Category Archives: Radioactive waste management and contaminated site clean-up

Radioactive waste

Radioactive wastes in the United States have many designations depending on their hazards and the circumstances and processes that created them. The NRC regulates most, but not all, sources of radioactivity, including LLW and HLW disposal, and residues from the milling of uranium and thorium. Uranium mill tailings, the final byproduct of uranium ore extrac­tion, are considered radioactive wastes. Radioactivity can range from just above background to very high levels, such as parts from inside the reactor vessel in a NPP. The everyday waste products generated in medical labora­tories and hospitals, contaminated by medical radioisotopes, is also desig­nated as RAW.

Tables 18.2 and 18.3 identify the types of commercial and DOE radioac­tive wastes. NRC regulations classify LLW in the commercial sector as Class A, Class B, and Class C. Radioactive waste owned or generated by the DOE is classified as HLW, TRU waste, or LLW. In addition, the DOE manages large quantities of uranium mill tailings and residual radioactive material. This residual radioactive material, which resulted from the Manhattan Project, is managed under the Uranium Mill Tailings and Radiation Control Act (UMTRCA) Title I. Waste may also contain hazardous waste constitu­ents. Waste with both radioactive and hazardous constituents in the United States is called ‘mixed’ waste (mixed LLW or mixed TRU waste). Generally, the source of HLW is reprocessed SNF. TRU waste consists of items such as protective clothing, tools, glassware, equipment, soils, and sludge con­taminated with man-made radioisotopes beyond or ‘heavier’ than uranium in the periodic table of the elements.

Table 18.2 US commercial RAW classification

Waste class

Description

HLW

The highly radioactive material resulting from reprocessing of spent fuel, including liquid waste produced directly in reprocessing and any solid material derived from such liquid waste containing fission products in sufficient concentrations and other highly radioactive material that the NRC, consistent with existing law, determines by rule requires permanent isolations

Class A LLW

Class A waste is determined by characteristics listed in 10 CFR 55(a)(2)(i) and physical form requirements in 10 CFR 61.56(a). (The US does not have a minimum threshold for Class A waste.)

Class B LLW

Waste that must meet more rigorous requirements on waste form than class A waste to ensure stability.

Class C LLW

Waste that not only must meet more rigorous requirements on waste form than Class B waste to ensure stability, but also requires additional measures at the disposal facility to protect against inadvertent intrusion.

GTCC LLW

LLW not generally acceptable for near-surface disposal.

AEA Section 11e. (2) byproduct material

Tailings or wastes produced by the extraction or concentration of uranium or thorium from any ore processed primarily for its source material content, including discrete surface wastes resulting from uranium solution extraction processes. Underground ore bodies depleted by such solution extraction operations do not constitute ‘byproduct material’ within this definition.15

a From the Nuclear Waste Policy Act of 1982, as amended. b Title 10 CFR Part 40, Domestic Licensing of Source Material (Section 40.4).

Nuclear research and test establishment facilities

There are two main nuclear research facilities in Canada: Atomic Energy of Canada (AECL) — Chalk River Laboratories (CRL), located in Chalk River, Ontario is operational, and AECL — Whiteshell Laboratories (WL), located in Pinawa, Manitoba is undergoing decommissioning. AECL is responsible for the long-term management of RAW generated by CRL, WL and the three partially decommissioned prototype reactors (i. e., Douglas Point, Gentilly-1 and Nuclear Power Demonstration, NPD), as well as for the low — and intermediate-level waste it accepts from off-site waste genera­tors on a fee-for-service basis. AECL is also responsible for managing its used fuel, including research reactor fuel and any used CANDU® fuel sent to its laboratories for examination, until the NWMO is ready to accept the waste for management in facilities constructed under the APM approach.

