Development of Advanced Reprocessing Technologies

A. Introduction

Currently about 10 500 tHM (tonnes of heavy metal) of spent fuel are discharged annually from
nuclear power reactors worldwide. Although this spent fuel still contains substantial fissionable
material (uranium and plutonium) that can be reprocessed and recycled as fuel, only 15% is currently
reprocessed. For most of nuclear power’s history, reprocessing and recycling of the separated U and
Pu in fast reactors has been the favoured strategy for the back end of the fuel cycle. While most
countries have adopted a ‘wait and see’ strategy on this matter, some countries have decided, due to
proliferation concerns and a lack of economic stimulus, to regard the spent fuel as waste and prefer to
dispose of it after 30-40 years’ storage without reprocessing. Lately, however, in some of these
countries there has been a resurgence of interest in reprocessing and recycling as key components of
developing future sustainable nuclear energy systems [Ref. 1, 2].

The main purpose of reprocessing is to better utilise natural resource by recycling the remaining
uranium and plutonium, thus reducing demands on fresh uranium mining and milling and ensuring a
more sustainable and long term use of nuclear energy. Reprocessing and recycling in fast reactors has
the potential to reduce the uranium demand per kWh by a factor of 50–100. Reprocessing of fuel from
light water reactors and gas cooled reactors and recycling of the separated plutonium as mixed oxide
(MOX) fuel is today commercially available.

Table 1: Composition of spent fuel from thermal reactors: associated issues and plausible solutions
Constituent Composition in Issue Disposition path
percentage

Uranium ~ 95 - 96 An energy resource. Separated uranium could be

recycled as fuel in reactors.
Plutonium ~ 1.0 An energy resource, but also the Separated Pu could be
major contributor to long term recycled in reactors as fuel.
radio-toxicity (and heat-load) of Proliferation concerns could
the waste. Separated Pu be reduced by not separating
constitutes a major proliferation pure Pu.
concern.
Minor actinides ~ 0.1 Important contributors to long- MAs can be burnt alone or in
(MAs) primarily term radio-toxicity of the waste. combination with Pu in fast
Np, Am, and Cm Proliferation concerns exist reactors.
concerning separated Np.
Stable or short- ~3-4 Some FPs such as Cs and Sr are Storage of high level waste
lived FPs (fission the primary contributors to the (HLW) for a few hundred
products) short term radio-toxicity and heat years or separation of Cs and
source in the waste. Other FPs, Sr for separate disposal after a
e.g. noble metals, could become few hundred years storage.
valuable. Separated Cs has industrial
applications.
Long-lived fission ~ 0.1 Contributors to the long term No industrial process to limit
products (LLFPs) radio-toxicity of the waste. the problem has been
viz., Tc and I developed.
Page 2

Figure IV-1 shows how the relative radio-toxicity1 of the different components of spent nuclear fuel
varies over time. For the first 100 years after spent fuel is discharged, its radio-toxicity is determined
by the fission products. It is then determined by plutonium. If the plutonium is removed, the minor
actinides determine the long-term radio-toxicity. It should be noted that both scales are logarithmic.

FIG. IV-1. Relative radio-toxicity of the different components in spent nuclear fuel from a light water
reactor irradiated to 41 MWd/kgU with respect to the radio-toxicity of the corresponding uranium
ore. [Ref. 3,4]

In comparison with direct disposal of spent fuel, present day reprocessing also provides some positive
effects on the remaining radioactive waste that needs disposal. These include:

• Long term radio-toxicity is reduced. This reduces long term concerns for the repository, which
could simplify the repository design and increase public acceptance.
• Long term heat production is reduced, which increases the capacity of a repository, as the
packaging density in most cases is determined by the heat load.
• The volume of high level waste is reduced.

These effects can be further enhanced in advanced reprocessing systems, where minor actinides are
also separated with the purpose of burning them, thereby further reducing the long term radio-toxicity
and heat load in the remaining waste. In addition, some valuable fission product materials, e.g.
caesium and platinum group metals, could be extracted for industrial use. Heat reduction is mainly
achieved by removing the caesium and strontium followed by plutonium and americium.

___________________________________________________________________________
1
Radio-toxicity is calculated by dividing the radioactivity (Ci) of a nuclide in the spent fuel by the maximum
permissible concentration (Ci/m3) of that radionuclide in drinking water.
 Page 3

B. PUREX – current industrial reprocessing technology

All current commercial reprocessing plants use the PUREX2 process. It was developed for civil
applications during the 1960s, following experience gained from military programmes.

