Nuclear Instruments and Methods in Physics Research B 208 (2003) 6673

www.elsevier.com/locate/nimb

Applications for radiation processing of materials

M.R. Cleland *, L.A. Parks, S. Cheng
Ion Beam Applications, 7695 Formula Place, San Diego, CA 92121, USA

Abstract
The physical and chemical properties of polymeric materials can be modied by treatment with ionizing radiation in
the form of gamma rays, X-rays and energetic electrons. High-energy electron beams are especially useful in this regard.
Polymerizing (curing), grafting, crosslinking and chain scissioning reactions can be initiated by irradiation. The results
of such reactions can enhance the utility and value of commercial products. Brief reviews of a variety of successful
applications are given in this paper. Additional information is provided about reaction yields (G-values), temperature
rises during treatment and the radiation stability of common polymers.
2003 Elsevier B.V. All rights reserved.
PACS: 01.30.Cc; 01.30.Rr; 81.05.Lg; 81.05.Qk; 81.40.Wx; 82.50.Kx
Keywords: Radiation processing; Electron beam processing; Curing; Polymerizing; Polymerization; Grafting; Crosslinking; Chain
scissioning; Polymer degradation; Temperature rise; Radiation stability

1. Introduction
Practical applications for radiation processing
of materials have been evolving since the introduction of this technology nearly fty years ago.
Crosslinking plastic materials, sterilizing medical
products and preserving foods were the earliest
developments. Processes for curing monomeric
coatings and inks were developed somewhat later.
The use of these and other processes has grown
and they are widely practiced today. Electron
beam crosslinking is used to produce heat-shrinkable plastic lms for packaging foods and other
consumer products, heat-shrinkable plastic tubing
and encapsulations for industrial products, plastic
foam and hydrogels for medical applications. The

Corresponding author.

insulation on electrical wires and the jackets on

multi-conductor cables are crosslinked to increase
heat tolerance and to improve the resistance to
abrasion and solvents. Crosslinked plastic pipe is
used for hot water distribution systems. Sheet
rubber components for automobile tires are partially crosslinked before the tire is made to stabilize
the thickness of these materials during the nal
thermal cure. Radiation-cured, solvent-free coatings and inks are used for magazines, newspapers
and a variety of packaging materials. Other applications include reducing the molecular weight
by scissioning of polymers, e.g. polytetrauoroethylene, polypropylene and cellulose, grafting of
monomers onto polymers to modify their surface
properties, and curing ber-reinforced composite
materials [1,2].
Many papers describing these applications have
been published in the proceedings of the twelve

0168-583X/03/$ - see front matter 2003 Elsevier B.V. All rights reserved.
doi:10.1016/S0168-583X(03)00655-4

M.R. Cleland et al. / Nucl. Instr. and Meth. in Phys. Res. B 208 (2003) 6673

International Meetings on Radiation Processing

[3], the four International Conferences on Ionizing
Radiation and Polymers [4] and the Pacichem
Conference Sessions on Polymer Radiation
Chemistry [5]. A number of books have also been
published on radiation chemistry and practical
applications of radiation processing [68]. Another
source of information is the on-line bibliography
of papers on radiation chemistry, which is maintained by the University of Notre Dame [9].
Industrial irradiation processes using highpower electron accelerators are attractive because
the throughput rates are very high and the treatment costs per unit of product are often competitive with more conventional chemical processes.
The utilization of energy in electron beam processing is more ecient than typical thermal processing. The use of volatile or toxic chemicals can
be avoided. Strict temperature or moisture controls
may not be needed. Irradiated materials are useable
immediately after processing. These capabilities are
unique in that benecial changes can be induced
rapidly in solid materials and preformed products.
The emphasis on polymers, both synthetic and
natural, is inuenced by a basic principle of radiation chemistry, namely that the energy per unit
mass or absorbed dose needed to obtain benecial
eects is lower in materials with higher molecular
weights [1014]. The dependence of absorbed dose
on the molecular weight and G-value of the reaction is discussed in the next section. This relationship explains why radiation processing is
seldom applied to inorganic compounds.