In 2006, the Government of Canada adopted a new long-term (70-year) strategy to deal with the nuclear legacy liabilities that have resulted from over 60 years of nuclear research and development carried out on its behalf at AECL sites. The overall objective of the long-term strategy is to safely and cost-effectively reduce the liabilities and associated risks based on sound waste management and environmental principles in the best interests of Canadians. The Nuclear Legacy Liabilities Program (NLLP) was estab­lished in 2006 and is being implemented through a Memorandum of Under­standing between Natural Resources Canada (NRCan) and AECL (NLLP, www. nuclearlegacyprogram. ca; Miller et al., 2008; Metcalfe et al., 2009). AECL’s ongoing LLW and ILW will be dealt with in waste management facilities that will be built under the NLLP.

At other nuclear research sites, RAW materials are segregated by licen­sees into short-lived and long-lived RAW. Short-lived RAW is stored on-site to allow for decay until it can be disposed of in a conventional manner. Long-lived RAW is kept on-site temporarily until a certain amount or volume is accumulated; thereafter it may be sent off site using a commercial service provider, as available, or transported to AECL-CRL for safe storage, also under a fee-for-service basis.

As of March 2011, there are seven operating research reactors in Canada (see Fig. 19.1). In the past, research reactors have typically used highly enriched uranium (HEU) fuel, obtained from the United States for the fuel cores. Within the last decade, some of the cores have been converted to low-enriched uranium (LEU) fuel as part of the Global Thread Reduction Initiative (see Section 1.4.3). The used fuel from the research reactors is either sent to AECL-CRL for storage or, in the case of HEU, returned to the United States for processing.

Prohibited waste

1. Liquids and gaseous substances will not be accepted.

2. Waste packages must not contain free-standing liquid.

3. No un-stabilized explosive or untreated pyrophoric material will be accepted.

4. No compacted, solidified or conditioned waste shall be accepted at solid waste operations (SWO) unless such waste has been subject to a quali­fied and NLM-approved conditioning process.

China: experience of radioactive waste (RAW) management

Z. FAN, China Institute of Radiation Protection, China, Y. LIU and J. WANG, Beijing Research Institute of Uranium Geology, China, G. REN, University of Hertfordshire, UK and W. E. LEE, Imperial College London, UK

DOI: 10.1533/9780857097446.2.697

Abstract: Progress in the management of China’s radioactive waste (RAW) is described, including waste generation, waste management policy, and current practices in regional disposal of low and intermediate level waste (LILW) and development of a geological disposal facility for hight level waste (HlW).

Key words: China radioactive waste management, geological repository, regulations and policies.

22.1 Introduction

China started its commercial nuclear industry in the early 1970s; however, development was slow prior to 2000. To meet the energy demands of its rapid economic growth and social development over the last 30 years, China has been building an electricity supply system with multiple sources. Coal — powered electrical plants still play a major role. Meanwhile, cleaner energy, including nuclear, will see significant growth considering factors of resource, transportation, environmental concern and climate change.

Decommissioning practice and issues

Nuclear facilities in the process of being decommissioned in Japan include Tokai-1 NPP of the JAPC, the Advanced Thermal Reactor ‘Fugen’ of the JAEA and the Plutonium Fuel Fabrication Facility (PFFF) of the JAEA. Hamaoka Nuclear Power Station Reactor’s No. 1 and 2 of Chubu Electric Power Company shut down in January 2009 and their decommissioning plans were approved by the METI in November 2009.

Pyrochemical wastes

In addition to the issue of treatment of surplus weapons grade materials, increased interest is being shown in the immobilization of special categories of waste arising from the pyrochemical reprocessing of Pu metal for weapons use. These differ from the wastes generated during the reprocessing of spent fuel as they can contain high concentrations of actinides together with substantial quantities of halides, particularly chlorides, as illustrated in Table 25.7, which gives the compositions of simulated salt wastes under investiga­tion at the UK’s Atomic Weapons Establishment (AWE).

Wastes containing large quantities of chloride are not amenable to immo­bilization in borosilicate glass because of the very low solubility of chlorides in this type of glass. Similarly, Synroc-type ceramics cannot be employed either due to low halide solubility.