In the PUREX process (which is summarized in Fig. IV-2), the spent fuel is first chopped into small
pieces and then dissolved in nitric acid and subjected to a solvent extraction process using tri-n-butyl
phosphate (TBP). Uranium and plutonium are selectively taken up in the TBP phase resulting in good
separation from the rest of the fission products and minor actinides3, which are retained in the initial
acid medium. The U and Pu are then separated in multistage extraction cycles and purified. The
present state of the art in PUREX reprocessing provides a 99.9 % separation of U and Pu. In some
variants of the PUREX process the Pu is coprecipitated with uranium to avoid the separation of pure
plutonium. This is the case in the Japanese reprocessing plant at Rokkasho. The waste stream (the
liquid high level waste) that contains fission products, minor actinides and activation products, is
processed and vitrified, i.e. mixed with glass material to form a borosilicate glass, and encapsulated in
a steel container.

Spent Fuel Storage

Off-gas Treatment

Mechanical
Disassembly
Hulls (HLW)
High Level Waste
Acid recovery
Acid dissolution

Solvent Extraction Solvent Treatment

Fission Product
Solvent Extraction Uranium Oxide
Consolidation (HLLW)
High Level Liquid Waste & Partitioning Conversion

Plutonium Oxide Reprocessed

Conversion Uranium

Plutonium

FIG. IV-2. Key steps in the PUREX process.

In a PUREX reprocessing facility the spent fuel is thus separated into its four components: uranium,
plutonium, high level waste containing fission products and other transuranic elements, and metallic
waste from the fuel rods and assemblies.

The PUREX technology is actively used on a large scale in France, Japan, India, Russia, and the
United Kingdom. It is used to reprocess uranium and mixed oxide (MOX) fuel from different types of
reactors (LWR, PHWR, GCR and LMFR4) and also fuel with different chemical forms and
enrichments, e.g. from research reactors. Around 90 000 tHM have been reprocessed in civilian

___________________________________________________________________________
2
Plutonium-Uranium Extraction (PUREX)
3
The main minor actinides are neptunium, americium and curium
4
LWR = light water reactor, PHWR = pressurized heavy water reactor, GCR = gas cooled reactor and LMFR = liquid
metal cooled fast reactor.
Page 4

reprocessing facilities. The current annual industrial reprocessing capacity is around 4600 tHM
globally, and it is expected that an additional 2000 tonnes might be added in the next 10 years.

C. Developments in reprocessing technologies

The current generation of reprocessing plants has been continuously improved in regard to the
following [Ref. 5]:

i) flexibility (adaptations to increased burn-up, MOX treatment);

ii) reduction of effluent discharges and impacts on the environment;
iii) reduction of occupational exposure (e.g. during preventive maintenance and
inspections);
iv) reductions in waste volumes (of both HLW and intermediate level waste (ILW));
v) simplification of the process (e.g. through reducing the number of cycles needed);
vi) increased safety through reduced criticality hazards, and better proliferation resistance
by real time accounting of nuclear materials.

Nevertheless reprocessing systems still have to address some more challenging concerns, namely:
i) proliferation issues associated with producing separated plutonium;
ii) issues associated with high level waste, owing to the presence of minor actinides and
long-lived fission products (LLFP);
iii) economics and costs; and
iv) the processing of transuranic-rich fuels that are being developed for future advanced
nuclear reactors.

Much of the ongoing development work for reprocessing technologies deals with these issues. The
economic competitiveness of reprocessing and recycling of fissile materials depends on the price of
natural uranium and on the possible gains from reduced demands for repositories.

Collaborative international efforts are underway, including INPRO and GIF5, for developing
innovative reactors and fuel cycles that are competitive and safe, with simplified procedures for
managing radioactive waste and with features to increase the proliferation resistance of nuclear
materials. Similar to the evolution of innovative nuclear reactor development, reprocessing technology
is evolving in stages.

New wet processes are under development in which also the minor actinides and some LLFPs are
separated for later destruction (incineration) in different types of reactors, including fast reactors and
accelerator driven systems. Other methods are also being developed in which plutonium is never
separated in a pure form but always mixed with minor actinides for proliferation resistance. In a longer
time perspective different dry reprocessing technologies are also being developed, e.g. pyro-
processing, which could provide benefits in terms of economics, size and fuel cycle flexibility through
their higher radiation resistance. Several different lines of development are being considered and
tested on a laboratory scale. In some cases the step towards industrial implementation is fairly short,
while others will require substantial work before they can be introduced at an industrial level. The
following section gives some examples of advanced processes.

