CALIFORNIUM-252 PRODUCTION AND NEUTRON SOURCE

FABRICATION

1. B. KNAUER and R. C. MARTIN

Chemical Technology Division
Oak Ridge National Laboratory
P.o. Box 2008
Oak Ridge, TN 37831-6384

1. Introduction

The element californium was discovered in 1950 from the bombardment of helium ions
on a 242Cm target in the 60-in. cyclotron at the Berkeley Crocker Laboratory. The reaction
product, originally thought to be 244Cf, was later identified as 245Cf [1]. It was not until
November 1952 that the isotope 252Cf was discovered in the debris from the MIKE
thermonuclear test at Enewetak [2]. Early investigations of its properties indicated a half-
life of between 2 and 3 years (actually 2.645 years) and a significant branching fraction for
decay by spontaneous fission, making 252Cf an especially good and compact source of
neutrons.
These desirable properties led to a sustained (and still continuing) national effort to
produce and recover macroscopic quantities of2 52Cf. This effort was initiated late in 1952
with the start of the irradiation of multigram quantities of 239pU in the Materials Test
Reactor (MTR) at the Idaho National Engineering Laboratory. In 1958, six years later,
microgram quantities of2 52Cf from this irradiation were recovered at Lawrence Berkeley
Laboratory. The demand for 252Cf quickly exceeded the supply as heavy element research
increased. The National Transplutonium Element Production Program was undertaken in
1958 to produce large quantities of 252Cf to meet the increasing demands and to produce
the other transplutonium elements for the research community. This program led to a
large-scale market evaluation program at Savannah River Laboratory (SRL) and the
somewhat smaller research effort at Oak Ridge National Laboratory (ORNL) in the late
1960s. Since 1973, the entire supply of 252Cfin the western world has been produced in
the High Flux Isotope Reactor (HFIR) and recovered at the Radiochemical Engineering
Development Center (REDC) of ORNL.

2. Background: DOE's Californium Sales/Loan Program

The Market Evaluation Program, established in the late 1960s at SRL, was instituted
to develop the commercial market and applications for 252Cf, determine the potential
7
J.G. Wierzbicki (ed.), Californium-252.lsotopefor 21st Century Radiotherapy, 7-24.
© 1997 Kluwer Academic Publishers.
8

demand for the isotope, and ascertain whether a large-scale production capability would
be required at SRL to meet needs for 252Cf. This program included a training series,
demonstration centers, and seminars on the application of252Cf neutron sources in industry
and education. Early estimates projected that as much as 5 g of 252Cf per year would be
needed to meet the growing demands for the isotope.
Based on the early estimates, the U.S. Department of Energy (DOE) - at that time the
U.S. Atomic Energy Commission (AEC) - established the Industrial Sales/Loan and
University Loan Programs to make the isotope available for industrial, educational, and
medical applications. Facilities at SRL were constructed to develop, fabricate, and license
a variety of source designs for both the industrial and medical applications. And, in 1970,
the AEC announced that 252Cf would be made available for commercial and medical
applications at a cost of $lO/flg. The fIrst sale of I mg of2 52Cf took place in early 1971 to
the University of Kentucky Chemistry Department to perform activation analyses on
specimens retrieved from the moon [3]. Other sales quickly followed, including sales to
a half-dozen foreign countries.
In parallel with the Market Evaluation Program and the activities of the Industrial
Sales/Loan and University Loan Programs at SRL, efforts were conducted at ORNL in
conjunction with the Transplutonium Element Production Program to design and fabricate
252Cf neutron sources for use in research applications at other national laboratories and by
other integrated government contractors. Since research sources were provided only to
facilities exempt from licensing restrictions, they quite often contained relatively large
quantities of 252Cf (Le., up to as much as 57 mg). However, the Research Program did not
provide 252Cf on a sale basis for industrial or medical applications.
Following the initial flurry of interest in 252Cf and as experimental and demonstration
programs were replaced by established applications, the demand for 252Cf leveled out in the
range of 0.5 to 1.0 g per year, with both the industrial and research programs maintaining
a high level of participation in providing neutron sources to their respective user
communities. In 1983, the DOE Office of Nuclear Materials Production decided to move
the Industrial Sales/Loan and University Loan Programs (both administrative and
operational activities) to the REDC Californium Facility. The "temporary" facilities at SRL
needed to be replaced, and the recent program activity fIt very nicely with the
Transplutonium Element Production Program at ORNL.
In order to accommodate the activities ofthe Industrial Sales/Loan and University Loan
Programs while retaining full capabilities for the Transplutonium Element Production
Program, additional facilities and equipment had to be provided in the REDC Californium
Facility. The Californium Facility upgrade and transfer of program responsibilities were
completed in 1986. Since that time, all activities and operations (except medical source
fabrications) sponsored by DOE for the production of 252Cf, the fabrication of all 252Cf
source designs, and the distribution of 252Cf, both on a sale and loan basis, have been
conducted at the REDC Californium Facility.
The very specialized equipment and the capability to provide physically small
californium neutron sources for medical research and applications remained at SRL until
1994, at which time DOE completed the shutdown of all facilities related to the fabrication
of 252Cf into medical source forms. In response to the continuing demand for medical
sources, efforts have been initiated at the REDC Californium Facility to develop new 252Cf
 9
brachytherapy sources and to resume the fabrication of the various medical source designs
originally developed at SRL, such as the applicator tube (AT) currently in use at Wayne
State University for cancer treatment and research.

