A dissertation submitted to the Department of Physics, University of Surrey, in partial fulfilment of the degree of Master of Science in Radiation and Environmental Protection



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Table 6
Table 6 shows the dose rates calculated by Microshield. The build-up factor is assumed to be within the source and the program is able to re-create the dimensions of the RSV and automatically calculate the dose rate given the activity, which is different for each RSV.



RSV Number

C-14 Solid

C-14 Liquid

H-3 Solid

H-3 Solid

Fe-55

Co-60

Ni-63




MBq

MBq

MBq

MBq

MBq

MBq

MBq

























1

1435

3

194

580

84

44034

19

5

36197.2




90.46




3190.59

9187.94

1576.1

6

695




72




3356

4480

456

8

1843.55




2312.68




71.21

368.54

228.67

10

702




109




12655

10560

923

11

27




142




5409

9861

277

12

8604.42




6653.95




1628.01

1293.06

474.67

19

133




100




66329

86794

6429

23

130




45




672

48769

4665

24

29




123




4608

21150

1145

25

113




13




11

25921

46

27

1854.75




18869.92




1502.94

1064.39

11.23

30

65




158




72800

235993

6121

32

403




4644




469

160021

222

33

57




46




61

218

10

35

17.9




51.1




372.76

998.31

79.22

36

5948




54




34651

12519

1130

37

42




160




1342

189594

81

38

990.7




741




939.7

9778.74

59.6

40

97.8




35.4




1364.43

15840.85

972.98




59385.32

3

34614.51

580

211516.64

888445.83

24926.47

























100.00%

59382.3507

2.99985

34612.779

579.971

211506.06

888401.41

24925.224

























0.01%

2.969266

0.00015

1.7307255

0.029

10.575832

44.422292

1.2463235

Table 7
Table 7 shows the difference in total radionuclide activity when a HEPA filter is used.

HEPA filters remove 99.99% of radionuclide content and so the total radionuclide content for all 20 RSV’s is shown along with the HEPA filter totals.




Figure 14
Figure 16 is a cost comparison and highlights the fact that maintenance on the resins which are currently stored at Devonport are costing double the amount of money compared with the other two prospective options.

OPTION

POSITIVES

NEGATIVES

Option 1

Authorisations are in place

14C content high, some resins need to be stored for years See table 2

Process is budgeted for annually

Very expensive to dispose of 14C See table 3

Waste not stored passively and does not satisfy the regulators

Option 2

Can be used to treat difficult wastestreams

Costs £3 million to build

Removes >98% 14C

Devonport will need to apply for increased discharge limits

Destroys chelating agents

HEPA filters are used creating a secondary waste and could pose a problem for operator dose on handling

Small size makes it easy to accommodate







There is space on the existing NLS







Simple Design

Potential for mass volume reduction and associated economic benefits

Option

Positives

Negatives

Option 3




Cannot process large volumes of waste

Some processes are unable to destroy chelating agents

Chemicals can be expensive

Many chemicals can be irritant and may pose a Health and Safety concern

Option 4

Has the ability to destroy even the most difficult carbonaceous material

May need further treatment to treat the ash

Very good for reducing waste volume

Involves very high temperatures and could pose a Health and Safety concern




Ash can become very active if the feed material is not managed

HEPA filters required to reduce emitted radionuclides with associated operator handling concerns

Condensate collects, producing a secondary waste stream, along with filters, filtration material, adsorption material, liquid scrub solutions and blowdowns.




Expensive materials needed in construction in order to prevent corrosion

Option 5

Will be a very large project, providing employment for hundreds of people over many years

A multi-billion pound project

Has backing from the NDA and the IAEA

Only certain areas have the correct geological rock formation to house a repository

Reliable waste packaging and engineered controls will compliment security of the geological barrier

The project could take many years to implement

Repository design includes the option of retrieval for future processing

This is only an interim solution until a better solution can be found

Waste would be stored passively




Figure 15





Winfrith

Devonport

Favoured Site

Current Facilities

Prototype ModulOx plant

LLW cementation plant



Neither

Winfrith

Waste Management Capabilities

This is a core activity on this site. Treats and conditions waste from other UK sites.

