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Nuclear Instruments and Methods in Physics ResearchB 113 (1996) 81-87

NOMB

Beam Interactions with Materials 8 Atoms

EISEVIER

 

Review of industrial applications of electron accelerators

 
 

R. Mehnert

 
 

Institutfir

Oberfliichenmodijzierung,

Permoserstr.

15, D-04303 Leipzig, Germany

 

Abstract

Electron

beam

applications

are based

on different

physical

action

principles:

generation

of strong

local heating

(electron

beam treatment), Coulomb interaction with electrons in inorganic and organic materials generating molecular excitation and ionization (chemical processing) or defects (semiconductor treatment), and bremsstrahlung generation (materials inspection).

Mainly for research applications (pulse radiolysis, free electron laser) pulsed electron accelerators are used. The wide field of

electron

beam

applications

is covered

by four accelerator

“families”:

electron

- sources

(30-150

keV)

with

internal

scanned

beam,

- gap low-energy

single

electron

accelerators

(100-300

keV),

- transformer-

or Cockroft-Walton-type

electron

accelerators

(300-4500

keV),

- electron

linear

accelerators

(l-10

MeV).

As application

examples,

the curing

of coatings,

electron

beam

degradation

of chlorinated

hydrocarbons

in air and electron

beam

curing

of fiber-reinforced

composites

are discussed

in more

detail.

1. A survey

of industrial

applications

of electron

beams

accelerators

are presently

used for industrial

EBC

applica-

 

tions.

When

electrons

with

typical

energies

in the

keV

and

In

a

similar

way,

degradation

of

pollutants

in

air

or

MeV range are absorbed in matter, secondary electrons are

water

can

be initiated

by electrons.

Electron

energies

be-

produced as a result of the energy degradation

process. By

tween

150 and

500

keV

are

sufficient

to ensure

electron

Coulomb interaction of these electrons with the atoms or

penetration

between

0.1

and

1.5

m

in

air.

For

technical

molecules of the absorber, finally ions, thermalized elec-

applications

electron-induced

chain

reactions

play

an im-

trons, excited

states

and radicals

are formed.

portant

role. Mineralization

of chlorinated

hydrocarbons

in

Radiation

chemical

processing

of monomers

and poly-

air

is

one

example

of

such

an

energy

efficient

electron

mers such as polymerization of monomer/oligomer sys-

beam

process.

A

chlorine

radical

stimulated

oxidation

tems, crosslinking, grafting and degradation of polymers is

chain

reaction

is

the

main

mechanism

leading

to

the

based on the generation of chemically reactive species.

mineralization

products

HCl,

Cl,,

CO

and

CO,.

It was

Crosslinking occurs when two radicals produced on neigh-

shown

that

no

hazardous

radiolysis

products

are

formed

boring polymer units recombine. The relative molecular

during

the

irradiation

process

[6].

Irradiation

with

fast

mass increases and the melting point rises. Crosslinking of

electrons

offers

a universal

method

to degrade

also

many

polyethylene

cable

insulators

is most

widely

applied.

But

other

air

pollutants

such

as

aromatics,

ethers

and

even

also the production of polymer foams, shrink tubes

and

dioxines

and furanes.

Considerable

efforts

are also made

to

foils

is industrialized

since

many

However,

the

most

important

years

[ 1,2].

application

of fast

elec-

demonstrate

tion

of

the

the technical

electron

beam

feasibility

and economical

dry

scrubbing

process

opera-

for

flue

trons with typical energies between 120 and 300 keV is the

gases

[7-91.

 

curing of solvent-free monomer/oligomer coatings, var-

Waste

water

treatment

makes

use

of

the

electron-in-

nishes,

paints

and printing

inks.

 

duced

formation

of

reactive

species

in

water:

solvated

Electron

beam

curing

(EBC)

is defined

as: “the

use of

electrons,

OH

and

H radicals.

Reactions

of

these

species

electron

beams

as

an

energy

source

to

induce

a

rapid

with

water

pollutants

can

lead

to products

which

are less

conversion

of especially

formulated

100% reactive

liquids

harmful

or

easily

removable

by

filtration.

