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Waste sources and classification

11

materials such as equipment, tools, pipes, sludge, resins from water purification, protective clothing, etc. The only difference is that these materials contain radioactivity in one form or another.

However, the production of radioactive wastes is not limited to nuclear power generation, but also occurs in all areas that utilise radioisotopes (e.g., hospitals) or handle or produce NORM. Further, an area that is often not mentioned, due to political sensitivity, is waste arising from military applications. While the spectrum of radionuclides in military wastes may be different, the materials are generally no different to those seen in civilian and non-nuclear industries that use similar processes (e.g., even depleted uranium (DU), used in anti-tank shells among other munitions, is also used industrially).

Therefore, military applications, the nuclear industry, medicine and a range of other industries, as well as various research activities, all generate radioactive waste as a result of their operations.

2.4.1. Nuclear fuel cycle

Commercially, electricity has been generated by the nuclear industry for nearly 50 years, since the first Magnox reactor came on-line in the UK. Currently, around 20 per cent of the world’s electricity requirement in 31 countries is met by nuclear power (440 reactors, 366 GW(e) at the end of 2004; IAEA, 2005).

The civilian nuclear industry produces radioactive wastes from many sources and these can best be described by examining the nuclear fuel cycle (Fig. 2.1). This cycle

 

Fuel rods

 

 

 

 

 

 

Reactor

Spent fuel

 

 

 

 

 

Fuel

 

 

 

 

fabrication

 

 

 

Depleted

 

Pu

 

Storage

396 U-235

 

 

uranium

 

 

 

 

 

 

 

 

Enrichment

 

 

Reprocessing

 

 

 

 

 

 

 

 

Wastes

 

0.796 U-235

 

U

 

 

 

 

 

Vitrification

 

Conversion

 

 

 

 

to UF6

 

 

 

 

U3O8

 

 

Storage

 

 

 

 

Tailings

Mining

Disposal

Fig. 2.1. The nuclear fuel cycle showing all the processes from mining uranium ore to final disposal of radioactive waste (Uranium Information Centre, 2006).

12

D.F. McGinnes

describes each step from the mining of uranium through reactor operation and then either to recycling (in nuclear industry jargon, the ‘‘closed cycle’’) or direct disposal of spent fuel (once-through cycle) The waste produced (‘‘arising’’ in the industry jargon) from the commercial processes applied in each part of this cycle are discussed below:

2.4.1.1. Mining

The majority of mining waste arises as ‘‘tailings’’ or, in other words, the leftovers from the mining and extraction process consisting of the residues remaining after the uranium ore has been processed by milling and acid leaching to produce ‘‘yellow cake’’ uranium oxide, U3O8.

To put this in perspective, to provide fuel for 1 year’s operation of a typical large light water reactor (with an electricity output of 1 GW(e)), between 45,000 to 50,000 tonnes (100 per cent) of uranium ore are required to produce 200 tonnes (0.4 per cent) of yellow cake. This then leaves between 43,000 and 48,000 tonnes (99.6 per cent) of tailings requiring further management.

On completion of open-cast mining activities, the tailings are generally returned to the pit from where the uranium ore was originally extracted and the site rehabilitated for further use (see Fig. 2.2). For mines where the replacement of the tailings is not generally economically feasible, the storage facilities used to manage the tailings during mining operations are, generally, transformed into a long-term stable structure and the site rehabilitated for further use.

2.4.1.2. Fuel production

The production of fuel from yellow cake involves three activities: conversion, enrichment and fuel fabrication (Fig. 2.3).

The first stage of this process (Fig. 2.4) is the conversion of U3O8 powder (200 t) to UF6 (32 t), which is a gas at temperatures above 56LC; this is required for the enrichment process (centrifugation or diffusion) where the U-235 content of the gaseous UF6 is enriched from natural levels of 0.7 wt% to levels of between 2 and 4.95 wt%. In terms of the 1 GW(e) reactor mentioned above, this means that the 200 tonnes of concentrate produce 25 tonnes of enriched uranium containing 3–4 wt% U-235 and leaves 175 tonnes of depleted uranium containing 0.3 wt% U-235. Finally, the enriched UF6 (32 t) is converted to a UO2 powder (25 t) for compressing and sintering into fuel pellets, which are then fabricated into fuel assemblies (Fig. 2.5).