Effluent treatment available.



Management of own waste.

Effluent treatment available.



Winfrith

Authorisations

UKAEA site currently has a 300GBq gaseous discharge limit. Current ModulOx plant is an authorised discharge location, but a specific 14C authorisation for AEA Technology will be required.

Authorisation for 42 GBq 14C gaseous discharge. Specific authorisation for new plant would be required.

Either

Other MoD liability waste.

Receives radioactive waste from wide variety of sources. Could treat other similar waste streams from other MoD sites.

May be difficult or impossible to gain new regulatory approval to receiving waste from other nuclear licensed or MoD sites for treatment, as waste treatment is not a core activity or recognised function of the dockyard.

Winfrith

Figure 16
The figures used in this project are current with the resins in storage now, but the activities will change according to half-lives etc. There may be up to a 20% error margin on these resins but this is a best estimate. The figures have been used to calculate the approximate doses that exist and could therefore be scaled accordingly when quantities are known should any additional facilities be put in place. The figures prove that the doses to operators are low and that it would be possible to implement a new plant and still keep operator and public doses to below the limits set by Devonport.
Conclusions

It is possible to develop a new disposal route which conforms with government policy and regulatory guidance on radioactive waste management.

The ModulOx plant so far seems to offer the best solution, and could potentially be sited at both Devonport and Winfrith. This could be the quickest solution to implement out of the 5 options studied.

Broadening the treatment process of chelated resins to include high 14C resin waste satisfies management principles concerning waste accumulation on site and the use of existing routes as necessary.

There are two major drawbacks which would affect the implementation of a new facility on site. Firstly, an authorisation would need to be sought from the regulators to allow the discharge of increased amounts of 14C. Without this discharge authorisation, the facility cannot be implemented.

Secondly, there is no ModulOx plant that DRDL or the MoD can have immediate access to and therefore cannot guarantee long-term access. It may therefore be difficult to achieve the financial support required for a new facility.



Table 8 [35]
Winfrith already has a prototype plant, authorisations and financial support. According to table 6, this could be the most logical site for ModulOx treatment and conditioning of treated waste for disposal to Drigg.

If the‘store, treat and dispose’ method fails for any particular resin watestream, then a back-up plan will need to include the development of a long-term conditioned waste store with an immobilisation plant on the Devonport site.

A deep geological repository could be a good option for interim storage until a better, more environmentally safer option can be found. If the repository was never intended to be sealed then it would be easy to recover the waste for further processing and may also have a better effect on the public and could help in convincing them that this was a conceivable way forward.
Figure 15 shows the projected costs of 3 of the options studied. It can be concluded that despite the ModulOx plant costing ~£3 million initially, it will, in the long-term cost less to maintain than the current method. There is also the possibility of processing other sites waste if authorisation can be granted, allowing the company to make a profit out of the plant.

References

1 Waste Water Engineering Treatment, Disposal, Reuse. 3rd Ed. 1991. Singapore. Metcalf & Eddy. Mc-Graw-Hill Int. Ed’s Civil Engineering Series.


2 Immobilisation Science Laboratories, University of Sheffield. August 2007. Report prepared by Alstec as part of Rosyth resin treatment.
3 Waste Management Strategy Report, Integrated Waste Strategy for the Devonport Site Environmental Management. May 2009. M. Leisvik
4 Available at: www.world-nuclear.org/sym

[Accessed on 3rd June 2009]


5 Devonport Royal Dockyard Limited, Disposal of solid radioactive waste directly (or via Sellafield) to the low level waste repository near Drigg. B. Wright and K. Watterson

FP-19-12-000


6 Perry’s Chemical Engineers Handbook. 7th Ed. R.H. Perry and D.W.Green. 1997. USA
7 Division of Nuclear Physics, AMS and Radiating Physics Group.

