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Kristiina Sadian, Rickard Johansson and Christian Alex Uppsala University 5/25/2010
ABSTRACT
As long as fission nuclear power is used, efforts will be made to maximize revenues and increase the power output to fuel input ratio. This includes higher burn-ups, uprating, and longer fuel cycles, resulting in higher demands on the entire reactor. However, the focus of this study lies in the limitations of the fuel cladding, more specifically, in the consequences of hydrogen pick-up. Oxidation of the Zircaloy cladding liberates hydrogen, of which a part diffuses into the Zircaloy matrix and eventually precipitates to zirconium hydride platelets. This degrades the mechanical properties of the Zircaloy, and causes hydrogen embrittlement, delayed hydride cracking, and formation of hydride blisters, which in turn might result in fission gas release, and other undesirable consequences. Therefore, it is imperative that research continues to investigate known phenomena, which might behave differently with new operating parameters. In Sweden, this is carried out by Studsvik, who recently prolonged an international research project aiming to gain an in-depth knowledge of cladding related issues.
TABLE OF CONTENTS
Introduction and background .................................................................................................... 3
Purpose and aim of this study ............................................................................................................................. 3
Nuclear reactors in the world today .......................................................................................... 4 General cladding information .................................................................................................... 5
What is the cladding? .......................................................................................................................................... 5 PWR ..................................................................................................................................................................... 5 BWR ..................................................................................................................................................................... 5 CANDU................................................................................................................................................................. 5 Desired cladding properties ................................................................................................................................ 6 Cladding materials............................................................................................................................................... 7 Fuel cladding materials used in Swedish reactors............................................................................................... 8
Incidents caused by hydriding in fuel claddings ....................................................................... 13 Transporting used up fuel ........................................................................................................ 14
Transporting damaged fuel claddings ............................................................................................................... 15
Fission gas release and radiation dosages ............................................................................... 15 Current Research and Development ........................................................................................ 16
Ongoing projects ............................................................................................................................................... 16 Cladding material .......................................................................................................................................... 16 SCIP ............................................................................................................................................................... 16
Bibliography.............................................................................................................................. 17
Reactor type Pressurised Water Reactor (PWR) Boiling Water Reactor (BWR) Pressurised Heavy Water Reactor 'CANDU' (PHWR) Gas-cooled Reactor (AGR & Magnox) Light Water Graphite Reactor (RBMK) Fast Neutron Reactor (FBR) Other
Main Countries US, France, Japan, Russia, China US, Japan, Sweden Canada
Number 265
GWe 251.6
Coolant water
Moderator water
94 44
86.4 24.3
UK
18
10.8
Russia
12
12.3
water
graphite
4 4 441
none graphite
In Sweden, there are 10 reactors operating currently at three different locations; three BWRs at Oskarshamn, three BWRs at Forsmark, and tree PWRs and one BWR at Ringhals. Figure 1 shows the ownerships of the Swedish nuclear power plants where Vattenfall AB holds the majority ownership of Forsmark and Ringhals. In Sweden during 2008, the total electricity production was 146 TWh of which nuclear power was 61,3 TWh which 2 corresponds to about 42%.
1 2
(World Nuclear Association) (Svensk Energi) 4 Nuclear reactors in the world today | Uppsala University
PWR
The enriched fuel pellets are inserted into Zircaloy tubes that are bundled together. The tubes are 3 approximately 1 cm in diameter and the fuel cladding gap, which is about 0.1 mm, is filled with helium gas to improve the conduction of heat from the fuel to the cladding and to prevent pellet cladding interaction. One 4 assembly is about 4 m long and consists of 179-264 tubes. The reactor core is formed by 121-193 assemblies.
BWR
The BWR fuel assemblies are similar to those used in PWRs. However, each BWR fuel assembly is put into a canister to prevent local density variations, and thus prevent changes to neutronics and to thermal hydraulics. 4 The assemblies consist of 91, 92 or 96 fuel rods and between 368 and 800 bundles are loaded into the reactor.
CANDU
The CANDU assemblies consist of unenriched (or low enriched) fuel pellets inserted in Zircaloy tubes that are bundled together. Each assembly is about 0.5 m long and consists of 37 or 43 fuel rods and the reactors core 4 consists of 4500-6500 fuel assemblies.
3 4
FIGURE 3. THE LEFT ASSEMBLY IS A WESTINGHOUSE PWR FUEL DESIGN. THE MIDDLE ASSEMBLY IS A WESTINGHOUSE SVEA96 OPTIMA2 BWR FUEL.
