
Before each run an experiment sheet is filled out by the treatment system. Operating and maintenance
the computer operator. Along with filling in descrip- costs are estimated to bc $41/h. Howcvcr. no indirect
tive information, the order of doses is randomized costs such as supervision. overhead. etc. arc included.
using a random number generator and recorded on The estimated maintenance costs arc consistent with
the form. Once the experiment begins, the times at our experience described earlier.
which samples are drawn and the times at which Amortization period and intcrcst rate assumptions
selected beam currents are reached are recorded. can significantly affect hourly capital charges. as can
Influent samples are taken no sooner than 2 min after the number of operating hours per year. flow rate and
a desired beam current is obtained in order to let the required operator time. The current ucir delivery
system approach equilibrium before taking the corre- system can be operated over a range of flow rates
sponding effluent sample. The timing becomes critical from 230-610 Ihmin (6G160 ga/min). Since the maxi-
in tanker experiments where the available pumping mum absorbed dose delivcrcd by the clcctron beam
The Miami EBRF wastewater treatment application 307
beam irradiation. Chem. Prof. L)n'iron. Pro~. VIII hit. of wastewater: a revicv.. Pr¢~. 8th 5[vnlp. ]|'lisle'Writer
Conj. Lublin, Poland. Treatment, p. 191. Montreal.
Levaillant C. and Gallien C. L. (1979) Sanitation methods Trump J. O. 11980) High energy electron radiation of
using high energy electron beams. Radiat. Phys. Chem. 14, wastewater liquid residuals. Final report to U.S. National
309. Science Foundation. MIT, Cambridge, MA.
Nickelsen M. G., Cooper W. J., Kurucz ('. N. and Waitc Waile T. D., Kurucz C. N., Cooper W. J., Narbaitz
T. D. (1992) Remowd of benzene and selected alkyl R. N. and Greenfield J, H. (19891 Disinfection of
substituted benzcnes from aqueou,, solutions utilizing wastewater ellluents with electron radiation. In t'r~,c. ,tin.
continuous high energy cleclron irradiation. J. ISttth'on. Soc. Cir. En,g. ,Vat. ('~m/: Eratroll. k.)l,l~., p. 619
Sei. Teehnol. 26, I44. Austin, TX
Pikaev A. K. and Shubin V. N. (19841 Radiation treatment Waite T. D., Cooper W. J., Kurucz C. N., Narbailz R. and
of liquid wastes. Radial. Ph3.~. ('hem. 24, 77. Greenlleld J. (1991} Full scale lreaDllenl of ,aastewater
Singh A., Sagert N. H., Borsa J.. Singh H. and Beianett G. S. clttuent with high energy elcctrtms. ('hem. Prt,t. ti)triron.
(1985) The use of high-energy radiation for lhe treatment 24, 563.