Carbon-14 generated by Nuclear Power Reactors. Investigations including ion exchange resins and environmental samples. A Magnusson. 2005.


8 Environment Agency. Certificate of Authorisation and Introductory Note. Authorisation Reference AN7104/CC3093. Devonport Royal Dockyard Limited. 01-06-2009
9 BPEO Study on Management Options for spent Resins. Serco Assurance, Oxfordshire.June 2005
10 Development and Deployment of the ModulOx process for the destruction of organically contaminated wastes. T.J. Abraham, M. Williams and J. Wilks. WM’05 Conference, Feb.27th- Mar.3rd 2004
11 Design and Operation of Radioactive Waste Incineration Facilities. International Atomic Energy Agency. Vienna. 1992. [online]

Accessed at http://www-pub.iaea.org/MTCD/publications/PDF/Pub921e_web.pdf

[Accessed on 2nd September 2009]
12 Department for Environment Food and Rural Affairs: White Paper on Managing Radioactive Waste Safely [online] June 2008.

Available at http://www.defra.gov.uk/ENVIRONMENT/radioactivity/waste

[Accessed 8th July 2009]
13 The Uranium Institute 24th Symposium

8-10th September 1999; London. The Deep Geological Repository; an Unavoidable and Ethically Correct Solution.


14 Environmental Health and Safety. Radiation Safety Manual for Laboratory Users. Appendix B: The Characteristics of Common Radioisotopes [online] Princeton University.

Available at:http://web.princeton.edu/sites/ehs/radmanual/radman_app_b.htm#h3

[accessed 28th July 2009]
15 HMNB Devonport [online]

Available at:http://en.wikipedia.org/wiki/HMNB_Devonport

[Accessed 27th July 2009]
16 TD-PSC-410

Nuclear Utilities Building Facilities Plant Safety Case. Issue 2. 01-09-2006.


17 SLG-PSC-420

Core Pond Water Treatment Plant Safety Case. Issue 2. 15-11-1996.


18 SLG-PSC-510

Effluent Receipt and Transfer Safety Case. 12-03-1998.


19 SLG-PSC-610

Reactor Systems and Processes Plant Safety Case, Volume 1, Active Jet Vacs. Issue 2. 01-05-1997.


20 TD-PSC-680

Movement of Radioactive and Contaminated Items on Licensed Site. Issue 1. 01-07-2003.


21 SLG-MNC-1100F

Nuclear Transfers Pre-Operational Safety Report in Support of the Vanguard Class. Issue3 01-05-2002.


22 SLG-PSC-310

MODIX Decontamination Plant Safety Case. Issue 4. 01-01-2003.


23 Argonne National Laboratory, EVS. August 2009. [Online]

Available at: http://www.ead.anl.gov/pub/doc/carbon14.pdf

[Accessed on 11th August 2009]
24 Argonne National Laboratory, EVS. August 2009. [Online]

Available at: http://www.ead.anl.gov/pub/doc/Cobalt.pdf

[Accessed on 11th August 2009]
25 Argonne National Laboratory, EVS. August 2009. [Online]

Available at: http://www.ead.anl.gov/pub/doc/Ni63.pdf

[Accessed on 11th August 2009]
26 SRS Facts about the Savannah River Site. September 2005. [Online]

Available at: http://www.srs.gov/general/news/factsheets/het.pdf

[Accessed on 11th August 2009]
27 http://www.2.nsyusu.edu.tw/COHP/laws/laws_bank/MSDS_sheets/Fe-55.pdf

[Accessed 11th August 2009]


28 Atoms, Radiation and Radiation Protection. 3rd Ed. Turner. Wiley-VCH. 2007
29 World Nuclear Association. Radiation and Life. [Online]

Available at: http://www.world-nuclear.org/education/ral.htm

[Accessed on 20-08-2009]
30 SSBN Vanguard Class Balistic Missile Submarine, United Kingdom. Naval Technology.com. [Online]