In

order

to

to solids”. Initiation by fast electrons leads

to radical

or

penetrate

water

layers

of

at least

a few

millimeters,

elec-

cationic polymerization followed by intensive crosslinking.

tron

energies

above

500

keV

are

needed.

After

a longer

Dense polymer networks exhibiting excellent abrasive,

period

of laboratory

studies,

severe

efforts

are now

made

scratch and chemical resistance are produced in such a

to

reduce

the

high

investment

and

operational

costs,

to

way [3-51. Worldwide more than 350 low-energy electron

understand

the

complex

radiolysis

processes

induced

in

0168-583X/96/$15.00

0

1996 Elsevier Science B.V. All rights reserved

 

SSDI 0168-583X(95)01344-X

II. ELECTRON ACCELERATORS

mixed pollutant solutions and to better control the degrada- T h e r e a

mixed

pollutant

solutions

and to better

control

the degrada-

There

are numerous

research

applications

of

stationary

tion

procedure.

However,

waste

water

treatment

using

and pulsed

electron

beams

which

are related

to present

or

82

R. Mehnrrt/Nucl.

Instr.

und Meth.

in Phys.

Res.

B 113

(19961

81-87

electron

beams

is still experimental

[lo].

future

applications

of the electron

beam technology.

Electron-induced

defect

formation

in

doped

silicon

Micro-, nano- and picosecond pulses of MeV electrons

semiconductors

is an industrial

application

which

is based

are an excellent tool in chemical reaction kinetics. These

on

both

the

formation

of

atomic

displacements

in

the

short electron pulses can be used to initiate chemical

lattice

and

the

electrostatic

interaction

of

fast

electrons.

reactions. Time-resolved optical absorption and emission

Homogeneously

distributed

defects

are generated,

e.g.,

in

spectroscopy, conductivity measurements and electron spin

silicon

power

switching

devices

allowing

the

fine-tuning

resonance are useful detection methods which give infor-

of switching

times

[ 1l].

mation about the nature of short-lived intermediates, their

During

stopping

of

fast

electrons

in

matter

a

few

reactions and kinetics. Pulse radiolysis is now used to

percent

of their

energy

is transfotmed

to bremsstrahlung.

 

study chemical

reaction

in

a time

interval

from

10-r’

to

The total mass

stopping

power

of electrons

consists

of the

10 s

[14].

mass

collision

and the radiative

stopping

power.

The latter

Nanosecond

electron

pulses

with

beam

currents

of

lo2

determines

the amount

of bremsstrahlung

which

is gener-

to IO4 A are used for laser pumping, microwave generation

ated

within

the

absorber.

Bremsstrahlung

conversion

of

and plasma heating.

electrons

is effective

for absorbers

with

large atomic

num-

Picosecond electron pulses from high-quality electron

bers

and electron

energies

above

5 MeV.

It

is often

used

beams are excellent sources for free electron laser excita-

for materials

inspection,

but also for sterilization

and food

tion.

irradiation

[ 121.

 

In Fig.

1 an attempt

is made

to schematically

summa-

 

From

the point

of view

of radiation

damage,

ionization

rize the most important industrial applications of electron

and

excitation

effects

are

important

for

gases,

liquids,

accelerators.

organic

solids,

polymers,

semiconductors,

ionic crystals

 

etc.

but

not

for

metals

[13].

Low-energy

electrons

with

typical

energies

of

a few

ten

to

150 keV

are not

able

to

2. Electron

accelerators

used

in industry

induce

atomic

displacements

within

the

crystallites.

The

electron

energy

is

transformed

to

heat.

Electron

beam

On a industrial

scale,

accelerators

are used

to generate

power

densities

up

to

IO6 W cm-*

can be obtained

from

electrons

with

energies

between

0.1 and

10 MeV.

windowless

electron

sources,

leading

to immediate

melting

The

lower

limit

of

the

electron

energy

is

due

to

the

of

the

metal.

The

large

field

of

electron

beam welding,

energy absorption

within

the

exit

window

foil.

This

foil

melting,

hardening,

film

deposition

and

defect

annealing

forms

the

interface

which

separates

the

vacuum

of

the

make

use

of

the

controlled

heat

generation

by

electron

acceleration

vessel

from

the outer

atmosphere.

For techni-

beams.

