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NUCLEAR WASTE MANAGEMENT

K. Periasamy, M.Tech (Chem. Engg), Chennai 96.

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Introduction In the Nuclear Energy debate people raise the following questions regarding the safety of Nuclear Power: a) Will the Reactor explode like a Bomb? b) What happens if power fails completely? c) What happens in case of Earthquake? d) What happens in case of tsunami? e) What happens in case of all back up power generators fail? f) What happens if Aircraft hits the Reactor building? When the Engineers give scientific replies for all these questions, they question, if it is so why there were accidents in 3 Reactors. Then the Engineers explain that these are 1st Generation Reactors designed and built 40 years back with less experience and with very optimistic outlook on the coincident probabilities and design margins. They were built when Nuclear Energy was in the primitive stage. Today it is a matured technology with 14000 Reactor years of experience. Nuclear Energy being a specialized and a bit complex subject, even the Engineers who have not worked in nuclear field find it difficult to understand and assimilate all the replies. However, with proper explanation they get convinced in their mind. But in their heart, which breeds the perceived risk for the fear of unknown like, fear for ghost, fear for darkness, fear for height, etc. the fear for radiation (which is also unseen) is retained!

Now this fear hidden in the heart (not in mind!) triggers the mind not to accept and give up the argument against nuclear power. Hence, they fire the next salvo, thinking that, this is their Brahmastiram. They say OK, we accept whatever you have explained about the safety of the Nuclear Reactors. But what happens to the highly radioactive nuclear waste which will last for Millions of years? What is the answer you have? At this point the normal nuclear reactor operating engineers pause and try to explain whatever they know about the low level wastes that are generated in the Nuclear Reactors during the maintenance of the plant. They also inform that the Spent Fuel which contains most of the radioactively is reprocessed and recycled. They dont give much detail on this. The reason is simple. It is another specialized area where distinctly different set of Engineers and Scientists are working. Since this debate about Spent Fuel Management is not common, let us start from basics. Nuclear Fission Before going into the Spent Fuel Waste Management, let us understand what happens during Fission. The Nuclear Fuel is made up of a mixture of Fissile atoms and Fertile Atoms [U-235 + U-238 (or) Pu239 + U-238 (or) U-233 + Th232]. These atoms are present as Oxides in powder form. This powder is compacted as small pellets and these pellets are inserted into a long thin walled tube made up of Zircoalloy. This tube is perfectly sealed and nothing, except neutrons can come out. This fuel pellets contained in Zircoalloy tube is called Fuel Pin. Several pins are bundled together with sufficient gap in between the pins for the flow of coolant and kept inside the Reactor, and this is called Core of the Reactor. When the fissile atoms (U 235, U 233 & Pu 239) undergo fission after absorbing one neutron, they usually split into two atoms, one with about 2/5th and another with about 3/5th of the mass number of the fissile atom. During this process, 2 or 3 neutrons are also released. For example, when U 235 undergoes

fission after absorbing one neutron, it forms Kr 92 + Ba - 141 and 3 neutrons (235+1=92+141+3). and their yields. These two atoms are called as Fission Products. The accompanying Graph provides information on the mass number of fission products

MASS NUMBER

Heat Transport When fission takes place these fission products and the neutrons are released at about 9000 Km/sec. Please note it is Km/Sec and not Km / Hr. So, they possess very high Kinetic Energy. But these fission products are instantly stopped by the U235/U-238/O/ Zr atoms present just adjacent to the fissile atom. Kinetic Energy is converted into Heat Energy. after transferring its heat to the Boiler Water. Hence this This heat is carried away by the The Boiler Water becomes high the

coolant surrounding the fuel. The coolant goes to the Boiler where it gets cooled pressure steam. The cooled coolant water comes back to the Reactor and

steam goes to the Turbine.

