Proliferation risks of highly enriched uranium (HEU) used for medical isotope production

Martin B. Kalinowski, Martina Grosch, Simon Hebel Carl Friedrich von Weizscker-Centre for Science and Peace Research University of Hamburg Beim Schlump 83, D-20144 Hamburg, Germany Email: Martin.Kalinowski@uni-hamburg.de

Abstract: To assess the proliferation threat from medical isotope production, the amount of required HEU has been estimated by analysing the world wide consumption of the most common medical isotope, Tc99m, and calculating the related irradiation procedure. The results of this method are compared with other estimations and the influence of different parameters is analysed, showing that the HEU use for Tc-99m production most likely amounts to about 15 kg per year. The lower estimate is 10 kg/a, the upper bound is 100 kg/a. Most of the excess uranium undergoes liquid storage awaiting its disposal as waste instead of recycling, posing a proliferation threat.

Keywords: Molybdenum, technetium-99m, isotope production, HEU, proliferation

1. Introduction
The use of radioisotopes for medical procedures has significantly increased for the last two decades as therapeutic and diagnostic procedures are being refined and more and more people have access to them. Most medical isotopes are produced in reactors by neutron irradiation of highly enriched uranium (HEU). To assess the resulting proliferation threat, one needs information on the amount of HEU that is used, however this information is not disclosed by the isotope producers. This paper will try to calculate the HEU requirement based on the actual consumption of medical isotopes. To this end, it will concentrate on Tc-99m, an isotope which is commonly used for examinations and accounts for about 80% of all radioisotope applications in medicine. It is produced and delivered in form of its predecessor Mo-99.

MDS Nordion Country Reactors for target irradiation Share of world 1 demand Production 2 capacity Canada NRU (CDN); Maple I & II (CDN) 40% 5000 6000 Ci/batch (several batches per week)

IRE Fleurus Belgium BR-2 (NL); Osiris (F); HFR (NL, F) 2030% 10000 Ci/week

Mallinckrodt Medical Netherlands HFR (NL)

Necsa / NTP South Africa Safari I (ZA)

25 % 10000 Ci/week

1015% 8000 Ci/week

Table 1: Major suppliers of Mo-99

Figure 1: Relation of irradiation reactors and the major processing facilities for global molybdenum-99 production.

The worldwide demand for Mo-99 is almost completely covered by the four largest producers: MDS Nordion, IRE Fleurus, Mallinckrodt Medical and Necsa/NTP [1]. Their production capacities and supplying research reactors are listed in Table 1. The relation between the major isotope extraction facilities and various production reactors is depicted in Figure 1. Currently 95 99% of Mo-99 is produced by irradiation of HEU targets, although the Reduced Enrichment for Research and Test Reactors (RERTR) programme promotes the conversion to LEU since 1978. As a result of these efforts to eliminate the civilian use of HEU, the global HEU demand for research reactors has been declining from 1,400 kg/a in 1978 to 800 kg/a in 2008, and is projected by Reistad & Hustveit [4] to further decline to 500 kg/a in a few years and to around 100 kg/a by 2020. In contrast, the use of HEU for medical isotope production is increasing and may amount to an annual consumption of 100 kg soon.

2. World wide technetium consumption

The worldwide Tc-99m consumption has been estimated by Grosch [5] based on global health care 1 Bonet, David & Ponsard [1] and Ferguson, Kazi & Perera [2] 2 IAEA [3]
2

data. This method is based on a report by UNSCEAR [6] which had estimated the global annual usage of medical isotopes. To that end, countries were divided into different health care levels defined by the population per physician as seen in Table 2, and the per capita rate of radiopharmaceutical procedures in each health care level. It is assumed by Grosch [5] that, while the absolute amount of procedures has increased since the 1990s, the relative frequency remains unchanged between the different health care levels. Health care level I II III IV Total Population per physician < 1000 1000 3000 3000 10000 > 10000 Fraction of world population 0.26 0.53 0.11 0.10 Usage of Tc99m 0.0256 0.0031 0.000180 0.000009 People examined 39,900,000 7,850,000 118,000 5,400 47,900,000 Total activity administered [TBq/a] 24,000 4,700 71 3 28,800

Table 2: The global usage of Tc-99m by countries of different health care levels.