2. Specic energy requirement

The specic energy requirement (energy per unit
mass) for radiation-induced chemical reactions is
proportional to the absorbed dose (D). According
to the denition of the common dose unit, one
kilogray (kGy) equals the absorption of 1 kilojoule
(kJ) or 1 kilowatt second (kW s) per kilogram (kg)
of material. Therefore, the specic energy (SE)
requirement in kilojoules per kilogram (kJ/kg) is
just equal to the dose in kiloGrays:
SE D

kJ=kg;

67

The specic energy requirement can also be expressed in terms of the molecular weight (Mol.Wt.)
and the G-value (G) of the reaction. The G-value is
dened as the number of reactions or events per
100 electron volts (eV) of absorbed energy.
Therefore, SE is given by
SE 6:022  1023 100=G 1:602  1019 =103 ;
2
SE 9:65  103 =G

kJ=mole;

SE 9:65  106 =G Mol: Wt:

3
kJ=kg:

The factors used in this derivation are: 6:022  1023

molecules/mole, 100=G electron volts per molecule, 1:602  1019 joules/electron volt, 103 joules/
kJ and 103 /(Mol. Wt.) moles/kg.
By combining Eqs. (1) and (4), the following
expression for the dose is obtained [1014]:
D 9:65  106 =G Mol: Wt:

kGy:

G-values for many reactions are in the range from

0.1 to 10, with 1 being a typical value for crosslinking pure polymers. For example, if the molecular weight were 100,000 and the G-value were
about 1, then the dose needed to convert all of the
molecules in the material would be about 100 kGy.
This dose would be sucient for many crosslinking applications.
On the other hand, if the molecular weight were
100 and the G-value were as high as 10, then the
dose would be about 10,000 kGy. Such a high dose
would be impractical because of the high energy
requirement and the high processing cost. If the
irradiation were done adiabatically (without cooling), the molecules would probably be decomposed at the very high temperature caused by the
treatment. In eect, the absorption of 100=10
10 eV in every small molecule would produce extremely unattractive results. In comparison, the
average thermal energy at room temperature is
about 0.025 eV per molecule and it is about 0.10 eV
at 900 C. If only a fraction of the molecules
needed to be modied to obtain the desired eect,
then the dose could be reduced by this fraction.
The implications of Eq. (5) help to explain why
most of the industrial applications for radiation
processing are focused on polymeric materials with

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M.R. Cleland et al. / Nucl. Instr. and Meth. in Phys. Res. B 208 (2003) 6673

high molecular weights instead of on inorganic

compounds. Polymerization starts with small
molecules but one ionizing event can initiate a
chain reaction, which produces a nal product
with a high molecular weight. Dilute solutions are
not constrained by this consideration, provided
that the radiolytic products from the solvent react
with the solute molecules. Then most of the solute
can be converted even if only a small fraction of
the solvent molecules are ionized. Examples of
such processes are the degradation of toxic compounds in waste water and the extraction of sulfur
and nitrogen oxides from combustion gases.

Table 1
Thermal capacities and temperature rises per kGy in common
plastic materials
Plastic
material

Thermal
capacity
(J/g K)

Temperature
rise (K/kGy)

Nylon 6
Nylon 6,6
Polycarbonate (max)
Polycarbonate (min)
Polyethylene
Polymethylmethacrylate
Polypropylene
Polystyrene
Polytetrauoroethylene
Polyvinylchloride

1.67
1.67
1.26
1.17
2.30
2.09
1.92
1.34
1.05
1.34

0.60
0.60
0.79
0.85
0.43
0.48
0.52
0.75
0.95
0.75

3. Temperature rise
The temperature rise in irradiated materials is
also proportional to the energy absorbed per unit
mass, so it is proportional to the absorbed dose,
provided that the energy released or absorbed by
chemical reactions and by heat exchanges with
the surroundings are small in comparison to the
absorbed dose. In the following equation, DT is
the temperature rise in degrees Kelvin (K), D is
the average dose in kiloGrays (kGy) and c is the
thermal capacity in joules per gram per degree
Kelvin (J/g K).
DT D=c