These activities produce small amounts of uranium-containing liquid and solid wastes that are packaged for storage and disposal. These are generally classified as L/ILW-LL.

The depleted uranium that results from enrichment operations is mostly recovered. A proportion can subsequently be reused, within the nuclear fuel cycle, by combining it either with recycled plutonium or using it to dilute highly enriched uranium from dismantled nuclear weapons to make fuel for nuclear reactors. In addition to the nuclear fuel cycle, due to its high density depleted uranium in its metallic form is also, as was noted above, used by the military sector as armour or casings for munitions.

2.4.1.3. Reactor operation

Assuming, once again, a typical large light water reactor of 1 GW(e) capacity, 200–350 m3 of L/ILW and 25 tonnes of SF will be generated per year.

Waste sources and classification

13

Fig. 2.2. (a) Open-cast uranium mine – before remediation (image courtesy of AREVA-NC). (b) Open-cast uranium mine – after remediation (image courtesy of AREVA-NC).

If the spent fuel is directly disposed of, this corresponds to a disposal volume of around 75 m3, following encapsulation. If the spent fuel is reprocessed, this produces around 3 m3 of vitrified waste (HLW), which is equivalent to a disposal volume of around 30 m3, following placement in a disposal canister (see, e.g., Johnson and King, 2003).

In terms of activity, 99 per cent of the total is contained in the spent fuel, consisting of activation and fission products and actinides (Table 2.3), and is either contained within the spent fuel matrix (vast majority) or in the fuel assembly structural materials (activation).

14

D.F. McGinnes

MINES

ENRICHERS

 

 

UF6

 

UF4

 

Pierrelatte (Drôme)

Mining

Cylinder 48Y

Concentrates

Avignon

 

 

Marseille

Malvési (Aude)

Narbonne

 

Malvesi and Pierrelatte conversion plants: certified ISO 9002 and ISO 14001

Pierrelatte plant (Comurhex company): the largest european fluorine producer, and the second biggest worldwide

Examples: WF6 used in electronics industry, F2N2 used to leak proof fuel tanks

Fig. 2.3. Example of the stages of fuel production (image courtesy of AREVA-NC).

Lowand intermediate-level waste is generally produced as a result of normal reactor operations, such as the cleaning of the reactor coolant systems and fuel storage ponds or the decontamination of equipment. Other wastes consist of various types of filters or metal components that have become radioactive as a result of their use in, or near, the reactor (Fig 2.6).

Feed

The UF6 gas partly crosses a membrane (filter)

U235F6 molecules are smaller, faster: they

cross the membrane more often, statistically

The gas is depleted in U235

Membrane

U238F6 molecules are bigger, slower: they cross the membrane less often, statistically

The gas is depleted in U235

Enriched

Exit

U238F6

U235F6

 

Feed

Depleted Exit

Enriched

 

Exit

The UF6 gas is centrifugated

U235F6 molecules are lighter and preferably move to the center of the rotor

Red bale / Gas enriched in U235

U238F6 molecules are heavier and preferably move to the periphery of the rotor

Yellow bale / Gas depleted inU235

Depleted Exit

Fig. 2.4. The fuel enrichment processes – diffusion and centrifugation (image courtesy of AREVA-NC).

Waste sources and classification

15

Fig. 2.5. Fuel assembly manufacturing – main steps (image courtesy of AREVA-NC).

Table 2.3

Sources of radionuclides within waste – an example from light water reactor spent fuel. Note that actinide decay chain daughter nuclides are not specifically listed as, over the time frames where they are important for a repository, their ingrowth via decay dominates.

Nuclide

Half-life (y)

Dec.