In the Turbine the steam rotates the Turbine and

escapes as a low pressure steam. This low pressure steam is condensed back as Boiler Water using sea water. The hot sea water (about 7C higher than intake) is returned back to the sea. The condensed Boiler Water is sent back to the Boiler. Please note, none of the three waters Reactor Coolant Water, Boiler Water and the Condenser Sea Water mix anywhere. They only exchange heat while one water passing inside the Tube and the other passing outside the tube in Boiler and the Condenser. Hence, there is no scope for the radioactivity contained within the Zircoalloy Tube to come out and mix with Sea Water. Waste Generation As mentioned above there are two ways by which waste is generated. One is the waste generated in the Reactors during operation and maintenance of the plant. These are generated by way of sampling, pumps / valves maintenance, bleeding of process streams etc. These are very low level radioactive liquid, gas and solid wastes. The liquid wastes are diluted to very insignificant concentration levels and dispersed. The gaseous wastes which are mostly short lived isotopes are diluted and dispersed at high altitudes. These decay very fast and hence do not pose any health hazards. The solid wastes, which are mostly the protective cloth worn by workers, cotton waste, etc are monitored for radioactive contamination. If there is any contamination with radioactive substances, they are made into small pieces, mixed with special cement and made as unleachable solid concrete and kept inside the plant and monitored for few years, till there is complete decay and there are no more radioactive substances left out. So the first waste source which emerges during the operation/maintenance of the Reactors is very low in radioactivity and is simple to handle. The second source of waste is that present as Radioactive Fission Products in the spent fuel. This contains almost all of the radioactivity that is produced in the Nuclear Fuel Cycle. Hence, it is discussed in detail in the following pages.

Spent Fuel The fresh Nuclear Fuel in a typical Pressurised Water Reactors (PWRs) like that of KNPP will have about 3% U 235 and balance U 238. The yield % and half life of various fission products that are produced in PWRs with about 35,000 MWd / Ton of burn-up will be as given below : Table 1 S.No Isotope Yield, % 1. I 135 2. Mo 99 3. I 131 4. Ru 106 5. Cs 133 6. Pm 147 7. Sb 125 8. Eu 155 9. Kr 85 10. Cd -113m 11. Sr 90 12. Cs 137 13. Tc 99 14. Sn 126 15. Se 79 16. Zr 93 17. Cs -135 18. Pd 107 19. I 129 6.33 6.10 2.83 0.39 6.79 2.27 0.03 0.033 0.27 0.0003 5.75 6.09 6.05 0.024 0.051 6.29 6.91 0.16 0.66 6.57 Hours 10 50% becomes Xe 135. Balance converts to Cs 135 Half-life Unit Remarks

65.94 Hours 8.02 Days 1.02 Years 2.07 Years 2.62 Years 2.76 Years 4.76 Years 10.78 Years 14.1 Years 28.9 Years 30.2 Years 2,11,000 Years 2,30,000 Years 3,27,000 Years 15,30,000 Years 23,00,000 65,00,000 Years 1,57,00,000 Years Suitable for destruction by transmutation Suitable for destruction by transmutation Gets converted into Cs-135

Please note, the yield % mentioned above is the average percentage of each fission product produced during the fission. But the actual content at the time of taking out the spent fuel after a few years of usage within the Reactor at various locations of the core will be different. This is because of the fact that each fission product

has a different half life, different neutron absorption cross section leading to transmutation, different vapour pressures, different volatility, etc. For example I-129 has very high neutron absorption cross section. Hence there is good possibility for the I-129 produced in the initial few years of usage of the fuel bundle to get converted to Xenon 130. Similarly the gaseous fission products like Argon, Krypton will rise up and accumulate at the top of the fuel pin, but will remain within the sealed Zircoalloy Tube. The Plutonium and Transuranics formed may undergo fission by neutron absorption, thereby reducing their percentage. Hence the yield percentage given above is only a guideline for estimation of the percentage of various fission product fraction. In general, there is net reduction in the overall percentage of problematic fission products making the waste management much easier. The Graph given below provides information on how the radioactive isotopes decay exponentially and the radioactivity falls drastically with time.