Available at http://www.navaltechnology.com/projects/vanguard

[Accessed on 20-08-2009]
31 Environment Agency. Radioactive Substances Act 1993- Certificate of Authorisation and Introductory Note- Disposal of Radioactive Waste from Nuclear Site Devonport Royal Dockyard Limited. June 2009.
32 http://www.google.co.uk/imgres?imgurl=http://www.nimr.org/images/techno/seaview/reacdiag.gif&imgrefurl=http://www.nimr.org/react.html&h=313&w=697&sz=51&tbnid=5Z2XYfvLqTghDM:&tbnh=62&tbnw=139&prev=/images%3Fq%3Dsubmarine%2Bnuclear%2Breactor&usg=__ZuLv46ewuwKZ2G4ZWtMBthLz_kk=&ei=iU-NSofnIZmhjAfc3a32DQ&sa=X&oi=image_result&resnum=7&ct=image

[Accessed on 20-08-2009]


33 Rolls- Royce PWR

Available at: http://en.wikipedia.org/wiki/Rolls-Royce_PWR

[Accessed 20-08-2009]
34 Available at: http://www.jessup-bould.co.uk/pyrolysis01.JPG

[Accessed on 21-08-2009]


35 Management of Spent Radioactive Ion Exchange Resin arising from SSN and TSSBN Reactor Plant Decontamination and On-Board Primary Coolant Treatment at Devonport Royal Dockyard –Phase 2 Report –Option and Strategy Selection.

AEA Technology

M.A. Twissell, December 2002

Appendix 1

Chemical Treatment Processes
Cold Wet Oxidation

This is a mild process which is conducted at ambient temperatures and used extensively in the pulp and paper industry. It uses soluble oxidants such as hydrogen peroxide, combined with a catalyst to remove low molecular weight material, such as sugar acids and phenols. There is emphasis to use oxygen based oxidants to avoid problems with formation of haloform compounds. This process only converts soluble organic compounds rather than totally oxidising. Ion exchange resins have resistant polystyrene resin at ambient temperatures, so this process will only destroy chelating agents.



Low Temperature Plasma Ashing

This process operates at low pressure and temperature in an oxygenated environment where the oxygenated plasma generated is induced by a radio frequency electro-magnetic field or microwaves. The organic material is destroyed but the downside of the process is that radioactive material remains in the ash, so a second treatment process may be necessary if the activity level does not constitute LLW. A positive side though is that the volatile components remain in the ash. Finland is experimenting with this process and has built a half-scale plant.



High Temperature Plasma Destruction

This process operates at elevated temperatures where an electric arc is generated in an inert gas atmosphere, usually temperatures are in excess of 5000’C. Careful selection of the additives and atmosphere means that conditions can be created in which most organic material is readily oxidised and dioxins are not created. This process has the capacity to operate as either a batch process or a continuous process, but the latter only if the molten product is tapped off and the feed controlled. The final product is normally a glass with addition of glass-forming materials such as silicate. The process has been designed to handle mixed organic-containing materials.

As with some of the previous processes, gas output needs scrubbing as high temperatures volatilise a wide range of materials.

It must be noted that some high temperature processes are not suited to handle wastes with large amounts of organic materials due to the pre-treatment process needed in order to reduce the organic component to manageable proportions.


Molten Salt Oxidation

This is a flameless oxidation process in which waste is added to a bath of molten salts and held at 600-900’C. The salts are nitrates which result in the complete oxidation of organic material and all inorganic materials are retained in the molten salt. This process is only able to occur on a small scale and there has been only a small amount of experimental work carried out on this process to date.



Thermo-Chemical Treatment

This is a thermal desorption process, where a powdered reactive metal fuel interacts with waste, which usually contains water. The process involves the formation of hydrogen and burning it in the presence of oxygen, which combusts the waste leaving an ash. Gas emission in this process is reduced because any reactive gases combine with the metal powder to form salts.



Melting

This is an induction heating process where temperatures of 1500’C and above are achieved. This is used for the melting of radioactive iron and steel. The process is being developed for other applications. There is no guarantee that C-14 levels will be reduced to levels acceptable for LLWR Drigg.