K:

The thermal capacity of water is 4.186 J/g K, so the

adiabatic temperature rise per kGy of dose would
be 1=4:186 0:239 K. Other materials have lower
thermal capacities and higher temperature rises. A
list of common plastics with their thermal capacities and temperature rises per kGy is given in
Table 1. Polyethylene has the highest thermal capacity and the lowest temperature rise. Polytetrauoroethylene (PTFE) has the lowest thermal
capacity and the highest temperature rise.
Similar data for common metals are given in
Table 2. In general, metals have lower thermal
capacities and higher temperature rises than plastics. Heating of the copper conductors in insulated
wires and cables is a deleterious eect that must be
taken into account when designing an irradiation
process for such products. Multiple passes through
the electron beam with heat dissipation between

Table 2
Thermal capacities and temperature rises per kGy in common
metallic elements
Elemental
material

Thermal
capacity (J/g K)

Temperature
rise (K/kGy)

Carbon
Aluminum
Silicon
Titanium
Iron
Copper
Germanium
Silver
Tin
Tantalum
Tungsten
Gold
Lead

0.71
0.90
0.71
0.52
0.44
0.38
0.32
0.235
0.227
0.14
0.13
0.128
0.13

1.41
1.11
1.41
1.92
2.27
2.63
3.13
4.26
4.41
7.14
7.69
7.81
7.69

passes is the usual method for controlling the

temperature rise with applications requiring more
than 100 kGy.

4. Polymerization
4.1. Coatings, adhesives and inks
Solvent-free coatings, adhesives and inks are
cured (polymerized) by treatment with low-energy
electron beams. These materials are combinations
of oligomers (polymers with low molecular weights)
and monomers, which control the viscosity before

M.R. Cleland et al. / Nucl. Instr. and Meth. in Phys. Res. B 208 (2003) 6673

curing. Volatile solvents are not needed and curing occurs without loss of material. Typical oligomers are acrylated urethane polyesters, acrylated
epoxies and polyethers. A typical multifunctional monomer is trimethylolpropane triacrylate
(TMPTA). Dose requirements are relatively low,
in the range of 1030 kGy, and line speeds as
high as 1500 m/min are achievable at 10 kGy with
high-current, low-energy, multiple-beam electron
accelerators [15,16].
4.2. Composite materials
Fiber-reinforced composite materials are used
where greater strength is needed. Such materials
are usually cured with heat, but electron-beam
curing oers signicant improvements in processing technique, curing time and cost. Typical materials are acrylated epoxies with carbon bers.
Doses are usually in the range of 150250 kGy
[1719]. Initial formulations are mixtures of oligomers and monomers. The radiation curing process involves a combination of polymerization and
crosslinking. The main applications are in automotive and aerospace industries.

5. Grafting
The surface properties of polymers can be
modied by graft copolymerization with dierent
monomers [20]. Grafting can be accomplished by
electron beam irradiation on common polymers
such as polyethylene, polypropylene and uoropolymers. Most work has been done on polymer
lms, membranes, bers and natural and synthetic
textiles. Some examples of monomers that can be
grafted onto polytetrauoroethylene (PTFE) lms
are styrene, acrylic acid, 4-vinylpyridine and Nvinylpyrrolidone [21]. Other examples are the
bonding of styrene on cellulose, vinylpyridines on
wool and p-nitrostyrene on polyethylene, polypropylene and polyvinyl chloride [22]. Permselective membranes can be made by radiation grafting.
Hydrophilic properties can be imparted to hydrophobic polymers [23]. Biocompatibility of various
polymers can be improved in this way for medical
uses [24]. Other applications include ion exchange

69

membranes, fuel cell/battery separator lms, permeation separation membranes, surface adhesion
promotion, chelating bers for sea-water treatment and recovering of precious metals, etc. Some
dose requirements may be less than 10 kGy.