Table 25.7 Compositions of AWE simulated pyrochemical reprocessing wastes (mass%)

Component

Type I

Type II

Type III

Type IV

HfO2 (PuO2

20.7

62.2

11.4

surrogate)

Ga2O3

28.0

9.4

10.5

Al2O3

9.8

1.7

2.2

Sm2O3 (Am2O3

4.6

11.7

1.0

surrogate)

MgO

6.3

10.1

FeO

1.5

0.7

Ta2O5

1.3

0.7

NiO

1.3

0.7

ZnO

35.7

SiO2

0.8

B2O3

0.8

CaCl2

80.0

CaF2

SmCl3 (PuCl3 and

20.0

10.4

5.0

8.5

AmCl3 surrogate) KCl

16.3

10.0

16.9

Source: Donald et al. (2007). British Crown Owned Copyright 2007/AWE.

Two approaches can be taken when dealing with this type of waste. One is to remove the halides prior to immobilization of the non-halide constitu­ents employing, for example, borosilicate or phosphate glass; the second is to accommodate the halides chemically in a suitable host. Halides can be removed by a number of methods, but one disadvantage of this route is that secondary waste is produced which must also be dealt with. One example is reaction of the waste with ammonium dihydrogen phosphate to yield ammonium chloride and water as by-products, together with a phosphate glass (Donze et al., 2000):

2NH4H2PO4 + MCl2 ^ MO. P2O5(glass) + 2NH4ClT + 2H2OT

Another example is use of lead silicate glass to yield lead chloride as a volatile by-product, the chloride reacting with PbO in the glass, and the resulting oxide dissolving in the glass (Forsberg et al., 1997):

3PbO + 2PuCl3 ^ 3PbCl2 T + Pu2O2

Iron phosphate-based glasses have also been suggested for immobilizing chloride wastes, but in the UK AWE’s experience, the bulk of the chloride is not incorporated chemically but is evolved during waste form processing, again generating a secondary waste. Calcium aluminosilicate-based glasses have also been suggested (Siwadamrongpong et al. , 2004) and have been shown to be partially effective in incorporating chloride constituents, immo­bilizing up to 17.5 mol% calcium chloride, for example (Schofield et al., 2008). Unfortunately, regardless of the amount of chloride in the initial batch, up to 30% of the chloride is evolved during the melting process, making this method no more attractive than methods suggested for remov­ing chloride prior to immobilization.

Alternatively, halides can be chemically incorporated into a number of ceramic hosts including chlorapatite, Ca5(PO4)3Cl and spodiosite, Ca2PO4Cl, with the actinides being incorporated into the substituted whitlockite-type phase (Donald et al., 2007), which is one of the methods being investigated at AWE. An alternative method involves occluding the halide species into a zeolite and heating above 800°C to form the sodalite mineral phase Na8(AlSiO4)6Cl2 (Lewis et al., 1993; Metcalfe and Donald, 2004). This method has been adopted by the Argonne National Laboratory (ANL) for immobilizing pyrochemical wastes arising from reprocessing of experimen­tal fast breeder reactor fuel, where salt-loaded zeolite is mixed with glass and converted into a monolith by either hot-isostatic pressing or pressure­less sintering. The phase assemblage produced by both processes is essen­tially the same, consisting of about 70% sodalite, 25% binder glass and 5% halite and oxide inclusions (Lewis et al., 2010). A similar method was inves­tigated by AWE for immobilizing weapons-related pyrochemical wastes but was rejected in favour of the phosphate route. In the case of the calcium phosphate immobilization route, waste powder may be reacted with calcium phosphate to yield a mixture of chlorapatite and spodiosite: for example:

PuCl3 + 8Ca3 (PO4)2 ^ 2Cas(PO4)зCl + 4Ca2PO4Cl + Ca6Pu(PO4)б

The resulting powder will subsequently be encapsulated in a sodium aluminium phosphate or similar glass to yield a monolithic product.