From the Table and Graph given above, we notice that there are three distinctive groups of radioactive materials. The First Group (S. No.: 1 to 3) which has very short half lives has I-135 (6.57 Hrs), Mo-99 (65.9 Hrs), I -131 (8 days). These radioactive atoms die down very quickly as soon as the Reactor is stopped and the spent fuel is taken out. They all become stable atoms and there will not be any radioactivity from these atoms after about one year. Management. The Second Group is the one which has medium half lives like So, we need not worry about them with regard to Waste

Kr85 (10.78 years), St90 (28.9 years), Cs137 (30.2 years), etc. These atoms emit strong Beta / Gamma radiation and hence play a major role in radioactive waste management. They constitute almost about 80% of the total radioactivity of spent fuel, though they constitute only about 50% in terms of quantity (Ref : Table-2). The Third Group is the long lived Fission products like Tc99, Cs135, I129, etc. The Actinides like U-235, Pu239, Pu-240, Am-241, Np237, etc. also have long half lives. But being useful as Fuel, the Actinides are completely recovered along with U 238 by Reprocessing and are reused. Hence, they do not come under waste category even though they emit radioactivity. The long lived Fission Products which are very low in quantity and also very low in radioactivity level remain as part of high level waste and need to be managed. These constitute the remaining about 20% of the total radioactivity. In essence, the radioactive waste management boils down to the management of very low quantity of long lived fission products and the appreciable quantity of medium half life fission products, with the later being the most problematic one.

Spent Fuel Reprocessing As mentioned above, the spent fuel has the U 238 and the Actinides like unused U 235 and those produced during Reactor operation ( like Pu-239, Np-237, Pu-240, etc.) and the various fission products formed during the fission and still left after decay and transmutation when the spent fuel is taken out of the Reactor. The spent fuel is normally stored under water inside the Reactor building for few years. This water gets heated up due to the decay heat released from the fuel. This water is continuously cooled using external cooling water. years this fuel is sent to Reprocessing Plants. Typically the composition of a 10 years cooled PWR fuel will be as given below : Table- 2 Atom / Group U 235 Pu 239 Other Actinides Stable Fission Products ( No Radioactivity ) Medium Half Live (St-90, Cs-137) Long Lived ( I -129, TC-99 ) Other Long Lived Fission Products Balance ( U-238 ) Total % 1.0 0.9 0.1 3.1 0.2 0.1 0.1 94.5 100.0 After about 5 to 10

In the Reprocessing Plant the Fuel Bundles are sheared to make the Fuel pins into small pieces and is dissolved in Nitric Acid. All the Oxides of Uranium, Plutonium and Fission Products get converted into evolved during this dissolution. Nitrates and go into acid solution. Volatile and gaseous fission products like (Kr-85, I-129, etc.) present in the fuel are These are continuously scrubbed in multistage scrubbers using chilled water and filtered in special HEPA Filters. The acid solution containing all Uranium, Plutonium and Fission Products is treated with an Organic compound called TriButyl Phosphate (TBP). This compound has very high affinity for Uranium, Plutonium and all other Actinides, but least affinity

for fission products. Hence, Uranium and Plutonium get captured in TBP leaving the Fission Products in Acid solution. This TBP containing the Uranium and Plutonium is then treated with dilute Nitric Acid to get back the Uranium and Plutonium into acid solution. This acid solution of Uranium and Plutonium is once again treated with TBP in a different process condition to separate Plutonium from Uranium. This separated Uranium and Plutonium are sent to Fuel Fabrication Plant for reuse in Fast Breeder Reactors. The Acid solution containing all the Fission Products is concentrated and then stored in special Under Ground Waste Storage Tanks. These Tanks are also cooled The total continuously, though the cooling requirements are much lower here.

