THE TREATMENT OF WASTES AT SELLAFIELD FOR SAFE STORAGE AND DISPOSAL

M Colder
BNFL Sellafield UK

J Palmer
United Kingdom Nirex Limited

ABSTRACT

British Nuclear Fuels plc (BNFL) manages and operates facilities for the reprocessing of spent nuclear fuel at Sellafield in the north-west of England. Over the past 40 years, a number of liquid and solid wastes have been generated and safely managed in a raw form within a series of silos and stores. Since the 1980's, BNFL has embarked on a major programme of development, design, and construction of new facilities to retrieve and treat radioactive wastes from ageing stores. A number of major plants have been, or are being, constructed to condition wastes in a form that will facilitate their continued safe on site storage and their eventual safe transport to, and disposal in, the deep waste repository planned by Nirex, the United Kingdom (UK) radioactive waste disposal agency.

This paper describes the work carried out by BNFL and Nirex to evaluate the safety of waste packages against the safety requirements of on-site storage, transport and disposal. Waste forms discussed include cement-immobilised wastes such as effluent treatment sludges and fuel cladding wastes and supercompacted wastes including a novel compacted dried-sludge waste form. Results of programmes evaluating waste form integrity and releases under impact and fire are given and the use of arising data in safety assessments are discussed.

INTRODUCTION

In the UK, BNFL is involved in all activities of the nuclear fuel cycle. At BNFL's largest site, Sellafield, operations mainly associated with fuel reprocessing have taken place for over 40 years,. These activities have generated a wide range of radioactive wastes and account for about two-thirds of the intermediate level waste (ILW) that will arise in the UK. ILW lies between the categories of high level waste (HLW) which comprises the liquid from the first cycle of reprocessing, and low level waste (LLW) which are defined as having activity contents below 12 GBq/te b g and 4 GBq/te a . HLW is vitrified at Sellafield and most of the UK's LLW is disposed of at BNFL's site at Drigg near Sellafield.

In the UK, the Nuclear Industry Radioactive Waste Executive was formed in 1982 and incorporated as a private limited company - United Kingdom Nirex Limited (Nirex) - in 1985. Its mission is to facilitate the final disposal of ILW and certain LLW and to investigate and develop disposal concepts and facilities.

A key objective for both BNFL and Nirex is to ensure that the treatment, immobilisation and packaging of waste, prior to a deep repository becoming operational, will produce packages that will be acceptable for ultimate disposal.

The work carried out by BNFL and Nirex to develop waste packages that can meet the safety requirements during production, storage, transport and ultimate disposal is described below. Included is a summary of existing waste management strategies and waste treatment processes and plants. The limitations of these technologies for heterogeneous wastes are highlighted and the development of alternative complementary processes are discussed. In particular, practical studies to develop and support the disposal of a novel supercompacted sludge waste form are discussed.

BNFL INTERMEDIATE LEVEL WASTE STRATEGY

Detailed technical studies by BNFL in the early 1980s highlighted the benefits from the early packaging of wastes and subsequent storage of waste in an encapsulated form, as this represented a reduction in the risk level, savings in lifetime costs and reduced dose uptake to operators. As a result of these findings, BNFL developed a strategy to treat ILW by direct encapsulation. Current and future ILW arisings would be treated as they arose with historical wastes retrieved and conditioned when appropriate. The timing for treating historical wastes would depend on the safety of continued storage in an unconditioned form and the availability of conditioning plants at Sellafield.

The adopted strategy is to produce essentially monolithic products that will maintain their integrity during on-site storage and a 50-year operational period in the disposal environment, plus being capable of meeting the requirements for transport to, and final disposal in, the deep geological repository. It has therefore been important for BNFL to work closely with Nirex, the company responsible for developing the transport and disposal systems.

WASTE TREATMENT PROCESSES

On-going reprocessing operations at Sellafield lead to a number of well-defined wastestreams requiring encapsulation. During the 1980s, processes and plants were developed to treat and condition these wastes based on their physical form.

Solid wastes (such as fuel cladding from decanning operations) were to be placed into stainless steel drums and immobilised using carefully formulated cementitious grouts. Grout infiltration was facilitated by vibration, the whole process being known as vibro-grouting.

Liquid and slurry wastes (such as effluent treatment flocs and pond sludges) were to be homogenised, metered into drums containing a sacrificial mixing paddle, and mixed with specially blended cement powders. This process was referred to as in-drum mixing.