Fluidized bed steam reforming has also been suggested for treating halide-containing wastes (e. g., Jantzen, 2003). The product from this process is a highly durable waste (Jantzen, 2006) consisting of a number of feld — spathoid phases having cage stuctures (e. g., nephelines and sodalite), which contain the halides.

Germany: experience of radioactive waste (RAW) management and contaminated site clean-up

G. H. NIEDER-WESTERMANN and W. BOLLINGERFEHR, DBE Technology GmbH, Germany

DOI: 10.1533/9780857097446.2.462

Abstract: The Federal Republic of Germany has committed to the complete phase out of nuclear energy production by 2022. Considerable effort has been expended on developing deep geological repositories for radioactive waste (RAW) associated with energy production and industry. Three such repositories, Asse, Morsleben and Konrad for wastes with negligible heat generation exist in Germany. Asse and Morsleben are both being closed in accordance with the German Atomic Energy Act, while Konrad has been licensed to receive waste and is currently being constructed. An exploratory facility for the deep geologic disposal of heat generating radioactive wastes is located at Gorleben, Lower Saxony. Related repository design studies continue to progress and specialized full-scale waste handling and emplacement equipment has been designed and tested.

Key words: nuclear energy phase-out, German Atomic Energy Act, waste canisters, interim storage, deep geological repositories.

14.1 Introduction

Germany is the fifth largest economy in the world and the largest within the European Union (US CIA, 2011). Germany is also the largest generator of electrical energy in the European Union. In 2010 electrical energy gen­eration was 622.5 TWh, of which 22.5%, or 140.6 TWh, was produced from nuclear power generation (AGEB, 2010), approximately 57.6% from fossil fuels sources, 15.9% from renewables, and 4% from other sources (AGEB, 2010, 2011; ENS, 2011). Prior to the Daiichi Power Plant nuclear incident in Fukushima, Japan, in March 2011, Germany operated 17 nuclear power plants (NPPs) with a total net capacity of 20.49 GW (ENS, 2011); six are boiling water reactors (BWRs) and eleven are pressurized water reactors (PWRs). In response to the incident in Fukushima and in the face of an increased anti-nuclear atmosphere in German society, the federal govern­ment immediately ordered the removal of 8 NPPs from service in response to the unfolding crisis and committed to a phase-out of nuclear energy by 2022. As a direct consequence, the actual contribution of nuclear energy to

Germany’s electrical power generation is currently 11%. Prior to the Fuku — shima incident, Germany had planned on extending the life of the NPPs by an average of 12 years to 2036.

German nuclear energy production peaked in 2001 at 171.3 TWh with 19 nuclear power plants in operation at the time. Since then two power plants, Stade and Obrigheim, have been shut down and are currently being decom­missioned. Seventeen further power and prototype reactors have either been shut down and are in the process of decommissioning or have been completely decommissioned (BfS, 2011a). The decommissioned plants include all of the Soviet designed VVER (water-water energetic reactor) constructed and operated by the former German Democratic Republic (GDR); the two prototype thorium high-temperature reactors; the proto­type fast breeder SNR-300 nuclear reactor near Kalkar, Germany; as well as several BWRs and PWRs. The locations of Germany’s key nuclear sites are shown in Fig. 14.1.

In addition to nuclear reactors used for power generation, a total of 37 research reactors have been constructed and operated in Germany. The majority of the former research reactors operated at very low to low power generation levels (i. e., in the range of 1.0 x 10-7 to 1.0 MW). Of the remaining eight research reactors, five also operate at these very low levels. Germany also maintains three nuclear fuel cycle facilities, while 11 further facilities are either in decommissioning or have been com­pletely decommissioned (BfS, 2011a, 2011b). Since the end of the Second World War Germany has refrained from developing nuclear military capabilities.