 

cal

applications

a

minimum

current

density

of

0.1

mA

Industrial

Applications

of Electron

Accelerators

1 m A Industrial Applications of Electron Accelerators e-beamtreatment polymer modification of metals

e-beamtreatment

polymer modification

of metals

(chemicalprocessing)

- cross-linking

- grafling

- degradation

(lithography

degradation of

pollutants

-wastewater

e g r a d a t i o n o f pollutants -waste water other

other applications

electron beam

“curing” of

I

- monomer/oligomer

systems

- composites

research applications (related to technology)

-

-

-fusion

-

pulse radiolysis

laser pumping

research

FEL

-

-

-

-

materials inspection sterilization “fine- tuning” of semicondudors food and feed irradiation

Fig.

I. Industrial

applications

of electron

accelerators.

Table 1 Low-energy electron accelerators used in industry Manufacturer, Model   Cathode

Table

1

Low-energy

electron

accelerators

used

in industry

Manufacturer,

Model

 

Cathode

Electron

Beam

Maximum

Remarks

 

configuration

energy

power

beam

width

 

(kW)

(keV)

(ml

Energy

Sciences

 

linear

cathode

150-300

2.3

up to 4 cathode systems

Electrocurtain

Inc. (ESI), USA head

 

per accelerator

Electrocure

 

multicathode

 

200

used in printing

Radiation

Polymer

Co. (RPC),

USA

multicathode with 2 grids

150-300

200

2.3

Broad

Beam

Dual

multicathode

300

980

2.3

consists

of

2

 

accelerators

Polymer

Physik

(PP),

Germany

needle

cathode

150-280

loo

2.0

2 cathodes

Scanner

possible

LEA

linear cathode

grid

120-250

60

1.0

used chiefly

 

in

with no control

 

printing industry

N&in-High

Voltage

Co. (NHV),

Japan

linear

cathode

150-300

200

1.0

Scanner

needle

cathode

300-500

65

1.2

Messer

Griesheim,

Germany

 

segmented

cathode

< 150

12

1.5

R. Mehnert /Nucl.

Instr. and Meth. in Phys. Res. B 113 (1996) 81-87

83

EBOGEN

MEC,

Germany

several

linear

< 120

 

cathodes

cm-*

window

area

is

required.

However,

electron

energy

presses, laminating machines etc. Their operation parame-

absorption

in

the

foil

of

more

than

30%

leads

to

foil

ters such as electron energy, beam power, irradiation width

deterioration.

For

15 pm

titanium

foils this limit is reached

and dose rate can be precisely matched to the demands of

at about

120 keV.

 

the industrial process. In all accelerators mentioned elec-

At electron

energies

larger

than

10 Mev

nuclear

reac-

trons are produced by a hot cathode at high-voltage

poten-

tions

can

occur

which

should

be

avoided

in

industrial

tial.

applications.

In

a

single

gap

the

electrons

are

accelerated

to

the

anode (usually

the

accelerator

window).

Up

to

electron

2.1. Low-energy

electron

accelerators

energies of about 300 keV a stable acceleration in only one

stage

and

self-shielding

is possible.

An upper

limit

of the

The

low-energy

electron

accelerators

mentioned

in

electron beam power is given by the maximum possible

Table

1 are

well

developed

and can

be used

as computer-

current per square centimeter of window area which is 0.2

controlled subsystems

in

coating

machines,

printing

mA cme2.

Table

2

Medium-energy

electron

accelerators

for industrial

use

Manufacturer,

Model

Electron

energy

Beam

power

Remarks

 
 

(MeV)

(kW)

Radiation

Dynamics

Inc.,

USA

0.3-0.55

90

self-shielded,

 

Dynamitron

0.8

beam

width

1.5 m

Serval

types

1.2,

1.5, 2.5,

3.0, 4.5

60-150

Nissin-High

Voltage

Co., Japan

0.5, 0.8,

1.0, 1.5,

40-150

beam width

1.2

Co&oft-Walton

 

2.0,

3.0, 5.0

or

1.8 m

NIIEFA,

St. Petersburg,

Russia

0.25-0.5

 

25-100

self-shielded,

UV-Series

0.75-

1.5

beam

width

<

2 m

Institute

of Nuclear

Physics,

0.5-

1.5

20-60

beam

width

1.5 m

Novosibirsk,

Russia

 