Vitrification

Waste material is melted with glass-forming additives to form a solid waste glass. Different melters are used, including induction-heated cold crucibles or Joule heated ceramic crucibles. Pre-treatment is normally required, usually pyrolysis, for high organic-containing materials in order to remove the carbonaceous material. This process is used for HLW, where a pre-treated calcine is introduced to a mixture containing a glass frit. The process of fusing HLW and ILW with glass-forming components (by electrode Joule heating to between 1400’C and 1800’C) has been further developed and is now being applied to LLW streams.

Toxic heavy metals and radionuclides are retained in the glass residue whilst organic material is vaporised off as CO2 and H2O.

Hot Acid Digestion

This process mixes hot sulphuric acid and nitric acids together at a temperature of ~300’C. The sulphuric acid carbonises the organic material and the nitric acid acts as an oxidant converting the carbon formed into CO2.Inorganic wastes are converted to sulphates which can be removed by filtration or dissolved from waste and treated either by cementation or by vitrification.

Many of these processes are designed for smaller waste volumes and would not be substantial enough to be used on a large industrial scale.

DRDL have a predicted volume of 450m3 of radioactive waste which needs treating and disposing of in the next years. One very strong contender though is incineration, the next option to be studied.



Appendix 2

Long Term Aerial Dose Release Ratios (LADRR)


  • Allows for calculation of the committed effective dose (CED) to the critical group from routine discharges of radioactivity to the atmosphere for a range of nuclides and effective stack heights (1m,10m,20m,30m,40m), for adults, children (<10yrs) and infants (<1yr).

  • To assess radiological impact of routine aerial discharges. The annual discharge of each nuclide (TBq yr-1) should be multiplied by the LADRR for that nuclide for the appropriate stack height and distance. This process should be repeated for each age group in turn, and the total dose for the most restrictive age group taken as the CED to the critical group.

  • LADRR’s are quoted for 10m increment release heights and are sufficient for calculations from release heights from ground level to 40-50m.

  • Ground level releases can be taken as 1m

  • Critical Group consists of members of public living close to point of release and consuming home grown food from gardens and allotments. Critical group lies along east side of site along the A3042.

  • DRDL LADRR’s methodology consists of 3 pathways by which the critical group may receive a dose contribution from aerial discharges.

  1. Inhalation Dose- Inhalation of activity in plume and of resuspended activity from ground deposition.

  2. Ground Gamma Dose

  3. Ingestion Dose




  • Cloud Gamma whole body dose and Beta skin dose are insignificant pathways for nuclides arising from routine discharges at Devonport.

  • Particulates- only root vegetables and leafy greens are considered for Devonport critical group due top the limited availability of other local food produce within Plymouth itself.

  • 3H – SA=Concentration of radionuclide in air/ Concentration of stable element in air.

This method assumes that specific activity of the radionuclide element in air will be identical to that in the food –stuff at equilibrilium. (Remember that the calculations are not straight forward as the stable element concentration in air depends on the current vapour pressure of water in air, which in turn depends on many environmental parameters).

External Doses

  • Outside Dose(I)=DEPF(I).NUCREL(I).UNIT DCFEXT(I).(I-FRACIN).SPERY

DCFEXT(I) NRPB-DL10 dose concentration factor (Sv Bq m-2)

FRACIN Fraction of time spent indoors (0.9)

SPERY Seconds per year




  • INSIDE DOSE(I)=DEPF(I).NUCREL(I).UNIT.DCFEXT(i).FR4ACIN.SPERY.

