Impact of americium on safety performance of liquid metal cooled reactors Janne Wallenius Professor Reactor Physics, KTH Generation IV reactors Background Radiotoxic inventory [Sv/g] 100 10 By recycling of Am & Cm (in addition to Pu) one may achieve TRU 240 Pu 239 1 Pu 238 243 Am 0.1 Pu 100 times less long lived high level waste 241 Am Storage time of residual waste < 1000 years 242 Pu 0.01 Unat 237 Np 101 102 103 104 105 Generation IV reactors t [y] 6 10 Increase capacity of geological storage by factor 3-6 Why fast reactors? Fissionprobability 238 Pu 239 Pu 240 Pu 241 Pu 242 Pu 241 Am 243 Am 244 Cm 245 Cm 246 Cm 247 Cm Recycling of Am & Cm in thermal spectrum increases Cf-252 inventory by factor ~ 1000, compared to fast spectrum recycle Fast reactors permit breeding of Pu, increasing fuel resources by a factor 100 0.2 0.4 0.6 Generation IV reactors 0.8 1 Impact of americium on safety of fast reactors Introduction of americium will lead to Reduction of Doppler feedback Increase in coolant temperature coefficient Reduced delayed neutron fraction Degraded performance under transients Generation IV reactors Impact on Doppler feedback 800 Doppler constant [pcm] 600 2 years delay between reprocessing and fuel loading yields 1% Am 400 200 0 Pu fraction in MOX fuel ~ 18 % yields conversion ratio ~ 1.0 in a typical sodium fast reactor (SFR) Am [%] 0 5 10 15 Fuel: (U0.82-x,Pu0.18,Amx)O2 Generation IV reactors In order to burn the Am production from one LWR of same power, an SFR fuel load with 3% Am is necessary. Americum is detrimental for Doppler feedback! Physics of Doppler feedback Doppler feedback mainly derives from neutron captures occuring below 100 keV Doppler contribution Capture spectrum E [keV] 0.1 1 10 100 Generation IV reactors 1000 The lower the energy of the resonance where capture occurs, the more efficient is the Doppler feedback In an SFR with standard MOX fuel, 65% of the Doppler feedback derives from neutron captures below 3 keV, constituting only 15% of all captures! Why does americium kill Doppler? Capture cross section [b] The capture cross section of 241Am is ten times larger than that of 238U at E > 100 keV. 2.5 2.0 1.5 Increasing Am inventory, fewer neutrons will reach the region where Doppler feedback is functional. 241Am 1.0 0.5 238U E [MeV] 0.2 0.4 0.6 Generation IV reactors 0.8 1 Even with 70% uranium in the fuel, the Doppler feedback may become negligible! Coolant temperature feedback 1 Fission probability Fission cross section of 241Am exceeds capture cross section already at 0.7 MeV. 0.8 0.6 241 Am 0.4 The more americium, the more sensitive is the fuel to changes in coolant density 238 U 0.2 En [MeV] 0.5 1.0 Generation IV reactors 1.5 2.0 Delayed neutron fraction 10 8 Yield [%] Increasing mass of mother nuclide shifts mass of the lighter fission product 235 U 6 245 Cm 4 Reduced yield of delayed neutron emitter bromine 2 A 90 100 110 120 130 140 150 160 Nuclide νtot νd/νtot 238U 2.53 1.89% 239Pu 3.02 0.22% 241Am 3.37 0.13% 244Cm 3.42 0.13% Generation IV reactors Increasing neutron number of mother nuclide increases prompt neutron yield Fraction of delayed neutrons emitted from fission products decreases with mass of the mother nuclide. Effective delayed neutron fraction Probability [MeV-1] Delayed neutron spectrum is softer than prompt neutron spectrum 1.5 1.0 0.5 0.0 0.0 βeff is smaller than β in a fast spectrum Delayed Probability of capture by americium larger than for prompt neutrons Prompt E [MeV] 0.5 1.0 1.5 Generation IV reactors 2.0 2.5 βeff/β decreases with concentration