3. Production of 252ef at ORNL

The HFIR and the REDC began operation in the mid-1960s with the primary objective
of producing 252Cf and the other transplutonium elements. In the HFIR, material in the
targets is transmuted to 252Cfthrough a series of neutron captures and beta decays. Neutron
captures increase the neutron number and, thereby, the mass, while beta decays increase
the atomic number. The 252Cf yields are controlled by the flux, fluence, and various
destructive reactions that occur, such as the fissions of 23 9pu, 245Cm, 249Cf, and 251Cf. Yields
of 252Cf are also limited by beta decay reactions. The two most important are the beta
decay of 241pU to 241Am and that of 249Bk to 249Cf, which has a large fission cross section.
Figure 1 shows the path of neutron capture and beta decay for producing 252Cf and
illustrates losses incurred due to fission.

. ,-- --
fm 254 fm 255 fm 256 257
100 Fm ':. 1

-
a "- Sf
Ea 253 b 254 Es 255

9. Es re-

-- -- r-
a.B-.Et B-
et 249 Cf 250 Cf 251 Cf o252
" C, 253 C, ,.(
9. Cf Ie- -f- Ie-

., .jn.f)~ 0"
.-
a n.n":-, Q. Sf B-, Sf Sf
Hic 249 Hie 250 Hie 251

Bk Ie-

-. , - -
B_ " B- B-
em 242 em 243 em 244 em 245 em 24& em 247 em 248 em 249 em 250

.6 Cm re- f- I-
·"
-e- -e-

--
a "- Q. In.f .1n.Il' Q. (n.' Q. Sf B- Sf
Am 241 'l'm 242 Am 243 Am 244 Am 245 Am 246

Am
."
-e- Ie- -e- Ie-

. · " s-

·- .
B-£C
B- '" B- "
Pu 239 Pu 240 Pu 241 I'\.Pu 242 Pu 243 Pu 244 Pu 245 Pu 2.4'

Pu
a, (n,1l
:-
. l-
-, (n"
t-
B-
Ie- Ie-
B-
-e-
s-

-"
Figure 1, Transmutation of target material in the HFIR to produce mef.

Initially, 252Cfwas produced at HFIRIREDC from the irradiation of targets containing

242PU. Yields of 252Cf were enhanced relative to earlier 252Cf production at the MTR
10
because of the very high, steady-state thermal neutron flux (2 to 3 x lOIS n/cm 2-s) available
at the HFIR. In addition, the use of 242Pu as the target feed material, rather than 239Pu,
enhanced the yield because it required the absorption of fewer neutrons to produce 252Cf
and eliminated losses due to 239Pu and 241pU fission. By 1968, most of the 242Pu had been
irradiated, with a substantial fraction being transmuted to 244Cm. This 244Cm, along with
244Cm produced at the Savannah River Plant, became target material for subsequent 252Cf
production. The continual irradiation and subsequent recovery of the 244Cm target material
have resulted in a significant and advantageous increase in the heavier curium isotopes.
The percentage of 244Cm in the target material has decreased from -90% to 30 to 40%. The
decrease in 244Cm and the subsequent buildup, primarily of 246Cm and 248Cm, have greatly
enhanced the yield of 252Cf. This is due largely to reducing the loss of target material to
245Cm fission and requiring fewer neutrons to produce 252Cf.
Currently, a typical transplutonium campaign involves the irradiation of 11 to 13
targets for 6 to 8 months in HFIR followed by processing and recovery in the remotely
operated and maintained hot cells at the REDe. The radiochemical processing to recover
and purify the 252Cf and other transplutonium element products from the irradiated targets
requires about 4 months to complete. Typically, REDC processing campaigns are
conducted every 12 to 15 months with 252Cf yields of 350 to 450 mg from targets
containing a total of 110 to 120 g of curium feed material. Production and recovery of
252Cf could be increased to -1.0 glyear if demand and mission merited such a program.

4. Properties of mef

Due to its spontaneous fission decay mode and its availability in macroscopic
quantities, 252Cf has been one of the most extensively studied transplutonium isotopes.
Most of the effort has been directed at understanding the spontaneous fission properties,
some of which are summarized in Tables 1 through 3. These properties should be taken
as "typical" or "representative" of 252Cf and not necessarily as the "best" or "refereed"
values. Table 1 shows the decay properties of californium isotopes that are routinely
produced during the production of 252Cf. Californium-253 has a short half-life, 17.81 d,
and will not be present in any of the fabricated neutron sources. Californium-254 decays
almost entirely by spontaneous fission. However, it is produced only in minute amounts
(due to the short half-life of its precursor 253Ct), and its contribution to the overall neutron
source strength is generally negligible. All the other californium isotopes listed in Table 1
will be present. The exact isotopic mixture is dependent on the conditions of irradiation
and subsequent period of decay.
Table 2 gives some of the gross spontaneous fission properties of 252Cf. The neutron
emission of3.768 n/fission (2.31434 x 10 12 n/s per gram of2 52Ct) does include the fission
product delayed neutrons.
The 252Cf neutron energy spectrum is given in Table 3. The National Bureau of
Standards (NBS)-evaluated spectrum in this table compensates for the deviations from an
ideal Maxwellian spectrum with the use of energy-dependent adjustment functions. The
relative uncertainties in the NBS neutron energy spectrum are small, with exceptions ofthe
relative uncertainties in the 0- to 0.25-MeV and 8.0- to 12.0-MeV energy groups.
 11