ELV-Series

 

II. ELECTRON

ACCELERATORS

20-60 beam width 1.5 m Novosibirsk, Russia   ELV-Series   II. ELECTRON ACCELERATORS
8 4 R. Mehnert/ Nucl. Instr. and Meth. in Phys. Res. B 113 (1996) 81-87

84

R. Mehnert/

Nucl. Instr. and Meth. in Phys. Res. B 113 (1996) 81-87

Table

3

Electron

linear

accelerators

for industrial

use

Manufacturer,

Model

 

Electron

energy

Beam

power

Remarks

 
 

(MeV)

(kW1

MEV Industries,

Jouy-en-Josas,

France

S-10

IO-20

S-band

CIRCE

II/III

 

AECL.

Kanata,

Canada

 

10

50

L-band

IMPELA

 

THORIY,

Moscow,

Russia

 

2-10

6-12

L-band

Elekroonika

 

Scanditronix, Uppsala, Sweden Scanditronix EB 10

 

10

30

L-band

Varian

Inc., Palo

Alto,

USA

2-10

0.6-5

S-band

Mega

Ray-Series

 

Inst. of Nuclear

Physics,

Novosibirsk,

Russia

 

1.o-2.5

10-35

radio

frequency

30 MHz

ILU

Ion Beam

Application

!%A., Belgium

 

10

30

107.5 MHz experimental

Rhodotron

 
10 30 107.5 MHz experimental Rhodotron   2.2. Electron accelerators with energiesfrom 0.5 to 5 MeV

2.2. Electron

accelerators

with energiesfrom

0.5 to 5 MeV

process

thick

plastic

and

rubber

sheets,

wire

and

cable

This

is

a class

of

electron

accelerators

which

have

a

insulation, plastic tubes and pipes and fiber-reinforced composites. Crosslinking of wire and cable insulation is

similar

high-voltage

generation

(see

Table

2).

Usually

the main application, followed by crosslinking of films,

transformer/rectifier

high-voltage

sources

are used and the

 

foaming and vulcanization of tire components. The most

acceleration

potential

is

built

up

at

the

sections

of

an

rapidly growing application,

however,

is electron

curing

of

acceleration

tube.

Medium-energy

electrons

are needed

to

fiber-reinforced composites.

 

MEC,

MG,

ESI

CDL:

current

density

limitation

assuming

Electron Energy (keV)

a 20 cm window

Fig. 2. Curing

applications

of low-energy

electron

accelerators.

2.3. Electron linear accelerators production rates, smaller space requirements moderate temperature increase during

2.3. Electron linear accelerators

production rates, smaller space requirements moderate temperature increase during curing.

and

85

only

R. Mehnert/Nucl.

Instr. and Meth. in Phys. Res. B 113 (1996) 81-87

Electrons

with

energies

up

to

10

MeV

are

usually

generated by linear accelerators (see Table 3). Both travel- ing wave as well as resonator-type accelerators are mainly

plays an important role.

3.2. Electron beam degradation of chlorinated hydrocar- bons in air

used for sterilization, food irradiation and fine-tuning of semiconductors. But also the curing of composite materials

Chloroethenes such as 1,2-cis-dichloro-, trichloro- and perchloroethene are frequently detected to be ground water pollutants. In a typical ground water remediation process the volatile chloroethenes are removed from water by

3. Industrial

application

of electron beams -

selected

air-stripping.

examples

The resulting polluted air is fed to charcoal absorbers.

3.1. Electron beam curing

 

This classical procedure implies several limitations: 1,2- cis-dichlorcethene is only weakly absorbed on charcoal but mainly released into air. Furthermore, chloroethenes are

During

1994 in Europe

nearly

24000

tons

of acrylates

frequently accompanied by aromatic pollutants. Incinera-

and

epoxides

were

used

as binders

for electron

beam

(or

UV)

curable

coatings,

varnishes,

paints

and printing

inks.

In

terms

of

end-use

sectors,

wood

coatings

 

account

for

a

45%.

Overprint

varnishes

and

web

converting

consume

25% and printing

inks have

15% of the market.