To obtain an estimation of the current use of radiopharmaceuticals in countries of health care level I, Grosch [5] has analysed the radioisotope use in Germany, Sweden and the United States, the latter of which is often claimed to account for one half of the global Mo-99 demand. Based on these data, one can assume that in health care level I countries, 3.2% of the population receive an examination or treatment using radionuclides in one year. Based on this assumption, the number of radiopharmaceutical procedures in the countries with the highest health care level can be estimated as demonstrated in Table 2. If approximately 80% of the procedures have involved Tc-99m with an average administration of 0.6 GBq Tc-99m per treatment, the total annual activity used in all Level I countries is assessed to be 24 PBq. According to fixed relationships between the four health care levels, the total amount administered worldwide in the last years would be 28.8 PBq of Tc-99m per year. According to UNSCEAR [6] the Tc-99m consumption was about 16 PBq/a in the years 1991 1996, suggesting an increase of 4.5% per year since then.

3. HEU consumption for medical isotope production

Certain generalized assumptions are made to calculate the global HEU consumption needed to deliver sufficient Mo-99 to serve the global Tc-99m demand. These parameters were selected under the assumption that the procedures are optimized and an efficient but realistic balance of HEU consumption per Mo-99 delivery is achieved. In the reactor, HEU targets of about 4-20 g each are irradiated using thermal neutrons for several days. After irradiation, the targets are dissolved in nitric acid and the Mo-99 extracted. The remaining waste is prepared for final disposal or, in some facilities, for later retrieval of the remaining HEU. To meet the global Tc-99m demand of 28.8 TBq, a certain amount of Mo-99 has to be produced. As these isotopes continuously decay during storage, processing and transport, the production to meet the global demand depends on the duration of the processing and delivery of molybdenum to the hospital as well as the efficiency of use. At the medical site, Tc-99m is withdrawn from the dispenser on a daily basis, as seen in Figure 2. This withdrawal procedure can be very efficient, extracting 99 % of available Tc-99m.

Figure 2: Development of the Mo-99 and Tc-99m activities during a 6 day transport phase and the consequent daily Tc withdrawals at the hospital.

Based on an estimation of the transport time (our assumption: 6 days) and the number of withdrawals (our assumption: six times) one can put the Tc-99m consumption in relation to the amount of Mo-99 produced. The result for this scheme is that about 0.7 TBq Tc-99m are gained for each TBq of Mo-99 produced. According to Table 1, the annual production capacity of the four largest producers is roughly 50,000 6-day-Ci per week, which translates to about 380 PBq/a of Mo-99. Using the factor 0.7 as explained above, one can derive that the main producers have the capacity to provide enough material for a Tc-99m consumption of 270 PBq/a. A comparison to our estimate of 28.8 PBq/a suggests that 10 % of the overall capacity is used, which is plausible. The required HEU mass can be derived by simulating the irradiation procedure. In the model, targets 14 -1 -2 with 15 g HEU of 93 % enrichment were assumed, exposed to a thermal neutron flux of 10 s cm for 5 days. Fission yield data from ENDF VI were utilised. The cooling and processing of the irradiated targets is assumed to take about 2 days. As a result of the calculation using these parameters, approximately 1000 targets of 15 g are needed to meet the global Tc-99m demand. This material contains nearly 14 kg U-235, i.e. a little more than half a significant quantity that the IAEA defines to be 25 kg.

4. Results
The calculations show a global HEU usage of about 15 kg per year for medical isotope production. The International Panel on Fissile Materials (IPFM) estimates a HEU consumption of 85 kg per year for the same time period. While the method seems valid given that the estimations are of the same order of magnitude, the difference is still considerable. This is not surprising considering the speculative nature of many input parameters, especially the transport and processing time as well as the annual Tc-99m consumption. To assess the influence of these parameters, a sensitivity analysis was performed for the most important ones (see Table 3).