TABLE 1. Decay properties ofselected californium isotopes [4]

Specific activity Branching fraction

Isotope Half-life (Ci/g) Decay mode (%)

wCf 350.6y 4.095 IX -100

SF 5.2 x 10-7
»OCf 13.08y 109.3 IX 99.923
SF 0.077
1.l'Cf 898y 1.59 IX 100
mCf 2.645 y 536.3 IX 96.908
SF 3.092
»3Cf 17.81 d 2.898 x 10' ~ 99.69
IX 0.31
1.l4Cf 60.5 d 8497 SF 99.69
IX 0.31

TABLE 2. Californium-252 spontaneous fission properties

SF branching fraction 3.092% [4]

Neutron multiplicity 3.768 nlfission [5]
Mean fission neutron spectrum energy 2.13 - 2.15 MeV [6-8]
Prompt y-ray multiplicity (mean) - IO/fission [9]
Average prompt y-ray energy 0.7-0.9 MeV [9]
Total prompt y-ray energy 6.7-9.0 MeV [9]

TABLE 3. NBS evaluation ofthe mCfneutron spectrum [6]

Xc. = [0.6672(E)" exp(- El1.42)] . I1(E), where E is in MeV

Energy interval
(MeV) I-t(E)
0-0.25 1 + 1.20E - 0.237
0.25 -0.8 1 - 0.14E + 0.098
0.8 - 1.5 1 + 0.024E - 0.0332
1.5 - 6.0 1 - 0.00062E + 0.0037
6.0 -20 1.0 exp[-0.03(E - 6.0)]

Energy interval Relative uncertainty (10)

(MeV) (%)
0-0.25 ±13
0.25 -0.8 ± 1.1
0.8·1.5 ± 1.8
1.5 - 2.3 ± 1.0
2.3 - 3.7 ± 2.0
3.7 - 8.0 ± 2.1
8.0 -12.0 ± 8.5
12

However, the number of neutrons emitted in these two energy groups is small compared
with the total neutron emission.

5. REDC Californium Facility

The Californium Facility, located in Building 7930 of the REDC at ORNL, was placed
in operation in the late 1960s. The primary objectives at that time were (1) [mal
purification of 252Cf from lanthanides and other actinides, (2) recovery and separation of
the alpha-decay daughter 248Cm from the purified 252Cf, and (3) fabrication of 252Cf into
small, intense neutron sources having a variety of capsule designs. These neutron sources
were distributed to researchers at other national laboratories and/or the facilities of
integrated government contractors for a variety of applications under the provisions of the
DOE Office of Basic Energy Sciences (OBES) as part of the DOE/OBES heavy-element
research program.
In 1983, the DOE Californium Industrial Sales/Loan and Medical/University Loan
Programs were transferred from SRL to ORNL. Under the Industrial Sales/Loan Program,
252Cf in the form of bulk oxide and palladium-californium oxide composite pellets and
wires is sold to foreign and domestic commercial encapsulators and 252Cf neutron sources
are loaned to agencies of the U.S. government. Under the Medical/University Loan
Program, 252Cf neutron sources are loaned to medical and university researchers.
Additional facilities and equipment were provided in the REDC Californium Facility to
accommodate the added operations.

5.1. FACILITY DESCRIPTION

The Californium Facility, shown schematically in Figure 2, was originally located

entirely within the Cell G area. The area within the lA-m-thick walls of Cell G was
partitioned off into four workstations that contained the processing equipment needed to
purify californium, recover 248Cm, and fabricate various neutron source designs.
Processing equipment included high-pressure ion-exchange columns to purify the
californium and separate 248Cm. Furnaces, constant-temperature baths, hydraulic presses,
capsule welders, helium-leak detectors, and neutron assay counters are some of the in-cell
equipment used in neutron source fabrications. All operations that involve high levels of
contamination are conducted in the Cell G workstations. These include primary capsule
fabrication of all source designs, primary capsule testing, and preliminary neutron assays.
In order to accommodate the additional operations and activities of the DOE
Californium Industrial Sales/Loan and Medical/University Loan Programs while retaining
full production and fabrication of the DOE/OBES Program, the Californium Facility was
expanded in 1983 both within the existing Cell G area and into the areas of Cell B, Cell C,
and the Fuel Storage Pool. A pneumatic transfer system was also installed to move sources
rapidly and remotely between the various hot cell workstations and the californium storage
pool. It is important to note that all areas in the Californium Facility, except for Cell G, are
contamination free.
 13

"."-:.

CELLO CELL C

.....

Figure 2. Schematic diagram of the cell operating areas of the Californium Facility.

5.2 FACILITY OPERATION

The californium recovered from the irradiated targets is purified as much as possible
from fission products, cationic and anionic impurities, and other actinides in the hot cells
of REDC Building 7920. Final purification from residual curium isotopes, especially
244Cm, is necessarily performed in the hot cells of the REDC Californium Facility. Levels
of 244Cm are very closely controlled in the Californium Facility, and cross contamination
by 244Cm of both 252Cfand its 248Cm alpha-decay daughter can be virtually eliminated. All
subsequent californium operations, including all neutron source fabrications, are carried
out in the Californium Facility.
The basic flowsheet for processing californium at the Californium Facility is depicted
in Figure 3. First, the californium is processed by high-pressure cationic-exchange
chromatography to remove traces of curium and other actinides remaining from the initial
processing. Two options are then considered for the purified californium. One option is
to use the purified californium immediately in the preparation of bulk californium
shipments and/or neutron source fabrications. The second option is to load it into platinum
capsules and store it for about 2 years to allow for decay of 2S2Cf to 248Cm. At the end of
the decay period, the californium is reprocessed to recover the 248Cm and is then either
14

reloaded into platinum capsules and stored for another decay cycle or set aside for the
preparation of bulk californium shipments and/or neutron source fabrications.