6. Crosslinking
Crosslinking is the most important eect of
polymer irradiation because it can usually improve
the mechanical and thermal properties and chemical, environmental and radiation stabilities of
preformed parts as well as bulk materials. Both
polymer crosslinking and degradation by chain
scission occur during treatment, but one or the
other of these eects may be predominant in some
materials [1013]. Examples of both types are given in Table 3. More than fty years ago, polyethylene was the rst polymer to be recognized as
cross-linkable by irradiation [10], and it is still the
most important commercially because of the great
variety of products made with it.
G-values for crosslinking GX and for chain
scission GS in a number of pure polymeric materials are given in Table 4 [25]. Materials with
GS=GX ratios below 1.00 are favored for crosslinking applications. Polyethylene has an attractive
ratio because its GS values are about half as high
as its GX values. Natural rubber has a very
favorable ratio because of its very low GS value.
Polybutadiene also has a very favorable ratio because of its very high GX value. The ratios for
polymethylmethacrylate, nylon and polypropylene are not particularly favorable. The ratios
for polytetrauoroethylene and polyisobutylene
Table 3
Radiation characteristics of generic polymers
Mainly crosslinking

Mainly scission

Polyethylene
Polyacrylates
Polyvinyl chloride
Polysiloxanes
Polyamides
Polystyrene
Polyacrylamides
Ethylene vinylacetate

Polyisobutylene
Polymethacrylates
Polymethylstyrene
Polymethacrylamides
Polyvinylidene chloride
Polytetrauoroethylene
Polypropylene ether
Cellulose

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M.R. Cleland et al. / Nucl. Instr. and Meth. in Phys. Res. B 208 (2003) 6673

Table 4
G-Values for crosslinking and chain scission in common polymeric materials
Polymeric material

Crosslinking GX

Scission GS

Ratio GS=GX

Low density polyethylene

High density polyethylene
Polyvinylidene uoride
Polymethylmethacrylate
Polymethylacrylate
Nylon 6
Nylon 6,6
Polyvinylacetate
Atactic polypropylene
Isotactic polypropylene
Polystyrene
Natural rubber
Polybutadiene
Polytetrauoroethylene
Polyisobutylene
Cellulose

0.81.1
0.51.1
1.00
0.5
0.5
0.67
0.50
0.30
0.27
0.16
0.0190.051
1.05
5.3
0.10.3
0.5
(low)

0.40.5
0.40.5
0.30
0.77
0.04
0.68
0.70
0.07
0.22
0.24
0.00940.019
0.10.2
0.53
3.05.0
5
11

0.47
0.56
0.30
1.54
0.07
1.01
1.40
0.23
0.81
1.50
0.41
0.14
0.10
20
10
(high)

are extremely unfavorable for crosslinking. Polystyrene has a favorable ratio, but its GS and
GX values are both extremely low because of the
stability of aromatic compounds.
The values of GX and GS both change with
absorbed dose. Usually GS would increase more
than GX does with increasing dose. So, it is
possible that upon reaching a certain dose level,
cross-linking dominated polymers, e.g. polyethylene or natural rubber latex, will change to be degradation dominated. GX and GS are also
dependent on irradiation conditions, such as temperature and atmosphere. A good example is
PTFE, which undergoes degradation readily under
ambient conditions, but can be cross-linked at elevated temperatures (>340 C) in an oxygen free
atmosphere.
Typical dose requirements for crosslinking are
in the range of 50200 kGy. Additives, typically
multifunctional monomers, may be mixed with the
basic polymer to enhance the crosslinking eect
and reduce the dose requirement. Antioxidants,
UV stabilizers and ame retardants may also be
added to meet industrial performance specications. Such additives may reduce the crosslinking
eect. So, the properties of commercial compounds may be dierent from those of pure polymers. However, the information given in Tables 3
and 4 may be helpful in selecting the type of material for a particular application.