___________________________________________________________________________
5
INPRO = International Project on Innovative Nuclear Reactors and Fuel Cycles; GIF = Generation IV International
Forum
 Page 5

C.1. Wet processes developments

For wet processes there are two different lines of approach: (i) advanced separation of different
components in the high level liquid waste (HLLW) generated by the PUREX process (advanced
separation) or (ii) changing the chemistry in the first separation step so that only uranium is separated,
while keeping plutonium, minor actinides and fission products in the waste solution for later
processing (e.g. UREX6).

Advanced separation

The purpose of the ongoing development work on advanced separation methods is to remove minor
actinides and some fission products from the HLLW in order to reduce the radio-toxicity and heat load
in the final high level waste. The minor actinides will be incorporated in reactor fuel for transmutation
(nuclear incineration), while the separated fission products are conditioned for long term storage or
separate disposal.

The processes typically involve the following steps:

• recovering minor actinides (MA) and lanthanide fission products

• purifying the MAs from the lanthanides
• individually separating the MAs
• recovering Cs and Sr

Several processes using different types of extractants and solvents have been studied in different
countries and tested in hot facilities. Some examples are listed in Table 2. Each process uses its
specific extractant and solvent. Very high separation efficiencies will be required to reduce the long
term radio-toxicity of the remaining HLLW by a significant factor. In addition to high separation
efficiency the minimisation of secondary process waste, e.g. by using amides instead of phosphorous
reagents, is also an important goal.

Table 2: Review of advanced aqueous partitioning methods [Ref. 1, 6, 7, 8, 9, 10]

Process Purpose Country Special aspects
DIAMEX Extraction of minor France Diamide Extraction Process
actinides and Solvent based on amides as alternate to
lanthanides from phosphorous reagent
HLLW Generates minimum organic waste as the solvent
is totally combustible

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6
URanium EXtraction
Page 6

TODGA ditto Japan Tetra-octyl-diglycol-amide

Amide similar to DIAMEX
TRUEX Transuranic elements USA, Russia, Extraction by using Carbamoyl Methyl
(TRU) Extraction Japan, Italy, Phosphine Oxide (CMPO) together with TBP
from HLLW India
SANEX-N Selective Actinide France, Process for separating actinides from lanthanides
Extraction process Germany from HLLW by useing neutral N-bearing
for group separation (Institute for extractants, viz. Bis-triazinyl-pyridines (BTPs)
of actinides from Transuranium
lanthanides Elements
(ITU))
SANEX-S ditto China, Use of acidic S-bearing extractants, for example
Germany, India synergistic mixture of Cyanex-3017 with 2,2-
bipyridyl
TALSPEAK ditto USA, Trivalent Actinide Lanthanide Separation by
Sweden Phosphorus Extractants and Aqueous Komplexes
Use of HDEHP as extractant and DRPA as the
selective actinide complexing agent
ARTIST ditto Japan Amide-based Radio-resources Treatment with
Interim Storage of Transuranics
This process is made-up of: 1.) Phosphorus-free
branched alkyl monoamides (BAMA) for
separation of U, Pu; 2.) TOGDA for actinide and
lanthanide recovery and 3.) N-donor ligand for
actinide / lanthanide separation
SESAME Selective Extraction France, Japan Process for separating Am from Cm by oxidation
and Separation of of Am to Am(VI), subsequent extraction with
Americium by Means TBP for separation from Cm
of Electrolysis
CSEX Cs Extraction USA, France Using Calix-crown extractants
CCD - PEG Extraction of Cs and Czech, EU, Chlorinated cobalt dicarbollide and Poly-ethylene
Sr from the raffinate Russia, USA glycol (CCD-PEG) in sulfone based solvent is
planned for extraction of Cs and Sr from UREX
raffinate
SREX Sr Extraction USA Using dicyclohexano 18-crown-6 ether
GANEX Uranium extraction France Group recovery of all actinides based on branched
followed by group amide compound N,N-di-(2-ethyl-hexyl)-iso-
extraction of all butanamide (DOiBA) and subsequent DIAMEX /
actinides SANEX
UREX + Uranium Extraction USA A series of five solvent-extraction flow-sheets
+ other processes for that perform the following operations: 1) recovery
further separation of Tc and U (UREX), 2) recovery of Cs and Sr
(CCD-PEG), 3) recovery of Pu and Np (NPEX),
(4) recovery of Am, Cm, and rare-earth fission
products TRUEX, and 5) separation of Am and
Cm from the rare earth fission products (Cyanex
301).

___________________________________________________________________________
7
Cyanex refers to compounds belonging to the family of organo-dithio-phosphinates (R2PS2-).
 Page 7

FIG. IV-3. One of the strategies for treating PUREX raffinate under development at Commissariat à
l’énergie atomique (CEA), France.