Since 2002 the German federal government has been officially committed to a phase-out of nuclear electric power generation. Although the opera­tional lifespan of Germany’ s NPPs was initially extended by the current government, the events at the NPPs in Fukushima, Japan, have resulted in a change of course by the federal government and the phase out has been expedited. Germany will now complete its phase out from nuclear energy production by 2022.

Current organization (since 2006)

The Legislator decided in 2006 to endow the Agency with a clear frame­work (executive) for intervention on contaminated sites.

Law number 2006-739 of 28 June 2006 (ANDRA, 2006) relating to the sustainable management of radioactive materials and waste specifies the public service missions of ANDRA by setting three objectives:

• Determining and publicizing the national inventory of radioactive mate­rials and waste.

• Management of certain wastes from the general public, in particular when the public, totally foreign to any use of radioactivity, become holders of radioactive objects (by inheritance, for example) sometimes unaware of the radioactive nature of the objects which they hold (e. g., radium objects),

• The remediation of former radioactively contaminated (orphan) sites and the management of the waste generated.

The law included the principle of a State subsidy contributing to financing the missions of general interest entrusted to the Agency.

The financing mechanisms described above in Section 15.4.1 is replaced by an annual public subsidy securing stable financing of the operations and thus allowing the programming of multi-annual intervention according to the site prioritization. The public subsidy also allows total financing of the works, and makes the situation of certain private individuals easier (e. g., when they cannot finance, or only in part, the rehabilitation works to their property).

The public subsidy also allows financing of storage of polluted soils at the remediation sites and the storage of radium-bearing objects that require, in the absence of a definitive solution (disposal of LL-LLW — see Section 15.2.2), to be stored on dedicated sites (located on the CEA sites in Saclay and Cadarache). Of course, in parallel, ANDRA strives to minimize the volume of polluted soils coming from remediation sites.

To manage this work on remediation, a new department was created in ANDRA in January 2007 (within the Industrial Direction). Its role is to lead and coordinate the Agency’s work on the remediation mission. Delib­erations on the decision-making structure for the use of the State subsidy was the object of extensive work from 2006 to the beginning of 2007 with participants from the Ministry of Industry and from the Safety Authority. This work resulted in the creation of a National Commission for assistance in the Radioactive Area (CNAR) which expresses an opinion on the use of this public subsidy, on the allocation priorities for the funds, on the strate­gies of treatment of the polluted sites and on the questions of doctrine regarding the waste.

The functioning of this committee is similar to that of other structures with similar missions in the governmental sphere (such as those for envi­ronmental remediation). The CNAR, chaired by the Chief Executive Officer of ANDRA, includes representatives of the authorities (Safety Authority, the appropriate ministries, technical public institutions such as the French Technical Support Organization (‘Institut de Radiprotection et de Shrete Nucleaire’, or IRSN), NGOs: two environmental protection associations, elected representatives) and two qualified persons (a representative of a public institution and a specialist in remediation).

The CNAR was created by deliberation of ANDRA’s Board of Directors in April 2007. It met twice in July and September 2007 and immediately began to discuss operational issues.

In 2012, the structure remains active, unchanged, and is handling the remediation mission.

Sharing experience

The Environment Agencies’ Requirements Working Group (EARWG) was established in 2003 to share information regarding best practice in RAW minimisation. An objective of the UK LLW Management Plan is to identify and share waste minimisation practices in order to minimise the burden on the environment from disposal of radioactive wastes at the LLWR. In addi­tion to minimising waste disposals to the LLWR, the use of recycled materi­als rather than virgin resources is preferable because it saves energy, reduces emissions of greenhouse gases and other air and water pollutants and, of course, conserves natural resources.

There are a number of factors, including economic, regulatory and avail­ability that make the re-use and recycling of materials previously classified as solid RAW a challenging task. Nonetheless, segregation by decontamina­tion or physical removal may enable radioactive material to be removed from the bulk of low radioactivity material (i. e. high volume low activity or

exempt material). This means that only a relatively small volume of material needs to be classified as RAW, whilst the bulk of the low radioactivity mate­rial has the potential to be re-used or recycled. There is a range of physical, chemical, electrochemical and dismantling techniques that result in the segregation of solid material.