I 244Cm I

Figure 3. Californium Facility processing flowsheet.

All chemical processing of californium at the Californium Facility is conducted in the

workstations (cubicles) of Cell G (see Figure 2). Chemical processing operations include
high-pressure ion exchange, pressurized extraction chromatography, resin loading and
calcination, and oxalate precipitation and calcination. The operations to fabricate, test, and
assay the primary capsules for all neutron source designs and bulk shipping containers are
also performed within the workstations of Cell G. Many of these operations require the
handling of relatively large quantities of californium in both liquid and solid form, and,
therefore, the areas in Cell G are highly contaminated. All primary capsules, shipping
containers, and storage packages must be thoroughly decontaminated by acid leaching
prior to being transferred to the "clean" areas of the Californium Facility for subsequent
source fabrication operations and/or shipment preparations.
The remaining operllting areas in the Californium Facility are utilized for the
fabrication of the secondary capsules of all source designs, the [mal decontamination and
neutron assay of 252Cf sources, the loading/unloading of shipping containers, and the
storage of the REDC inventory of 252Cf neutron sources and storage packages. These areas
(Cell B, Cell C, and the storage pool) are maintained in a contamination-free condition.
Operating personnel can enter Cells B and C to set up equipment or experiments, stage
shipping containers for loading and unloading, and perform maintenance operations. The
 15

cell doors are interlocked to prevent personnel entry if significant sources of radiation are
present and to de-energize the x-ray unit power supply and the pneumatic transfer systems
when the doors are open.

5.3 SOURCE FABRICATION

As stated earlier, the Research Program at ORNL and the Industrial SalesfLoan and
University Loan Programs at SRL were conducted concurrently from the late 1960s until
1986, when they were combined at the REDC Californium Facility. Consequently, the
source designs developed for these programs employed chemical forms and fabrication
techniques that were quite different, even though the resulting neutron source capsules
were very similar.

5.3.1. Research Program mC/Neutron Sources

Research Program neutron sources, referred to as ORNL-type [10,11], incorporate

californium oxysulfate, Cf20 2S04 , as the chemical form. The physical form is the
oxysulfate dispersed in aluminum powder and pressed into a compact pellet. To prepare
ORNL-type sources, a resin-loading/calcination procedure has been developed. First, a
small aluminum can with a porous frit at the bottom end is loaded with cation-exchange
resin and aluminum powder to make what is essentially a small ion-exchange column. The
column is assembled into the loading configuration, and a dilute nitric acid solution of
californium is passed through the resin to load the californium. The loaded column is
disassembled from the loading apparatus, dried, and then calcined at 450°C to convert the
californium to the oxysulfate form.
After resin calcination, aluminum powder is added to fill the column, which is then
placed in a die and pressed hydraulically to form a pellet. The source pellet is placed in
a primary capsule, a spacer is inserted to hold the pellet in position, and the end plug is
inserted and seal welded. The welded capsule is x-rayed and helium-leak tested to ensure
the integrity of the weld. This makes a singly encapsulated NSS or NSZ neutron source,
depending on whether the capsule material is 304L stainless steel or Zircaloy-2.
If double encapsulation is required, the threaded portion of the primary capsule is
removed. The primary capsule is then loaded into the secondary capsule, the end cap is
inserted, and the closure weld is made as shown in Figure 4. The resulting doubly
encapsulated source is designated as an NSD or an NZD. These sources may contain up
to 35 mg of 252Cf. The LSS and LSD sources shown in Figure 4 may contain up to 50 mg
of 252Cf.

5.3.2. Industrial Sales/Loan and University Loan Program mC/Neutron Sources

The Industrial SalesfLoan and University Loan neutron source designs [12] developed
at SRL incorporate californium oxide, Cf20 3, as the chemical form. These source designs,
referred to as SR-Cf-Series sources, are fabricated by first precipitating californium from
dilute nitric acid solution using oxalic acid. The californium oxalate slurry is filtered into
a Pt-l 0 wt % Rh primary capsule, and a top frit is inserted to entrap the oxalate, which is
16

then dried and thennally decomposed to the oxide fonn. Following closure of the end
plugs by seal welding, the primary capsule is assembled and seal welded in secondary
capsule components of either 304L stainless steel or Zircaloy-2.

n _~·20
1r? . '".
UNC-U
_'2-24 UNC-ZA

::::~
THREAD

VOID 8
N
c
-

li fa
N ~ ~
ALUMINUM PELLET
- ~ NSSORNZS
CHARRED RESIN CAPSULE WITH
THREADED PORTION
... CUT Of'f'

-oj 0.499 In I-
MODEL NSS OR NZS MODEL NSD OR NZD
(SINGLE ENCAPSULATION) (DOUBLE ENCAPSULATION)

_'~-20 UNC-ZA

~
_~4-20UNC-2A THREAD
THREAD

......
OUTER CONTAI NER

VOID

•N •
...
ill
SPACER SPRING
.!
N
ALUMINUM PELLET i;
~~
LSS CAPSULE WITH
THREADED PORTION
~.!
CHARRED RESIN I CUT Of'f'

CALlf'ORN IUM I
P::::<IF~
~o.e25ln~
MODEL LSS MODEL LSD
(SINGLE ENCAPSULATION) (DOUBLE ENCAPSULATION)

Figure 4. Research Program 2SlCfneutron source designs (ORNL-type).