Materials with low GS=GX ratios are usually able to tolerate very high doses without excessive degradation. The radiation stabilities of
some common polymers are given in Table 5.
Polymers with benzene rings in the chain tend to
have high radiation stability. Polystyrene and
polyethylene terephthalate (PET) are outstanding
examples of radiation-resistant materials, while
polypropylene, polytetrauoroethylene (PTFE)
and cellulose cannot tolerate very high doses. In
general, radiation degradation is greater with
gamma rays or X-rays in comparison to highpower electron beams because lower dose rates
and longer treatment times allow more oxidative
reactions to occur.
6.1. Insulated wire and cable
The crosslinking of insulation on electrical wires
and cables was one of the rst practical applications of electron beam processing. It was introduced by the former Raychem Corporation (now
Tyco Electronics) during the 1950s, and it has
been adopted by many other manufacturers since
then. Some polymers used in this application are
polyethylene, polyvinylchloride, ethylene-propylene rubber, polyvinylidene uoride, and ethylene
tetrauoroethylene copolymer. Product improvements obtained by irradiation include increased
tolerance to high temperature environments and

M.R. Cleland et al. / Nucl. Instr. and Meth. in Phys. Res. B 208 (2003) 6673

71

Table 5
Radiation stability of polymers with high doses
Polymer type

Radiation stability

Tolerance dose Dt (kGy)

Detrimental eects above Dt

Polyethylene
Polypropylene
Polystyrene
PET
PVC
Polyurethane
Polycarbonate
PTFE
Cellulose

Goodexcellent
Poorfair
Excellent
Excellent
Goodexcellent
Goodexcellent
Excellent
Poor
Fair

1003000
1080
80030,000
150030,000
40015,000
1001000
500010,000
560
80600

Discoloration
Discoloration, disintegration
Brittleness, discoloration
Brittleness, discoloration
Brittleness, discoloration
Brittleness, discoloration
Discoloration
Disintegration
Brittleness, discoloration

overloaded conductors, re retardation, increased

abrasion resistance and tensile strength, reduction
in cold ow, increased resistance to solvents and
corrosive chemicals and some other characteristics
[2628]. Irradiated wires are used in automobiles,
military vehicles, aircraft, spacecraft and many
other applications where high performance is required.

introduced by the Cryovac Division of W.R.

Grace & Co. during the 1950s [30]. Modern
packaging lms use blends of several dierent
polymers to provide desireable properties like
clarity, toughness, oxygen exclusion and moisture
retention.

6.2. Heat-shrinkable plastic tubing

Automobile tires are made with several dierent

components, e.g. the innerliner, the chafer strip,
the sidewall, the body and tread plies and the
fabric or steel reinforced belt. These materials are
irradiated to obtain partial crosslinking before the
tire is assembled. This stabilizes their thicknesses
during the nal thermal curing process. It also
prevents the steel belt from migrating through its
supporting matrix. The result is a higher quality
tire with more uniform thickness and better balance. This allows the tire to be made thinner to
save material and reduce cost. A thinner tire also
generates less frictional heating on the road.
Typical materials are isoprene and diene elastomers. Doses are in the range of 3050 kGy [1,2,31].

Thin-walled plastic tubing is crosslinked to enhance the so-called memory eect. Irradiation
xes or stabilizes the original dimensions of the
tubing. When it is heated above the temperature
where the unirradiated material would melt, the
tubing becomes elastic and can be expanded to
several times its original diameter. When cooled, it
maintains the expanded dimension but retains the
memory of its original dimension. When heated
again, it contracts to the original dimension.
Polyethylenes are commonly used for this application [29]. Many commercial products have been
developed to take advantage of the memory eect.
Some examples are encapsulations for electronic
components, bundles of electrical wires and exterior telephone cable connectors.
6.3. Heat-shrinkable plastic lm
Thin plastic lm is also crosslinked to enhance
the memory eect. The applications are mainly
in the food industry, where heat-shrinkable
wrapping material is used to make attractive,
sealed packages. This process was developed and

6.4. Rubber tires

6.5. Plastic pipe

Crosslinked polyethylene pipe is used for heating concrete oors with hot water. Composite
plastic and metal pipes are used to distribute hot
water for heating buildings. The composite pipe
consists of an inner layer of polyethylene to keep
the water from contacting the middle layer of thin
aluminum, which resists the water pressure, and an
outer layer of polyethylene for abrasion resistance.