Based on these technologies, the following ILW conditioning plants have been built and are currently operational: The Magnox Encapsulation Plant (MEP) for treating solid magnox swarf wastes; the Waste Encapsulation Plant (WEP) for treating solid fuel hulls wastes, effluent treatment slurries and raffinate purification slurries; and the Waste Packaging and Encapsulation Plant (WPEP) to encapsulate routine arisings of effluent treatment flocs.

The products produced by these plants are cementitious monoliths where the radioactive activity is immobilised by intimate mixing with the cement matrix. Overall containment and handling features are provided by a stainless steel drum.

Extensive research work by both BNFL and Nirex on these types of waste form has been carried out to assess release fractions from such packages during normal operations and accidents. This work has shown releases to be low, with accident releases increasing progressively in a predictable manner with increasing severity of the accident. For example, following a 25 meter drop, particles generated within the drum of less than 100 microns (i.e., of a size capable of being resuspended and dispersed) represent approximately one millionth of the original waste inventory, showing the potentially available source-term for accidental releases to be extremely low. These release data have subsequently been used in safety assessments for a generic disposal facility and has been shown to be consistent with the requirements foreseen as being necessary for the safe transport and disposal of waste.

In addition to operational factors, the effect of these packages on post-closure repository performance has been assessed. Here, the high alkalinity of the cement grout is beneficial, reducing the concentration of key radionuclides by up to five orders of magnitude and suppressing microbial activity (and its associated gas generation). This, combined with the low permeability of the matrix which restricts radionuclide migration and corrosion rates of metals, also means that the long-term disposal requirements foreseen by Nirex could be satisfied by these packages.

Having developed plants and technologies to manage the current and future waste management liabilities, attention was focused on applying the existing plants and now- proven technologies to managing the historical liabilities of wastes that had accumulated and been stored at the site since its initial inception in the 1950s. A number of these historical wastes are well defined and are suitable for routing directly to existing facilities with minimal pre-treatment following retrieval. However, some historical wastes on the Sellafield site consist of a complex mixture of solids and viscous sludges which are not readily compatible with either the vibro-grouting or in-drum mixing processes. Therefore, initial process studies concentrated on retrieval and treatment processes that can segregate the waste mixtures into well-defined sludge and solids streams that are consistent with the feed requirements of the existing plants. One such waste stream was corroded magnox fuel cladding which had arisen from underwater storage of the magnesium alloy cladding for over 20 years. In addition to the cladding itself, the wastestream contains irradiated uranium fuel adhering to the cladding or present as discrete fragments of broken fuel elements, residues furniture such as fuel rod-end pieces, springs etc. Miscellaneous engineering wastes have also been added to the waste storage silos over the years. Consequently, a systematic programme to investigate process options for treating this wastestream was undertaken. The first treatment option considered was based on wet settling. Later, a process based on drying and compaction was also investigated. The next section describes the advantages and disadvantages of the wet settling and drying/compaction processes for treating corroded magnox fuel cladding wastes.

ORIGINAL TREATMENT PROCESS - WET SETTLING

Background

The wet settling concept was devised in 1991 to treat ILW stored at Sellafield. It was developed to segregate ILW into two fractions, one solids based, the other sludge based. These fractions could then be processed using treatment principles and technology described previously.

The process also had advantages in that the technologies adopted were consistent with existing processes operated on site and thus raised few new safety issues. One of the main safety issues associated with this waste stream was the presence of a pyrophoric compound, uranium hydride, a corrosion product of uranium. Conventional practice was to keep all uranium damp to prevent any uranium hydride present from reacting with air and igniting. This requirement was readily achieved in the wet settling process.

Preliminary discussions were held with the Regulators on processing and on-site storage and Nirex with regard to disposal to appraise them of BNFL proposals.

Process Description

The key stages in the wet settling process were:

Process Critique

As detailed process and engineering design progressed during 1992, a number of major problems were encountered.

  1. The sludge conditioning process was complex and problematic to engineer.
  2. Significant volumes of liquid effluent were produced during the conditioning process.
  3. Sludge volumes were increased during the conditioning process resulting in significantly more drums of waste being produced for encapsulation than had previously been predicted. The extent of volume increase was dependent on the chemical composition and particle size of the sludge (which in turn was a function of the amount of shear introduced into the process), hence the number of drums produced was also less predictable.

Despite an extensive research and development programme focusing on process and product quality concerns, robust solutions to the issues listed above were not forthcoming. By late 1992 a decision was taken to explore other processing solutions.

Early in 1993, following a Value Engineering and Optioneering exercise, the Drypac concept was adopted as the reference process to treat corroded magnox fuel cladding wastestreams.