Figure IV-3 shows the stepwise combination of different processes developed by CEA in France. For
the first ‘post-PUREX’ step, the co-extraction of minor actinides (americium and curium) and
lanthanides, the DIAMEX process is used [Ref. 7]. In the second step, SANEX, the actinides are
separated from the lanthanides, and in the third step americium is separated from curium. A process
called SESAME is under development for this. In the last step caesium and strontium are extracted
from the remaining waste stream.

During current reprocessing operations, neptunium is partly discharged with the fission products into
the HLLW and partly associated with the U and Pu stream. The purification of U and its separation
from Np is achieved in the second extraction cycle of the PUREX process. An advanced PUREX
process, PARC (PARtitioning Conundrum), is being developed with the main objective of separating
Np and Tc in the first extraction cycle.

Pure uranium separation

As an alternative to PUREX-based processes a series of new processes are being developed that
separate uranium (UREX) while keeping plutonium, minor actinides and fission products in the waste
solution [Ref. 10]. Subsequently all actinides can be recovered as a group. Also caesium and strontium
can be separated. These UREX based separation processes have become one of the key emphases in
the US DOE’s Advanced Fuel Cycle Initiative (AFCI), which provides the technical foundation for the
Global Nuclear Energy Partnership (GNEP). A similar process, GANEX8, is being developed in
France.

C.2. Pyro-chemical processes

Pyro-chemical processes were first investigated in the 1950s as an alternative to PUREX to increase
the radiation resistance and stability of material used in extraction processes. An initial pyro-chemical
process was constructed at the Experimental Breeder Reactor II (EBR-II) in the USA during the
1950s. Later many concepts for pyro-chemical partitioning were developed, and in some cases pilot
plants were built and operated. The techniques were based on using metals and salts at high

___________________________________________________________________________
8
Group ActiNide EXtraction
Page 8

temperatures: melt-refining, volatilisation, gas-solid reaction, fractional precipitation, vacuum

distillation, electro-deposition, electro-refining, electro-winning9 and others. This technology, which
has a lower separation factor, can possibly decrease reprocessing costs nonetheless by taking
advantage of the ability of fast reactors to use fuel with more impurities than would be acceptable in
thermal reactors. The advantages of some of these pyro-processes are:

• Adaptability to reprocess spent fuels, including MA based fuels, with shorter cooling periods
(this advantage relates principally to future fuel cycles),
• Ability to co-recover actinides largely in a single process,
• Compact plants that can accept several forms of fuel,
• Very short turn-around time for the fuel, and associated cost savings from the resulting
reduction of otherwise large fissile materials inventories,
• Generation of minimum transuranic waste,
• Very high intrinsic proliferation resistance for the fissile materials owing to:
• Limited purity of the end product, which limits its direct use in nuclear weapons,
• A built-in isotopic barrier because of the presence of isotopes with high decay
heat, high spontaneous neutron yield and lethally high radio-toxicity,
• Co-location of reprocessing and fuel fabrication facilities with the reactor.

However, the main challenges facing pyro-processes are the requirement for an oxygen- and moisture-
free plant environment, and the need to develop materials that will not only withstand high radiation
levels but have excellent resistance to high temperature corrosion in molten metals and molten halide
salts.

The common features of pyro-chemical processes are dissolution of spent fuel elements in a molten
salt bath around 500 to 800°C, followed by some degree of selective recovery of constituent elements
for recycling or conditioning. Semi-industrial scale reprocessing technologies based on electro-
refining processes (ERPs) were developed in the USA in the 1980s for U as well as (U,Pu) metal fuels.
Likewise, for UOX and MOX fuels Russia has developed the electro-winning process combined with
remote vibro-pack technology for fuel rod fabrication. These were tested in fast reactors in the 1990s.
A schematic diagram of the electro-refining cell and a flow-sheet for the ERP are shown in Fig. IV-4b.

In the molten salt refining process developed in the USA, the spent metallic fuel (U-Zr or U-Pu-Zr
alloys) is chopped into small pieces and loaded in the anode basket of an electro-refining cell with, as
the electrolyte, molten LiCl/KCl eutectic mixtures at around 773K. A cylindrical rod of low carbon
steel is used as the cathode. CdCl2 is added to the electro-refining cell to transfer most of the actinides
and fission products as chlorides to the electrolyte bath. On passing a current through the cell, the
uranium in the anode forms uranium ions in the molten salt electrolyte and then the uranium is
reduced and deposited as uranium metal on the cathode. After uranium recovery, the solid cathode is
replaced by a liquid cadmium cathode. Under this condition, electrolysis leads to co-deposition of U,
Pu, MAs as well as some lanthanide elements into the liquid cathode. More reactive fission products
remain dissolved in the salt phase. Fission products less reactive than actinides, namely noble metals
and zirconium, are not dissolved and remain in the anode basket (see Fig. IV-4a).