volume of this liquid waste obtained in processing 30 Tons of spent fuel that will be discharged from a 1000 MW Plant per year will be about 10,000 Liters only. The Reprocessing Process explained above is called PUREX Process and India has been using this process for about 40 years. US and other Countries is total ignorance! Waste Immobilization The Acid solution containing the left out fission products after decay for about 25 years is taken out from the Under Ground Tanks and sent to Waste Immobilization Plant for further processing and ultimate disposal. In this Waste Immobilization Plant, this solution is concentrated further till the Fission Products become almost like a glass and this is made as an impermeable glass matrix with the addition of certain chemicals. The volume of this glass will be hardly about 3000 Liters for the spent fuel obtained from a 1000 MW Reactor operated for one year. In terms of fission products weight, it is just 1050 Kgs [(3.1+0.2+0.1+0.1)/100)x30x1000]. Out of this, only about 120 Kgs [(0.2+0.1+0.1)/100x 30 x 1000) is radioactive fission products. Compare this with the 60,00,000 to 80,00,000 Tons of CO2 & few thousand tons of Silica particles spewed into the atmosphere and the 3,00,000 - 6,00,000 Tons of We are one of the pioneers in this Technology. The media hype on Denying of Reprocessing Technology to India by

fly ash containing a host of heavy metals like Mercury, Lead, Arsenic, etc. dumped near the plant. Further, all natural radioactive substances which are likely to be present in coal are also brought into the public domain. The main issue is that, this radioactivity associated with coal goes unnoticed and unmeasured. This liquid glass is poured into large number of small canisters made of special Titanium / Copper material which are not corrodible by any chemical available in nature at normal ambient temperatures or even at moderate temperatures. The canister is seal welded. The entire process is called Vitrification and Immobilization. Each canister is then embedded in about 1 cubic meter of special unleachable high density concrete. These concrete Blocks are kept for few years in the Plant and subjected to all extreme weathering and stress cycles to verify the integrity of the Block. Then these Blocks are kept in deep abandoned mines and monitored for few years. Then they are permanently embedded. If needed, water samples around the place can be verified through deep bore wells for monitoring on long term basis. As we can notice, by the time it is ultimately disposed it is almost about 60 years since the fuel has been taken out of the Reactor. Since the half life of the problematic fission products is about 30 years, about 75% of the original activity of these fission products would have died down leaving only 25%. But, since the half lives of long lived fission products (the Third Group mentioned earlier) are very high, there will be no appreciable reduction in the activity level of these fission products. That means only about 40% (80 x 0.25 + 20) of the total original Since everything is completely radioactivity of the medium and long lived fission products in spent fuel will be there in the glass during ultimate disposal. immobilized and kept out of reach of any human activity there is nothing to worry about. Even this radioactivity will get reduced substantially faster in the initial few centuries as can be seen from the decay curve. Another way of managing these fission products is to send the fission products back into Reactors for converting them into less radioactive or non radioactive or shorter half life products. This process is called Transmutation. We will exercise this option also in Fast Breeder Reactors in future. Tc-99 being amenable for transmutation, this will greatly reduce the quantum of radioactivity to be managed.

Conclusion From the above discussions one can understand that the quantum of radioactive materials which need to be handled is very small. The radioactivity which needs to be managed is also very less due to the recovery and reuse of Actinides (Uranium and Plutonium) and natural decay of the problematic fission products during long periods for which the fission products are kept in various plants inside thick concrete Cells. India has the complete technology for Fuel Reprocessing and Waste Immobilization, thereby closing the Nuclear Fuel cycle in the most environmentally benign manner starting from Uranium Mining to Waste Immobilization. There need be no apprehension regarding the Spent Nuclear Fuel Management in India. Please note the complete processing of the Spent Fuel is done in about 1M thick concrete cells and all operations are done remotely. Even welding of the canisters is done remotely. As far as possible no moving parts are employed in these process plants and hence the maintenance requirements are very minimum. In my opinion, since we have the complete Technology for Reprocessing and Waste Management, we can import the large quantities of Spent Nuclear Fuels which have been lying idle for several decades in many Countries like France, Germany, Japan, US, Canada, etc. and process them to recover the valuable Plutonium for use in our Fast Breeder Reactors or PWRs. If required, we can also retain all the fission products recovered during this processing. We know how to handle it. This will be a golden opportunity for India to build more FBRs thereby speeding up the switch over to Thorium U233 based Reactors. &&&&&&