 
 

These

three

major

application

fields

impose

different

 

demands

on the electron

accelerators

used

for curing

(see

Fig.

2).

The

electron

beam

curing

of

coatings

on

rigid

sub-

 

strates

-

chiefly

furniture,

doors,

laminated

panels,

par-

quet,

gypsum

tiles,

plastic

sheets

and metal

-

requires

a

large

range

of

electron

energies.

Some

of

these

coatings

 

are

on

non-porous

substrates

and

reach

only

masses

per

unit area

of less

than

50

g m-‘.

Electron

energies

in the

 

range

of

150 keV are sufficient

for these

applications.

On

the other

hand,

curing

of higher

coating

masses

on porous

 

substrates

and curing

of edges

need electron

energies

up to

250 keV.

 
 

In the

case

of rigid

substrates

the production

rates

are

not

determined

by

the

curing

step

but

rather

by

other

 

operations

such as feeding

and substrate

pretreatment.

Low

or moderate

electron

beam

powers

are therefore

adequate.

b

 

Electron

beam

curing

of coatings

on flexible

substrates

often

takes

place

100-300

m mini

from

roll

to roll.

Production

speeds

are common,

at coating

weights

from

of

1

to 30 g rnm2. Therefore,

ate-to-high

electron

beam

low electron

energies

powers

are needed.

and moder-

In

printing,

especially

in

web

offset

printing,

presses

reach

speeds

up

to

1000

m

mini’.

Although

the

real

printing

speeds

are

usually

much

lower,

extremely

high

beam

powers

are

required,

but

relatively

low

electron

energies

can be chosen.

 

As

schematically

shown

in Fig.

2, also

in the

case

of

one-side

curing

of

printing

inks

a

lower

limit

of

the

electron

energy

is

set

by the current

density

limitation

due

to the window

foil damage.

 

In industry,

electron

beam

curing

is often

in competi-

tion

with

thermal

drying.

The

radiation

process

offers

 

significant

advantages

over

the

thermal

process:

No

sol-

vent

release,

reduction

of

the

energy

consumption,

high

Fig. 3. The mobile off gas cleaning plant AGATE-M.

II. ELECTRON ACCELERATORS

8 6 tion of the absorbers dioxine generation. R. Mehnert / Nud. Instr. nnd Meth.

86

tion of the absorbers dioxine generation.

R. Mehnert / Nud.

Instr. nnd Meth. in Phys. Res. B 113 (19961 81-87

containing

such

mixtures

can lead

to

Electron irradiation of air polluted with

1,2-DCE),

I, 1,l -trichloroethane

trichloroethene (TCE).

(1 ,l

,I -TCA)

and

chlorinated

hydrocarbons

offers an alternative method to

An overall

removal

efficiency

of 90%

was reached

at

a

decompose

the

pollutants.

Electron irradiation of air pro-

beam power

of

11 kW.

The

total

costs

of

the

treatment

duces

double

forms

to react with the chloroethenes

In air, oxidation

products

can

ization

removed

OH

bond.

mainly

radicals.

These

radicals

add

to

the

ethenic

The intermediate

chlorine

radicals.

takes place

OH adduct

mainly

leading

and Cl,.

The

from

the

off

and

Chlorine radicals are able

decomposes

and induce a chain reaction.

to the mineral-

acid and Cl,

HCl, CO, CO,

be

completely

gas

by

dry

including electricity, dry sorption materials, ozone catalyst, personal and depreciation amounted to 0.34 DM per m3 of treated ground water.

AGATE-M

fully used for the removal of volatile organic compounds

such as xylene and esters from an industrial paint shop.

The irradiation

plant

has also been

success-

sorption

or wet scrubbing.

 

3.3. Electron beam curing of$ber-reinforced composites

In

order

to

demonstrate

the

process

on

real

ground

 

water

remediation

sites,

the

mobile

irradiation

 

plant

Advanced

composites,

especially

carbon-fiber-rein-

AGATE-M

was developed

(Fig.

3).

forced

epoxies,

are widely

used

in aircraft

and

aerospace

The unit treats

a gas flow

of

up to

1200 m3 hh

and

is

industry

because

of

their

outstanding

strength-to-weight

installed

in

a

standard

30

ft

container

and

needs

only

and stiffness-to-weight

ratios,

corrosion

resistance

and ac-

electricity

(380

V,

32 and

63 A) for operation.

The

waste

ceptable

cost.