___________________________________________________________________________
9
Electro-winning and electro-refining processes are standard metallurgical processes for extracting and purifying
metals. In electro-winning a current is passed from an inert anode through a liquid leach solution containing the metal
so that the metal is deposited onto the cathode. In the electro-refining process, as the current passes through the anode,
which is made of impure metal, the metal dissolves into the solution and gets deposited as refined metal onto the
cathode.
 Page 9

b)
Spent fuel Spent fuel
(metal) (oxide)
Fresh fuel
MOX U , Pu, MA (metal)
product + Cd
Electro-chemical Salt & Cd removal
reduction by Distillation
U
U - Pu -
Chopping MA - FP
U product U - Pu -
MA
U-Pu-Zr-
Electro-refining + salt Injection
MA - FP
casting
Na removal U,Pu,MA recovery
(Distillation) (LiCl -KCl + Used salt ( LiC l- KCl
U, Pu, MA ) + U, Pu , MA, FP )
Cd-Li U, Zr
Na, Cs, Sr, etc. Multistage
Scrubbing
extraction
Oxidation Salt recycle Used salt
(LiCl-KCl) Cd-U-Pu-MA (LiCl - KCl + FP)

Zeolite column
(FP removal)

Zeolite + LiCL- KCl + FP

Na2O, Cs2O, SrO, …. Used mold
Salt waste
B(OH)3, Al2O3 (Quartz)
solidification

FIG. IV-4. a) Schematic of an electro-refining cell and b) the process flow sheet for an electro-refining
process under development at Idaho National Laboratory (INL), USA and Japan Atomic Energy
Agency (JAEA), Japan and ITU, EC

Recent technological development efforts [Ref. 11] in the USA range from laboratory-scale studies of
new processing concepts such as the electrolytic reduction of spent LWR oxide fuel to the
engineering-scale demonstration of high-throughput uranium electro-refining. Japan has a laboratory
scale facility for electro-refining metallic fuel [Ref. 12]. In addition, development work is underway
on extracting transuranic elements (TRUs) by pyro-chemical methods from HLLW generated from the
PUREX process applied to LWR fuels. Other Member States (China, Czech Republic, France, Korea,
India), as well as EC/ITU have also embarked on some of these pyro-chemical methods on a
laboratory scale. At the Research Institute of Atomic Reactors (RIAR) at Dimitrovgrad, Russia the
recycling of fuel at tonnage scale has been successfully demonstrated using a pyro-chemical method
based on the electro-winning process as part of demonstrating a closed fuel cycle with mixed oxide
fuels for the BOR-60 fast reactor. Another promising method is fluoride volatilization for processing
the TRU-rich fuels or targets that are being considered for a future generation of dedicated burner
reactors or accelerator-driven systems (ADSs).
Page 10

The development of pyro-chemical processes requires also the development of state-of-the-art

equipment that is suitable for applying such processes at an industrial scale. The path to industrial
utilization is thus perhaps longer for the pyro-processes than for the advanced aqueous processes.

D. Synergistic combination of different fuel cycles

There are several research efforts looking for ways in which different fuel cycles, both existing and
future, can efficiently complement one another for sustainable nuclear energy development. Aqueous
processing methods have very high throughputs and sufficient industrial maturity to handle large
volumes of discharged fuels from LWRs. However, they are less suitable for reprocessing fast reactor
fuel with short turn-around times. Pyro-chemical processes can handle spent fuels with short cooling
times as well as with very high MA content in a significantly smaller processing facility. Furthermore,
these processes can recycle TRU waste, thus reducing the volume of TRU waste that needs disposal.
Due to impure product recovery, the process is very much proliferation resistant. Thus, synergistic
combinations of aqueous partitioning steps with pyro-chemical processing as depicted in Fig. IV-5
could be a promising option in the future.

LWR Fast Reactor Cycle

LWR Fuel Treatment Metal Fuel

Spent UO2 / MOX for Fast Reactor
Fabrication

Li Reduction or
Reprocessing Electro-chemical
(PUREX) Reduction
Salt / Metal Fast Reactor
Separation
MOX Waste
U,Pu,MA

Denitration/ Electro-refining /
HLLW Spent Metal fuel
Chlorination Reductive extraction

Waste
Pyrometallurgical
Process
Treatment High Level Waste
/ Disposal

FIG. IV-5. Actinide recycling system by integrating oxide fuel treatment and the recovery of actinides
in HLLW.
 Page 11

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