The SR-Cf-100 Series, shown in Figure 5, and the SR-Cf-3000 Series sources are the
source configurations most often fabricated for the Industrial Sales/Loan and University
Loan Programs. The two capsules have the same diameter, 0.942 cm, but different lengths.
The SR-Cf-100 is 3.76 cm in length and is designed to contain up to 10 mg of 252Cf. The
SR-Cf-3000 is 5.36 cm in length and is designed to contain up to 50 mg of 252Cf.
Another basic fonn of californium used in commercial source fabrication, also
developed at SRL, consists of a palladium-californium oxide composite material [13]
which can be shaped into either wires or pellets. To prepare a Pd-Cfz03 composite source,
 17
the californium oxalate is precipitated as usual. Tetrammine palladous nitrate is added to
the oxalate slurry, and the ionic palladium (pd2+) is reduced to palladium metal by the
addition of hydrazine hydrate. During the reduction process, the californium becomes
dispersed uniformly in the mixture as the palladium metal deposits on the surface of the
finely divided oxalate precipitate. Following decantation of the supernate, the precipitated
mixture is washed, dried, and calcined at 700°C to convert the californium oxalate in the
palladium matrix to the oxide form. The calcined mixture is then transferred to a die and
green pressed to form a pellet.

ORNL D~G 88-6605

- PUW-
SCllLE: J" - 2"

CAVITY FOR CALIFORNIUM OXIDE

PRIMARY CAPSULE BODY

SECONDARY CAPSULE END CAP

NOTE: SEAL ~ELDED
SECONDARY CAPSULE BODY THREADED STEM ("10-32 UNF-2A)

- SECTION -
SCRLE: J. - 2"

Figure 5. Basic design (SR-Cf-IOO Series) for Industrial SaieslLoan Program and University Loan Program
mCf neutron sources.

The green-pressed pellet is transferred to a carbon crucible and either sintered at

1300°C to form a Pd-Cf20 3 cermet or melted at 1600°C to form an "alloy." A pellet may
be coined and then encapsulated as a SR-Cf-lOO Series neutron source. Pellets may also
be processed through the successive grooves of a rolling mill to form wires -15 cm long
with a nearly square cross section of -0.11 cm on a side. The wires are normally used for
sale of the 252Cf or for sources that are small in terms of 252Cf content. Wires are fabricated
with nominal 252Cf concentrations in three ranges: 200 J.1g!cm, 20 J.1g!cm, and 2 J.1g!cm.
18

Because the concentration is very uniform over the entire wire length, required source
strengths may be obtained extremely accurately by cutting a wire of the specified
concentration to the appropriate length. Wire segments can then be encapsulated into
standard source configurations or packaged and shipped to commercial encapsulators.

6. ISler Medical Sources

As part of its Market Evaluation Program, the AEC provided 252Cf neutron sources to
medical institutions for the evaluation of 252Cf in cancer therapy. SRL developed,
manufactured, and licensed several medical source forms for intracavity and interstitial
applications and also developed a 252Cf interstitial implant system analogous to an existing
192Ir system. All existing 2s2Cf medical sources were fabricated at SRL, with the last
sources fabricated in 1992 and presently in use at Harper Hospital of Wayne State
University. The REDC at ORNL is presently developing equipment and techniques to
fabricate and license new sources as full-strength replacements for an existing SRL design
as well as develop 252Cf sources for use in remote afterloading equipment.

6.1 MEDICAL SOURCE FABRICAnON AT SAVANNAH RIVER LABORATORY

SRL developed several 2s2Cf medical source designs in the form of slender needles and
loading cells. A total of approximately 3000 medical sources were manufactured at
SRL [14]. Three 2s2Cf source designs were developed for interstitial applications: the
afterloading cell (ALC, up to -5 j.J.g 252Ct), the short afterloading cell (SALC, up to 2.4 j.J.g
2S2Ct), and the seed source (ALC-P4C, up to 0.7 j.J.g 2S2Ct). The applicator tube (AT, up to
-30 j.J.g 2S2Ct) was developed for intracavity applications. The afterloading cells and the
AT source were doubly encapsulated in Pt-l 0% Ir alloy, while the singly encapsulated 252Cf
seeds were stacked in heat-shrinkable tubing to form assemblies of3 to 12 seeds. All of
these sources were based on Pd-Cf20 3 wire as the active component. SRL also
manufactured a thicker custom medical source called the Toshiba afterloading cell
(TALC-PC, up to 1000 j.J.g 2S2Ct), which contained a sintered Pd-Cf20 3 pellet of2.3-mm
diameter [15]. Table 4 shows the physical dimensions and maximum licensed 252Cf content
for each source design. The AT is the only medical source design fabricated at SRL since
1975 [14] and is presently being used for tumor therapy at Harper Hospital.
Except for the TALC-PC, the active material in the SRL medical sources was a thin
wire containing a Pd-Cfz0 3 cermet core that was clad in a sheath of Pt-l 0% Ir alloy. The
Cf20 3 was embedded within the palladium matrix and the Pt-Ir alloy cladding provided
additional containment of the 252Cf. The wire was segmented by a pinch-cutting tool that
provided a continuous sheath even across the cut ends of wire segments [16]. Preparation
of the Pd-Cf20 3 cermet material has been described previously (Sect. 5.3.2); in this case,
however, the green-pressed pellet (approximately 50% theoretical density) was sintered at
1300°C rather than melted at higher temperatures. The sintered pellet was then repressed
to approximately 90% theoretical density and inserted and pressed into a billet body that
was machined from Pt-l 0% Ir stock. A platinum plug was gold brazed into the billet to
complete the assembly. The composite billet was reduced in a specially designed
 19

swage/drawbench to produce a wire of desired thickness. An explicit concern was the beta
dose to medical personnel who manually handled the sources [17]. Use of high-density
(21.5-g/cm 3) Pt-Ir alloy for sheath and capsule walls alleviated this concern.