REVISED TREATMENT PROCESS - DRYPAC

Background

The Drypac concept consists of a segregation phase similar to the wet settling process to produce sludge/solids fractions. Sludge wastes are then dried to remove free water and compacted to reduce the overall volume of waste for encapsulation. Solid wastes are also compacted. The net result of the process is to concentrate activity in each package. Due to the novelty associated with the process, discussions commenced with Nirex regarding disposal and UK Regulators with regard to on-site safety at a very early stage.

Process Description

The key stages in the Dryac process are:

A schematic representation of the Drypac process is given in Figure 1.

Fig. 1. A schematic representation of the DRYPAC process.

Process Critique

In comparison to the wet settling process, the Drypac process has many advantages, including:

From a regulatory perspective two key issues of concern were:

From a Nirex perspective the concept where the waste is not ultimately grouted but compacted to form an ingot or puck, which is then surrounded by a high integrity grout annulus, raises a number of novel issues when assessing the operational and post-closure implications. These concerns primarily focused upon:

Development Work

To address the Nirex and regulatory concerns summarised above, a substantial R&D programme has been carried out. This has focused on safety and product quality issues as follows:

Safety Issues

Laboratory and full-scale trials have been performed to confirm the behaviour of waste materials in the drying process and enable a safety case to be made for the Drypac process.

Results

Uranium reacts with water to produce oxide, hydrogen and, under conditions of free water access, small quantities of hydride. The corrosion process thus results in a thin film of hydride being formed on the surface of the parent metal, covered by a protective coating of oxide.

When exposed to air the oxide coating limits the rate of oxygen access to the hydride layer. This results in a very slow reaction process - the hydride is effectively passivated. Trials based on the Sellafield Drypac Process drying process revealed that any uranium hydride initially present, would react slowly and be completely converted to oxide by the end of the drying cycle. Any risks associated with ignition of uranium hydride in the drying process were therefore eliminated.

The off-gas system is designed to extract hydrogen and ensure that the lower flammable limit in the dryer unit will not be exceeded. Full-scale development trials have confirmed the adequacy of the proposed off-gas system design, enabling a safety case to be constructed.

Product Quality Issues

The following work has been carried out to provide process/engineering data to the BNFL design teams and Nirex:

Small and full-scale trials have shown that the dried waste forms a monolithic block within the puck when compacted (see Fig. 2).

Fig. 2. Section of waste puck containing dried and supercompacted sludge.

The performance and release from these pucks during accidents have been assessed and compared to conventional cementitious waste forms through a series of impact and fire tests. Results have shown releases from this compacted waste itself to be higher than for typical cement waste forms by between one to two orders of magnitude, although the releases are progressive and increase with increasing energy input and are thus predictable. In the case of the Drypac product, however, the waste form break-up is not the only key parameter affecting safety during accidents. The compacted waste is contained in a double shell stainless steel drum with a high integrity grout annulus which affords substantially enhanced performance compared to conventional drums.

Full-scale impact trials and fire modelling work have shown the energy imparted to the compacted waste is substantially lower than for conventional-packaged waste and, under anticipated accident conditions, releases are actually lower and well within the foreseen requirements for operation of a deep waste repository and associated waste transport.

In addition, any hydride formed during storage was found to be limited by water availability, and rapid oxidation would be prevented by the robust design of the package and the monolithic nature of the compacted sludge. Hence, the risk from uranium hydride formation on repository safety was judged by Nirex to be low and acceptable. Examples of typical impact test performance are shown in Figure 3.

Fig. 3. Impact performance of DRYPAC packages (25m drop).

Figure 4 shows the results from thermal modelling of SDP packages and shows that the presence of the grout annulus affords good protection to the waste in fire accidents.

Fig. 4. Fire performance of DRYPAC waste packages.

With respect to post-closure performance, the compacted sludge waste form has been assessed against its potential release activity with time into the repository near-field. The assessments concluded that careful package design and limiting the contents of expansive waste components will prevent packages from breaching for sufficiently long periods to allow short-lived soluble species such as Cs-137 and Sr-90 to decay to insignificant levels. For key longer-lived species such as U-238, the concentration of materials in solution has been assessed to still be low due to the alkaline pH buffering and strong sorption provided by the magnesium hydroxide component of the waste. Therefore, post-closure assessments concluded that this packaging concept is capable of providing acceptable performance for this waste, despite the absence of intimate encapsulation. As a result of this work, construction of the $600 million Sellafield Drypac Plant commenced in 1996 and should become operational in 2003. The suitability of this packaging concept for other historical wastes is currently being investigated.

CONCLUSIONS

Based on conducted research and analyses, BNFL has reached the following conclusions:

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