GROUND_SHIELDING
GROUND SHIELDING Attenuation for deposition Gamma dose due to being indoors, set at 0.
TOTAL DOSE

  • DEP_DOSE=(INDOOR DOSE(i)+OUTDOOR DOSE(i)).OCCUPANCY

DEP_DOSE(i) Deposited Gamma dose to discharge of 1 TBq-1 of radionuclide(I) (Sv yr-1)


FOOD CHAIN

  • INGDOSE(J,I,K)=FOOD. IN(J,K).DEPF(I).DCFING(J,I).TRNFAC(K,I).NUCREL(I).UNIT.FOOD_MULTI(K).EXP(-RDEC (I).TCONS(K).SPERD)

INGDOSE(J,I,K) Dose due to foodstuff,k, contaminated by radionuclide(I) released at a rate of 1TBq yr-1 by age group J (Sv yr-1)

FOODIN(J,K) Food intake rate for foodstuff K by age group J (Kg yr-1)

DCFING(J,I) Dose conversion factor for ingestion of food contaminated by radionuclide (I) by age group J (Sv Bq -1)

TRNFAC(K,I) Transfer parameter to foodstuff K for radionuclide I (BQ Kg-1 food per Bqm-2 s-1deposit for one year)

FOOD_MULTI(K) Factor for local food consumption (set at x0.1)

RDEC(I) Radioactive decay constant of radionuclide (I) (s-1)

TCONS(K) Average time to consumption of foodstuff K from harvesting (d)

SPERD Seconds per day



INHALATION DOSE

  • INHDOSE(J,I)=AIRCON(I).BREATH(J).DCFINH(J,I)RESUSP.NUCREL(I)DPERY. OCCUPANCY.UNIT

INHDOSE(J,I) Inhalation dose for age group J due to aerial release of 1TBq of radionuclide(i) (Sv yr-1)

BREATH(J) Breathing rate of age group J (m3 d-1)

DCFINH(J,I) Dose conversion factor for inhalation by age group J of radionuclide I (Sv yr-1)

NUCREL (I) Annual release of isotope I (1 TBq yr-1)

RESUSP Resuspension factor (1.01 consistent with results ascribed in NRPB)

DPERY Days per yr

OCCUPANCY Occupancy factor for time spent at location in question (0.9)

UNIT Converts from 1TBq yr-1 to Bq s-1 (1TBq yr-1 =3.171E04 Bq s-1)





  • INGDOSE(J,I,K)=AIRCON(I).FOODIN(J,K).FOOD_MULTI(K).DCFING(J,I).(0.1).NUCREL(i).UNIT.EXP(-RDEC (i).TCONS(K).SPERD)/9.0E-04

So…. LADRR’s are the sum of the above pathways.




  • LADRR(J,I)=SUM (INGDOSE(J,I,K)+DEP_DOSE(I)+INHDOSE(J,I)

LADRR(j,i) Committed Effective Dose for age group J due to discharge of 1 TBq yr-1 of isotope I (Sv yr-1)




  • CED(J)=SUM (LADRR(J,I).ANNREL(I))

CED(J) Committed Effective Dose for age group J (Sv yr-1)

ANNREL(I) Annual release of isotope (I) (TBq yr-1)


Example;

0.2TBq yr-1 60Co from a stack of 20m effective height and 100TBq yr-1 of 51Cr from a stack of 1m effective height, the limiting age group dose can be calculated as follows:

Dose Release Ratios
60Co

2.67E-04 Adult

2.68E-04 Child

2.60E-04 Infant





51Cr

1.79E-07 Adult

2.47E-07 Child

2.55E-07 Infant

Multiply each LADRR by the respective release.
60Co

2.67E-04*0.2=5.34E-05 Sv yr-1 (and child/infant)


51Cr

1.79E-07*100=1.79E-05 Sv yr-1 (and child/infant)


Add doses for each group together, taking most limiting age group as the critical group.

60Co 51Cr

5.34E-05 1.79E-05 7.13E-05

5.36E-05 2.47E-05 7.83E-05**

5.20E-05 2.55E-05 7.75E-05


Appendix 3

Radionuclide Data and Radiobiological Information


Radionuclide

Decay

Decay

Half-Life

EMAX

Ni-63

ß




100.1y

65.9keV

Co-60

ß-

γ

5.3y

2.824MeV

H-3

ß-




4500d

0.0186MeV

Fe-55

Electron Capture

γ

2.7y

Mn X-rays

C-14

ß-




5730y

0.156MeV

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