TABLE 4. Californium-252 medical source designs from Savannah River Laboratory

External capsule Internal capsule Maximum

Source SRL dimensions (mm) dimensions(a) (mm) source
name model strength(b)
Length Diameter Length Diameter (J.Ig mCt)

Seed ALC-P4C!c) 6.05 0.81 4.0(C) 0.46 0.7

Short afterloading
SALC 17.9 0.97 15.0 0.41 2.4
cell

Aflerloading cell ALC 32.9 0.97 30.0 0.41 4.8

Applicator tube AT 23.1 2.79 15.0 1.35 29.8

Toshiba
TALC-PC 9.80 4.70 4.6 2.59 1025
afterloading cell

(a) The seed design is single encapsulated; all other designs are double encapsulated. The internal capsule
dimensions represent the approximate void geometry available for insertion of 2s2Cfsource material.
(b) Based on IAEA Certificate of Competent Authority for Special Form Radioactive Materials.
(c) The general model name for the seed is ALC-PXC, with X the active wire length in mm. Although X could
vary from I to 10, the ALC-P4C was the standard seed source [18].

Four swaging passes were required to reduce the billet diameter from 7.6 mm to
2.5 mm [19]. The wire was reduced to its fmal size by a series of pointing and drawing
operations; that is, the swager was used to "point" the composite wire so that it could be
inserted into the draw die and secured in a gripper while the die was pulled over the wire.
This process was repeated with draw dies of smaller and smaller diameter. The wire was
periodically annealed at high temperature to reduce the effects of work hardening. At
0.76-mm diameter, the size needed for AT sources, the wire was over 4 m long and the
252Cf-containing core only 50 cm long [14]. At 0.30-mm diameter, the size needed for
ALC, SALC, and seed sources, the wire was over 22 m long with a 2.5-m active core.
Handling these long lengths of wire was a major logistical problem, and the use of machine
oil as a draw die lubricant was messy for hot cell operations. The starting ratio of the billet
to core diameter was maintained throughout the swaging and drawing operations. The
252Cf content generally varied less than ± 10% along the length of the wire, and the lengths
varied less than ±5% from the nominal value [20].
The wire fabrication process was performed remotely in shielded hot cells by
equipment specially designed for operation with master-slave manipulators. The wire was
cut into specified lengths using a precision wire cutter and placed into the Pt-Ir alloy
capsule using a television camera and remotely controlled XYZ stage. The capsules were
20

mounted in a special collet to simplify handling during wire loading and welding, and the
collet was equipped with an adjustable depth stop and copper chill block to control melting
during plasma-arc welding. Seed sources were reported to have been fabricated in hands-
on glove box work [21]. After fabrication, the sources were decontaminated, assayed for
252Cf content, and prepared for shipment.

6.1.1. Afterloading Cells and Short Afterloading Cells

ALC and SALC sources were essentially line sources of 252Cf. They were made by
doubly encapsulating the clad californium-cermet wire in Pt-lO% Ir alloy tubing. All of
the closures were fusion welded. Nominal dimensions are given in Table 4. The inner
capsule was leak checked by an immersion-vacuum leach test in 4 M RNO]. The alpha
activity of the leach acid was measured after drying, with removable contamination
required to be less than 0.0135 nCi «10 dpm above background) for the source to pass
inspection. The outer capsule weld was leak checked using a helium-leak detector
calibrated to detect a leak rate ofless than 2.8 x 10-8 cm] of helium per second. The linear
uniformity of each source was confIrmed by making an autoradiograph which was read by
a computer-automated microphotometer [20].

6.1.2. Applicator Tubes

AT sources were made by doubly encapsulating IS-nun lengths of one or more of the
clad wires to provide 10 to 30 j.tg 252Cf per source as shown in Figure 6. Details of source
design, testing, and safety analysis for AT, ALC, and SALC sources are provided by
Permar [22].

6.1.3. Seed Sources

The ALC-P4C seed capsules each contained -0.5 j.tg of 252Cf inside a Pt-l 0% Ir alloy
capsule (single encapsulation). To ensure that no 252Cfwas in the closure welds and that
the 252Cf core was centered in the capsule, Pt-Ir alloy plugs, 1 nun long, were placed into
the ends of the encapsulating tubing. The capsule wall was designed to limit the beta
radiation from 252Cf to an acceptable level to the radiotherapist; that is, the beta-plus-
gamma dose was no more than one-third that from neutrons (assuming a relative biological
effectiveness of six) [17]. The outer diameter ofthe seed was chosen so that the outer
diameter of the completed assembly would be no larger than 1.1 mm, the diameter ofa 16-
gauge surgical needle.