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M.R. Cleland et al. / Nucl. Instr. and Meth. in Phys. Res. B 208 (2003) 6673

Both the inner and outer plastic layers are irradiated simultaneously with high-energy electrons.
6.6. Plastic foam
Plastic foam is made by mixing a foaming
compound with the basic polymer and then heating the mixture to form gas bubbles in the plastic
material. Polyethylene, ethylene vinlyacetate copolymer and polypropylene are suitable materials.
The foaming agent can be azodicarbonamide or
nitrogen gas. Radiation crosslinking allows the use
of higher expansion temperatures and simplies
the control of the expansion process. Applications
include foamed insulation in coaxial cables, gaskets, coated tapes, oor backing, helmet liners,
athletic safety pads, bra cups, automobile seat
padding and jewelry case liners [32,33].
6.7. Hydrogels
A hydrogel is a polymeric material which has
the ability to swell in water and retain a signicant
fraction (more the 20%) of water within its structure. However, it will not dissolve in water. The
network of hydrogel can be formed by radiation
crosslinking. Some polymers that can form hydrogels are polyvinylalcohol (PVA), polyacrylamide (PAAm), polyvinyl-pyrrolidone (PVP),
polyethylene oxide (PEO) and methyl cellulose
(MC). Hydrogels have excellent biocompatibility
and can be used for enzyme supports and controlled release of drugs which can be incorporated
in the hydrogel [34].

7. Degradation

ground readily. It can also be blended with unirradiated PTFE to adjust the melt ow and improve the processability. The resulting powder has
several uses, e.g. additives to greases, engine oils,
printing inks, coatings and thermoplastics. The
dose requirements can be very high, in the range of
5001000 kGy, although doses as low as 50 kGy
are also used for specic applications [1,3538].
7.2. Cellulose
Cellulose bers extracted from wood pulp can
be converted to a thick liquid called viscose, which
is used to make commercial products such as rayon fabrics and cellophane lms. The molecular
weight of the natural cellulose is reduced by
treatment with sodium hydroxide and heat. Then
this material is reacted with carbon disulde to
make viscose. Initial irradiation of the cellulose
causes a reduction in molecular weight, and enables the rest of the process to be completed in less
time with less chemical treatment. This reduces the
cost and also reduces the environmental pollution.
The dose requirement is about 15 kGy [39,40].
7.3. Polypropylene
Polypropylene and a few other polymers are
intentionally degraded by radiation in air to improve the processability for extrusion, etc. With
the reduction of the molecular weight, the melt
ow of the polymer will increase and the melt
viscosity will decrease. The irradiated polymer can
be mixed with the unirradiated polymer, and the
degree of degradation can be controlled so that the
mechanical property is not deteriorated too much
[41]. Doses are usually in the range of 1580 kGy.

7.1. Polytetrauoroethylene
8. Conclusion
According to the data given in Table 4, polytetrauoroethylene (PTFE) has a high G-value for
chain scission and a low G-value for crosslinking.
Therefore, irradiation will reduce its molecular
weight. This eect is used to convert scrap PTFE
into ne particles or micronized powder. The
unirradiated scrap is too tough, doughy and slippery to grind, but the irradiated material can be

Radiation processing is a practicable and economical method for modifying the physical and
chemical properties of polymeric materials. A few
industrial applications of this technology were
introduced about fty years ago, and many
more have been developed since then. The number
of irradiation facilities and the annual sales of

M.R. Cleland et al. / Nucl. Instr. and Meth. in Phys. Res. B 208 (2003) 6673

irradiated products have increased substantially.

The continuing growth of this industry is assured
by the benecial eects that can be obtained with
this treatment process.

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