Transport duration [d] value HEU [kg/a] 2 5.6 6 15 10 42

No. of withdrawals value HEU [kg/a] 3 22 6 15 12 12

Neutron flux [s cm ] value HEU [kg/a] 5e13 31 1e14 15 2e14 7.7

-1

-2

Irradiation time [d] value HEU [kg/a] 2 28 5 15 10 12

Table 3: Influence of different parameter values on the calculated annual HEU demand for Mo-99 production.

This analysis shows how the amount of required HEU according to the selected parameters is close to the realistically possible minimum. It increases significantly if a longer transport time and less Tc-99m withdrawals are assumed. On the contrary, the increase of withdrawals runs into a saturation at the minimum HEU consumption rate of 12 kg/a. The irradiation parameters are less relevant to the result: the amount of required HEU is inversely proportional to the neutron flux, which on the other hand is a parameter of high confidence as it can be confirmed by Saey [7]. Assuming a shorter irradiation time would almost double the HEU demand and should be carefully considered, as reactor irradiation time is very expensive for the Mo-99 producer. On the other hand, longer irradiation times would not significantly decrease the required HEU as the output of Mo-99 is limited by its short half life. Taking these uncertainties into account, it can still safely be concluded that the production of Mo-99 / Tc-99m alone requires most likely about 15 kg of HEU per year. At least 10 kg/a are required, 50 or even 100 kg/a might be used. This HEU, after some cooling time following irradiation, is handled in an environment with a low radiation barrier, and is mostly not recycled, but kept on site in liquid storage. This storage and handling of HEU is relatively small compared to the amounts circulating in other sectors, e. g. in research or naval military reactors. But it is an ongoing proliferation risk that could easily be avoided by converting to a LEU production procedure. If medical isotope consumption continues to increase with 4.5% per year as in the past decade while other stocks of HEU are reduced, the relative importance of medical HEU for nuclear non-proliferation will become more and more relevant.

5. Acknowledgment
The authors would like to express their gratitude to Britta Riechmann who provided support in literature research for this paper, including the preparation of Figure 1. This work was supported by the German Foundation for Peace Research (Deutsche Stiftung Friedensforschung, DSF).

6. References
[1] Bonet, H., David, B. and Ponsard, B.; Production of Mo-99 in Europe: Status and Perspectives ; th ENS RRFM 2005; Transaction Session 1, 9 International Topical Meeting on Research Reactor Fuel Management; Budapest, April 2005. [2] Ferguson, Charles D, Tahseen Kazi and Judith Perera; Commercial Radioactive Sources: Surveying the Security Risks; Occasional Paper No. 11; Monterey Institute of International Studies, Centre for Nonproliferation Studies; January 1998. [3] IAEA-TECDOC 1051; Management of radioactive waste from Mo-99 production; International Atomic Energy Agency, Vienna, November 1998. [4] Reistad, Ole and Styrkaar Hustveit; HEU Fuel Cycle Inventories and Progress on Global Minimization; Nonproliferation Review; Vol. 15, No. 2, July 2008; p 266-287. See also International Panel on Fissile Materials; Global Fissile Materials Report 2008. Figure 1.7.

[5] Grosch, M.; Complications of the Medical Radioisotope Production for the Non-proliferation Regime. Master thesis, University of Hamburg 2008. [6] UNSCEAR Report 2000; Sources and effects of ionizing radiation; Annex D: Medical radiation exposures; United Nations Scientific Committee on the Effects of Atomic Radiation, Vienna 2000. [7] Saey, P.R.J.; The Influence of Radiopharmaceutical Isotope Production on the Global Radioxenon Background; Journal of Environmental Radioactivity, Volume 100, Issue 5, May 2009, p 396-406; doi:10.1016/j.jenvrad.2009.01.004.