6.1.4. Seed Assemblies

The 252Cf seed sources were typically used in seed assemblies that resembled the "seed-
in-ribbon" system [20] devised for InIr. Each assembly was typically a series of 3 to 7 (up
to 12 maximum) point sources (seeds) of 252Cf spaced 1 cm apart at mid-point with
"Tefzel" spacers in a flexible Tefzel plastic tube, as shown in Figure 7. Tefzel
(ethylenetetrafluoroethylene) was selected because it was more resistant to radiation than
 21

0.053"
{1.3 mm
Bodkin Eyelet
{0.02S" (O.S mm)
in diameter}

- Outer Sheath
{0.020" (O.S mm)
wall thickness}

0.911" Source Wires

(23.1 mm)
Inner Capsule
{O.OOB" (0.2 mm)
wall thickness}

MATERIALS:
Source Wires
Pd-ef iJ 3Composite
pt·tO wt% Ir Clad

Inner Capsule
pt·tOwt% Ir

Ouler Capsule
pt·tO wt% Ir

Figure 6. Assembled applicator tube medical source.

252Cf INTERSTITAL IMPLANT SYSTEM

(Compatible with 16 go. surgical needle)

25Ze! Seed Assembly

• 0.4-0.5,.9 Z'ZCI In PHO% Ir .eeds
• Spaced on I·cm centers
• Olameler 1.1 mm (0.044 Inch)
• Melt-sealed In heal-shrunk lube of
"Tefle'" (e'hY'ene'etrofluoroelhylene)

Implanled Tube
Nylon or X-ray'opaque "EXRAO" (FEP "Tellon"'
• Ouler diaml.er 1.70 mm (0.068 Inch)
• Inner dlameler 1.35 mm (0.054 Inch)
• Olame'ral clearance 01 seed assembly. 0.25 mm (0.010 Inch I

Figure 7. Seed assembly for interstitial implants [17].

22

other heat-shrinkable plastics. The assembly was placed into an oven to shrink the tube
over the seeds and spacers, firmly locking them in position. Tefzel plugs were inserted into
both ends of the assembly and melt sealed in position by butt welding [17]. The 252Cf
content of each seed was required to be ±5% of the average within the assembly.
The calculated dose (n + y) at the interface between a O.5-ttg 252Cf seed and the plastic
sheath was about 100 Gy/day. To confrrm that Tefzel would not embrittle under
irradiation, an accelerated irradiation test was devised in which dummy seed assemblies
were exposed to a large (-5 mg 252Cf) neutron source for known lengths of time and then
subjected to accelerated bend tests [17]. A standard inventory of 41 seed assemblies,
typically containing -90 ttg of 252Cf, was provided by SRL to participants of the 252Cf
Medical Evaluation Program. The 252Cf seed assemblies could be pointed to pass through
a 16-gauge (1.65-mm outer diameter) hollow stainless steel needle which could be fitted
to the surgically implanted loading tubes of nylon or radiopaque Exrad".

6.2 MEDICAL SOURCE FABRICAnON AT ORNL

Historically, the only medical source fabrication performed at the REDC was the
insertion and sealing of 252Cf cermet pellets into the Pt-Ir alloy billets, which were then
shipped to SRL for wire fabrication. After SRL fabricated the last AT sources in 1992,
scoping studies were made for implementing medical source fabrication at the REDC.
Cost estimates for duplicating SRL equipment and operations were prohibitive, so
alternative techniques were developed based on standard ORNL wire fabrication for the
Industrial Sales/Loan Program (Sect. 5.3.2). Rather than sintering the cermet material at
BOO·C, the green-pressed pellet is heated to 1600·C to melt the Pd-Cf20 3 mixture. After
cooling, the cermet material has sufficient structural integrity to be rolled into a thin, self-
supported (i.e., unsheathed) wire on a jeweller's rolling mill. The standard configuration
for commercial sales is a I.I-mm square wire with nominal loading of 200 ttg 252Cf per cm
(-0.6 wt % 252Cf).
The REDC is pursuing two goals for medical source development. In the first, the
REDC will relicense the AT source for manufacture at ORNL to provide full-strength
replacement sources to Wayne State University and other medical centers on request. This
effort is required because existing AT sources have now decayed through two or more half-
lives. The melted cermet wires produced by the REDC could provide 252Cf contents of
> 1 mg in AT sources, compared with the licensed maximum of 30 ttg 252Cf. However,
these sources will not be relicensed to contain more than 100 ttg 252Cf because of the
neutron dose incurred by medical personnel during manual loading into patients.
The second goal is development of a miniature high-activity, remotely afterloaded 252Cf
source. These sources would significantly reduce treatment times, reduce dose to medical
personnel, and expedite treatment of brain and other tumors. To speed incorporation of
252Cf sources into existing afterloader hardware, the current design goal is to duplicate the
geometry of existing 192Ir gamma sources which are used in a remote afterloader marketed
by Varian Oncology Systems. The new 252Cf source will be limited to IO-mm length by
0.34-mm diameter and will be sealed inside a flexible nickel-titanium afterloader wire of
0.59-mm diameter [23]. The nominal goal for this source is a loading of 1 mg 252Cf.
 23

The 252Cf cermet wires for remote afterloader sources must be significantly thinner than
the wires currently produced. Rather than using draw dies to produce thinner wires as SRL
did, the REDC will swage the cermet wires to smaller and smaller diameters (i.e., rather
than drawing the die over the wire, the wire is fed into a swager with dies that hammer the
wire into a smaller diameter). The preliminary design for the remote afterloader source has
a core wire of heavily loaded 252Cf cermet material that is swaged inside a sheath of
palladium tubing to aid in decontamination. Preliminary projections of source strength are
based on developmental laboratory work using terbium as a chemical analog of californium
in the palladium matrix. The results indicate that a 252Cf loading of 5 wt % is feasible with
a total remote afterloader source strength approaching 200 jJ.g 252Cf. Other research on
alloy forms of analogs suggests significantly higher 252Cf loadings may be achievable
which could meet the nominal goal of 1 mg 252Cf in remote afterloader sources.
Fabrication and licensing of these sources will encourage significant expansion of research
and clinical studies in 252Cf neutron brachytherapy and neutron capture therapy.