Both EARWG and the LLWR Strategy Group maintain websites to share information.

The SAFEGROUNDS (SAFety and Environmental Guidance for the Remediation of contaminated land On UK Nuclear and Defence Sites) learning network was established in 1998 and provides a forum for develop­ing and disseminating good practice guidance on the management of radio­actively and chemically contaminated land on nuclear and defence sites in the UK. SAFEGROUNDS is now well established and shares information via its website.

Partly arising from SAFEGROUNDS, the SD:SPUR (Site Decommis­sioning: Sustainable Practices in the Use of Resources) learning network was established in 2004 to develop through dialogue safe, socially, economi­cally and environmentally sustainable practices in the use of resources arising from the decommissioning of nuclear sites. The project has pub­lished guidance on the potential applications for the re-use and recycling of these wastes, and the factors controlling their supply and demand, and has developed a set of sustainability indicators that could be used by site operators when identifying and choosing between options for the manage­ment of these wastes. Information from SD:SPUR is shared freely through its website.

Submarines

There are seven redundant nuclear submarines laid up floating at Rosyth and current operations are focused on one-year, six-year and twelve-year maintenance routines for each submarine to ensure they are kept in a safe state and that they will be in a condition suitable for their eventual decom­missioning. The strategy for decommissioning the UK ’s fleet of nuclear submarines was the subject of a consultation exercise carried out in late 2011/early 2012 (MoD, 2011). No date for deciding on the chosen strategy has been made but there are two significant conditions which will affect the decision and its timing. Firstly, decommissioning will not commence until a storage solution for the ILW arising has been agreed. This is a joint MoD and NDA programme in itself. Secondly, berthing space for laying up redun­dant submarines will be full by 2020, so if decommissioning has not started, then further berthing facilities would be required. The current favoured option in the consultation is that the seven laid up submarines at Rosyth would be decommissioned there, but none of the submarines which are operational at present would go to Rosyth for decommissioning.

In 2000, a joint MoD and Babcock project team decided that the nuclear support facilities that would become redundant in 2003 should be decom­missioned with the objective of de-licensing the nuclear site area of 0.83 ha to allow future industrial use. The first operations, which took four years, were to characterise the radioactive contamination, agree on monitoring protocols with the regulators and obtain the necessary authorisations from SEPA. For thoroughness in characterisation, retired employees were inter­viewed for their knowledge of historical discharges or spills, health physics logbooks were checked and the GPS-linked ‘Groundhog’ monitoring system was employed.

Rosyth has an active waste accumulation facility (AWAF) for storing LLW and ILW. It also has a LLLE outlet from the end of one of the dock’s piers. Monitoring of the sediments in the tidal and non-tidal basins detected no significant radioactivity.

The first phase of decommissioning and demolition of redundant facilities was undertaken by contractors and completed in 2009 with 99% recycling of non-asbestos building materials. This has led to low volumes of LLW requiring disposal at LLWR. Contaminated metals were authorised by SEPA to be sent to Studsvik AB in Sweden for treatment. 96% by weight was recyclable by Studsvik and one tonne of LLW was received back which was disposed of at the LLWR. A major facility decommissioned and demol­ished was the health physics building which contained the LLLE treatment plant. As LLLE treatment is a continuing requirement, a mobile unit has been procured.

The ILW waste from the decommissioning to date is organic ion exchange resin which is being stored in AWAF in 1.2 m3 transport container tanks. The strategy agreed with regulators and LLWR is to condition these resins in cementitious grout directly in one-third height ISO containers. The mon­olithic wasteform is LLW which is acceptable for disposal at LLWR. On this basis, the AWAF could be closed in 2016.

The lifetime packaged LLW disposed of at LLWR is estimated to be around 183 m3.

Decisions on delicensing are in abeyance awaiting the determination of the strategy on the SDP.