Nuclide type

Produced

Percentage

Relevance

 

 

 

 

from

of total

 

 

 

 

 

 

or activity

 

 

 

 

 

 

in spent

 

 

 

 

 

 

fuel (40y)

 

 

 

 

 

 

 

 

H-3

12.3

 

AP

Li (n, )

 

 

C-14

5730

 

AP

N (n,p)

 

 

Cl-36

3.0Eþ05

, þ

AP

Cl (n, )

 

 

Ar-39

269

 

AP

K (n,p)

 

 

Ca-41

1.0Eþ05

þ

AP

Ca (n, )

 

 

Mn-54

0.85

þ ( )

AP

Fe (n,d),

 

-dose rate

 

 

 

 

(d, )

 

 

Fe-55

2.7

þ

AP

Fe (n, )

 

 

Co-60

5.3

( )

AP

Co (n, )

 

-dose rate

Ni-59

7.5Eþ04

þ

AP

Ni (n, )

 

 

Ni-63

101

 

AP

Ni (n, )

 

 

Se-79

1.1Eþ06

 

FP

 

 

 

Kr-85

10.8

( )

FP

 

2.0 ( )

-dose rate

Sr-90

28.6

 

FP

 

16.7 ( )

 

Y-90

secs

 

Sr-90

 

16.7( )

heat

 

 

 

 

 

 

output,

 

 

 

 

 

 

-dose rate

 

 

 

 

 

 

 

(Continued)

16

 

 

D.F. McGinnes

 

 

 

Table 2.3

 

 

 

 

 

 

(Continued )

 

 

 

 

 

 

 

 

 

 

 

 

 

Nuclide

Half-life (y)

Dec.

Nuclide type

Produced

Percentage

Relevance

 

 

 

 

from

of total

 

 

 

 

 

 

or activity

 

 

 

 

 

 

in spent

 

 

 

 

 

 

fuel (40y)

 

 

 

 

 

 

 

 

Mo-93

4000

þ

AP

Mo (n, )

 

 

Zr-93

1.5Eþ06

 

FP

 

 

 

Nb-93m

16.1

 

FP

 

 

-dose rate

Nb-94

2.0Eþ04

( )

AP

Nb (n, )

 

-dose rate

Tc-99

2.1Eþ05

 

FP

 

 

 

Ru-106

1.02

 

FP

 

 

 

Rh-106

secs

( )

Ru-106

 

 

-dose

 

 

 

 

 

 

rate, heat

 

6.5Eþ06

 

 

 

 

output

Pd-107

 

FP

 

 

 

Ag-108m

418

þ ( )

AP

Ag (n, )

 

-Dose

 

 

 

 

 

 

rate

Sn-121m

55.0

 

FP

 

 

 

Cd-113m

14.6

 

FP

 

 

 

Sn-126

2.3Eþ05

 

FP

 

 

 

Sb-125

2.8

( )

FP

 

 

-dose rate

Te-125m

0.16

 

Sb-125

 

 

-dose rate

I-129

1.6Eþ07

 

FP

 

 

 

Cs-134

2.1

, þ ( )

FP

 

 

-dose

 

 

 

 

 

 

rate, heat

 

2.3Eþ06

 

 

 

 

output

Cs-135

 

FP

 

 

 

Cs-137

30.2

 

FP

 

26.2 ( )

heat output

Ba-137m

secs

 

Cs-137

 

25.0 ( )

-dose

 

 

 

 

 

 

rate, heat

 

 

 

 

 

 

output

Ce-144

0.78

( )

FP

 

 

-dose rate

Pr-144

secs

( )

Ce-144

 

 

-dose

 

 

 

 

 

 

rate, heat

 

 

 

 

 

 

output

Sm-151

93.0

 

FP

 

 

 

Eu-152

13.3

, þ ( )

FP

 

 

-dose rate

Eu-154

8.8

, þ ( )

FP

 

 

-dose

 

 

 

 

 

 

rate, heat

 

 

 

 

 

 

output

Eu-155

4.8

 

FP

 

 

 

Ho-166m

1200

 

FP

 

 

 

U-234

2.5Eþ05

 

AC

 

 

 

U-235

7.0Eþ08

 

AC

 

 

criticality

U-236

2.3Eþ07

 

AC

 

 

 

U-238

4.5Eþ09

 

AC

 

 

 

Np-237

2.1Eþ06

 

AC

U-238

 

 

Pu-238

87.7

 

AC

 

35.8 ( )

heat output

Pu-239

2.4Eþ04

 

AC

U-238

3.3 ( )

criticality,

 

 

 

 

 

 

heat output

Pu-240

6563

 

AC

Pu-239

5.5 ( )

heat output