7. References

1. Thompson, S. G., Street, K., Jr., Ghiorso, A., and Seaborg, G. T. (1950) The new
element californium (atomic number 98), Phys. Rev. 80,790-796.
2. Fields, P. R., et al. (1956) Transplutonium elements in thermonuclear test debris,
Phys. Rev. 102, 180-182.
3. Osborne-Lee, I. W. and Alexander, C. W. (1995) CALIFORNIUM-252: A
Remarkable Versatile Radioisotope, ORNL/TM-12706, Oak Ridge National
Laboratory, Oak Ridge, Tennessee.
4. Browne, E. and Firestone, R. B. (1986) in V. S. Shirley (ed.), Table o/Radioactive
Isotopes, Wiley-Interscience, New York, pp. 249-1 - 254-1.
5. Axton, N. E. (1986/87) Intercomparison of neutron-source emission rates (1979-
1984), Metrologia 23, 129-144.
6. Grundl,1. and Eisenhauer, C. (1975) Fission rate measurements for materials neutron
dosimetry in reactor environments, in Proceedings o/the First ASTM-EURATOM
Symposium on Reactor Dosimetry, pp. 425-454.
7. Holden, N. E. (1985) Mean fission neutron spectrum energies for 252Cf and fissile
nuclides 233U, 235U, 239Pu and 241Pu, in Proc. Int. Conf. Nuclear Data/or Basic and
Applied Science, Sante Fe, New Mexico, Vol. 2, pp. 1467-1470.
8. Walsh, R. L. (1989) Spin-dependent calculation of fission neutron spectra and fission
spectrum integrals for six fissioning systems, Nucl. Sci. Eng. 102, 119-133.
9. Hoffman, D. C. and Somerville, L. P. (1987) Spontaneous Fission, LBL-23475,
Lawrence Berkeley Laboratory, Berkeley, California.
10. Baybarz, R. D., Peterson, J. R., and Knauer, 1. B. (1969) A new encapsulation
technique for 252Cf sources, Trans. Am. Nucl. Soc. 12, 56-57.
11. Van Cleve, 1. E., Williams, L. C., and Knauer, 1. B., Jr., (1972) Fabrication of 252 Cf
neutron sources at ORNL, in Applications o/Californium-252, Proc. Am. Nucl. Soc.,
Natl. Topl. Mtg., CONF-720902, pp. 25-28.
24

12. U.S. Atomic Energy Commission (1972) 252Cf Source and Shipping Capsule
Assembly Design and Test Information, Appendices A, B, and E, SR-Cf-lOO
Industrial Sources, Savannah River Operations Office, Aiken, South Carolina.
13. U.S. Atomic Energy Commission (1973) 252Cf Source and Shipping Capsule
Assembly Design and Test Information, Appendix C, 252Cf Shipping Capsule
Assembly, SR-Cf-lOOO Series, Savannah River Operations Office, Aiken, South
Carolina.
14. Laxson, R. R. (1996) Source fabrication of implant tubes for interstitial and
intracavity applications, Oak Ridge National Laboratory, unpublished manuscript.
15. Boulogne, A. R. (1976) Safety Analysis of Doubly Encapsulated 252Cf Medical
Sources, Model TALC-PC, SRL-76004, Savannah River Laboratory, Aiken, South
Carolina.
16. Mosley, W. C., Smith, P. K., and McBeath, P. E. (1972) Neutron Sources of
Palladium-252Cf Oxide Cermet Wire, DP-MS-72-40, Savannah River Laboratory,
Aiken, South Carolina, CONF-720902--6.
17. Savannah River Laboratory (date unknown), 252Cfinterstitial implant system, Aiken,
South Carolina, unpublished manuscript.
18. Permar, P. H. (1976) Safety Analysis ofSingly Encapsulated 252CfMedical Sources,
Model ALC-PXC, SRL-76003, Savannah River Laboratory, Aiken, South Carolina.
19. Walker, V. W. (1975) Equipment and Operations for Preparing 252Cf Neutron
Sources for Interstitial Cancer Radiotherapy Research, DP-MS-75-9, Savannah
River Laboratory, Aiken, South Carolina, CONF-751101--21.
20. Laxson, R. R. (1994) Fabrication of medical implant tubes for interstitial and
intracavity applications, Oak Ridge National Laboratory, unpublished manuscript.
21. Laxson, R. R. (1996) Oak Ridge National Laboratory, personal communication.
22. Permar, P. H. (1977) Safety Analysis ofDoubly Encapsulated 252CfMedical Sources
(Models ALC, SALC, AT), SRL-76002 Rev. 2/77, Savannah River Laboratory,
Aiken, South Carolina.
23. Varian Associates (1994), VariSource7M, Remote Afterloader for High Dose Rate
Brachytherapy, brochure.