Carbon-,

glass-

and aramide-fiber-reinforced

gas

passes

through

the

inlet

filter.

Then

the

gas

can

be

composites

are

normally

produced

by

thermal

 

curing

of

humidified

and

flows

into

the

reaction

chamber.

It

is

epoxies.

The

carbon-fiber-epoxy

laminate

has

elastome-

housed

in

a

compact

lead

shielding,

which

contains

chanical

properties

comparable

to steel

but only

20%

of its

labyrinths

for incoming

and outgoing ducts. As accelerator

density.

However,

thermal

curing

is time-consuming,

can

a

LEA-3-type

operated

at

190 keV

and

60

mA

is used.

lead

to

residual

stresses

in

the

product

due

to

different

After electron

irradiation,

acidic

products

are filtered

by an

thermal

expansion

of

the

fibers,

and

the

matrix

and

compact

dry filter

unit. Ozone

is decomposed

catalytically

through-curing

is often

incomplete.

This

leads

to

the

re-

by an active

coke

filter.

lease

of

(toxic)

gaseous

products.

To

overcome

these

 

The

clean

gas is exhausted

by means

of a blower.

limitations,

during

the

last

decade

considerable

efforts

Fig.

4 shows

the decomposition

efficiency

obtained

at

have been made

to develop

facilities,

resins and processing

a

ground

water

remediation

site

in Dusseldorf

(Germany)

methods

for

electron

beam

curing

of

carbon-fiber-rein-

for

perchloroethene

(PCE),

1,2-cis-dichloroethene

(cis-

forced

composites

1151. A family

of

EB

curable

di-

and

1151. A family of EB curable di- and 100 80   m cis-1,2-DCEthene 60 n TCEthene

100

1151. A family of EB curable di- and 100 80   m cis-1,2-DCEthene 60 n TCEthene

80

 

m

cis-1,2-DCEthene

60

n

TCEthene

100 80   m cis-1,2-DCEthene 60 n TCEthene Fig. 4. Decomposition efficiency 1 . 9 4
100 80   m cis-1,2-DCEthene 60 n TCEthene Fig. 4. Decomposition efficiency 1 . 9 4
100 80   m cis-1,2-DCEthene 60 n TCEthene Fig. 4. Decomposition efficiency 1 . 9 4
100 80   m cis-1,2-DCEthene 60 n TCEthene Fig. 4. Decomposition efficiency 1 . 9 4
100 80   m cis-1,2-DCEthene 60 n TCEthene Fig. 4. Decomposition efficiency 1 . 9 4

Fig. 4. Decomposition

efficiency

1.9

4.8

7.6

electron beam power [kWj

obtained

after

electron

irradiation

of chlorinated

9.5

10.9

hydrocarbons

in air.

R. Mehnert / Nucl. Instr. and Meth. in Phys. Res. B 113 (I 996) 81-87

R. Mehnert / Nucl. Instr. and Meth. in Phys. Res. B 113 (I 996) 81-87

87

multifunctional epoxyacrylates is now available from dif- ferent manufacturers. This wide choice of resins can be favorably used for a variety of composite formulations.

Polymerization and crosslinking of these resins is initiated by electrons with typical energies of 10 MeV. High-power linacs (e.g. the IMPELA with 10 MeV and

50 kW beam power [16]) are used to cure up

to 3600 kg

h- of composite material. The maximum thickness of the laminate treated is 2

cm.

Based on first experiences in manufacturing of EB cured carbon-fiber composites the following advantages should be mentioned:

- Curing is done at ambient temperature. The tempera-

ture increase and distribution inside the laminate can be

controlled.

- Curing times can be reduced.

EB curable formulations do not autocure at ambient temperature. -

cured

-

The

amount

of

volatiles

released

from

the

composite is extremely small. With respect to their elastomechanical

properties,

EB

cured composites are now approaching the parameters of

the best made conventional

epoxy composites.

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R. Mehnert,

istry,

in: Ullmann’s

Encyclopedia

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II. ELECTRON

ACCELERATORS