of americium Impact of americium: Summary Fuel (U0.8,Pu0.2)O2 (U0.7,Pu0.2,Am0.1)O2 KD 550 pcm 230 pcm αNa +0.2 pcm/K +0.4 pcm/K βeff 390 pcm 330 pcm Reduces Doppler constant, Increases coolant temperature coefficient Decreases βeff Assume MOX fuel average temperature is 1500 Kelvin αD = -KD/T ≈⋲ -0.37 pcm/K (no americium): |αD/ αNa| > 1! αD = -KD/T ≈⋲ -0.15 pcm/K (10% americium): |αD/ αNa| < 1! Generation IV reactors Response to transient over-power Fuel (U0.8,Pu0.2)O2 (U0.7,Pu0.2,Am0.1)O2 αD -0.4 pcm/K -0.2 pcm/K αNa +0.2 pcm/K +0.4 pcm/K βeff 390 pcm 330 pcm Assume that 1$ of reactivity is inserted (withdrawal of control rod) Assume Δ∆TNa ≈⋲ 0.1 x Δ∆TMOX How much have coolant & fuel temperatures increased when the total negative reactivity feedback reaches 1$? Generation IV reactors Additional temperature feedbacks Axial expansion of the fuel: response time ~ speed of sound x fuel length Radial expansion of the assembly support grid plate. Fuel (U0.8,Pu0.2)O2 (U0.7,Pu0.2,Am0.1)O2 αax -0.3 pcm/K -0.5 pcm/K αR -0.6 pcm/K -1.2 pcm/K Data for 1500 MWth SFR. Geometry effects are large in small cores. Influence of americium is positive, but effect is smaller in cores with CR = 1 Generation IV reactors Transient overpower accident in a sodium fast reactor with MOX fuel 3200 Tfuel [K] 1 $ reactivity insertion simulated for MOX fuelled SFR with SAS4A/ SASSYS. 3100 3000 Adding 1% Am increases maximum fuel temperature by 75±15 K Tfail 2900 2800 0 Am [%] 1 2 3 4 Fuel: (U0.8-x,Pu0.2,Amx)O2 Generation IV reactors 5 Fuel failure limit (solidus) reached for 2.5% americium Failure margin can be maintained if nominal power is reduced by 6% for each percent Am added to the fuel. Metallic versus oxide fuels 1500 Metallic alloy fuels feature a much lower Δ∆T from core inlet to fuel maximum temperature Tfuel [K] 1450 Δ∆Toxide ~ 1500 K (failure margin ~ 700 K) 1400 1350 Δ∆Tmetal ~ 200 K (failure margin ~ 400 K) Tfail Similar increase in relative power consumes less of failure margin in a metal fuel 1300 1250 1200 0 Am [%] 1 2 3 4 5 Fuel: U0.88-x,Pu0.12,Amx-10Zr Adding 1% Am increases Tmax by 25±5 K Power reduction to maintain ultimate failure margin under a UTOP: Δ∆P = -3% per percent Am Generation IV reactors Dense ceramic fuels 30 Thermal conductivity [W/m/K] 25 UN Nitride fuels feature a unique combination of high thermal conductivity and high failure temperature 20 PuN 15 10 AmN Δ∆Tnitride ~ 500 K (failure margin > 1500 K) 5 0 T [K] 600 800 1000 1200 1400 Generation IV reactors Carbide fuels today can not be fabricated without evaporating americium! 1600 Δ∆P = -2.7% per percent Am Linear rating 50 Permitted linear rating [kW/m] 40 30 For similar SFR geometries with conversion ratio ~ 1.0, Nitride Nitride fuels allow largest linear power during normal operation Metal 20 Oxide 10 Am [%] 0 0 2 4 6 Generation IV reactors 8 10 Nitride fuels allow to accommodate more americium at the lowest power penalty. Summary & discussion Americium is detrimental for Doppler feedback, coolant temperature coefficient & effective delayed neutron fraction Power penalty of Am in MOX fuels: Δ∆P = -6% per percent Am Power penalty of Am in metallic & nitride fuels: Δ∆P = -3% per percent Am Major factor to improve safety and maximise americium burning rates: Ratio of margin to failure to total Δ∆T under nominal operating conditions. Nitride fuels provide best possible performance, thanks to combination of high thermal conductivity and high failure temperature. Generation IV reactors
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