CLADDING MATERIALS
Naturally, the type of cladding needed depends on which type of reactor is being used as this determines the operating parameters. Figure 4 shows operating temperature ranges for different reactors and claddings. The first industrial-scale nuclear power plant in the world used magnox fuel cladding, a magnesium alloy. However, disadvantages such as a very limited maximum temperature and a high reactivity with water, thus preventing long-term storage under water, has in the long run disfavored these types of reactors and cladding. Other popular claddings consist of stainless steel as well as aluminum. Stainless steel has found use in fast reactors and in light water reactors where the neutron-capture cross section is less important. Aluminum on the other hand has a low neutron-capture cross section but has inferior physical strength and poor corrosion resistance 5 at temperatures above 149C.
FIGURE 4. OPERATING TEMPERATURE RANGE FOR CLADDING MATERIAL FOR FISSION REACTORS6.
However, a vast majority of the reactors in use in the world today are water-cooled in which the element that best fits the criteria for cladding is zirconium. Thus, in all water moderated reactors different zirconium alloys are used. The beneficial properties of zirconium were first discovered by the U.S. Navy in the early 1950s as they were in search of a material with high corrosion resistance, high strength and low neutron capture crosssection. Although zirconium is relatively expensive compared to other cladding materials, it has proved to be extremely useful and thus developed to dominate the cladding market. Commercial zirconium always contains a few weight percent of hafnium which has a neutron capture crosssection in the order of 600 times that of zirconium. For this reason, hafnium has to be removed; nowadays almost all of the hafnium can be extracted. To improve the properties of the cladding further, other elements are added such as tin, nickel, chromium, iron and niobium. These elements make the cladding more resistant to corrosion, reduce hydrogen uptake, reduce weight gain and improve creep properties.
alloys.
Material
Zry-2 Zry-4 Zry-4, low Sn ELS 0.8 Zirlo M5 Duplex E110 E125/Zr-2,5%Nb Zr-2,5%Nb E635/Anikulloy
Application
BWR PWR PWR PWR PWR PWR PWR WWER/RMBK RMBK CANDU WWER/RMBK
For a more comparative overview of the most common types of the zirconium based alloys, see Figure 5. The 7 latest edition developed by Westinghouse is called OptZirlo .
6 7
(Studsvik Seminar 16) (Dahlbck) 8 (Rnnberg) 8 Cladding related problems | Uppsala University
Finally, the phenomenon that will discussed in further detail in this report, hydrogen uptake and its effects and consequences. Hydrogen appears as a biproduct of the oxidation of zircaloy, and is readily abundant, bound in water molecules, in the moderator surrounding the cladding. This hydrogen will travel into the zircaloy matrix and cause various undesirable effects.
HYDROGEN PICK-UP
It has long been known that hydrogen entering solid metals causes embrittlement, which in turn possibly results in undesirable cracking. Even though research and development has been conducted on the subject for several decades, many of the fundamental mechanisms are still not fully understood, to a great extent due to the fact that there are too many factors playing a role.
It has been shown in an operating PWR that approximately 16 % of these hydrogen atoms are picked up by the cladding. The hydrogen together with the zirconium creates hydride precipitates called zirconium hydrides, or simply hydrides. At a certain point, depending mostly on temperature, the hydride precipitation solubility is reached and hydride platelets will begin to form. Figure 8 below shows the solubility limit of hydrogen in zircaloy as a function of temperature.
10
8 9
Low burn-up (20-40 MWd/kgU) BWR PWR 20-100 ppm 20-200 ppm
There are elements, mainly in the moderator, that accelerate the hydrogen uptake. The most common accelerant is nickel, hence the name, the nickel window effect. Nickel acts as a catalyst and separates hydrogen molecules into hydrogen atoms which are far more readily picked up by the zirconium, hence the enhanced 9 hydriding. Since it is generally cooler on the outside of the cladding, hydrides have a tendency of moving from the inside of the cladding to the outside. This thermal diffusion causes hydrides to form rims surrounding the claddings. The rims have a significantly higher hydrogen concentration and are therefore a lot more brittle and thus more prone to fractures. For that reason, rims are a very undesirable effect of hydriding.
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To understand the hydrogen-zirconium interaction in detail it is helpful to know basic properties such as crystal 12 structures, density and such. These have been obtained and are shown in Table 4.
TABLE 4. BASIC PROPERTIES OF ZIRCONIUM HYDRIDES9.
EFFECTS OF HYDRIDING
Effects that can occur are accumulation of hydrides in blisters, delayed hydride cracking and embrittlement. Hydride blisters are, as the name suggests, accumulations of hydrides in certain areas in which hydrogen concentrations can be very high. Several types of failures have been discovered in this research. Some of them are covered below.
HYDROGEN EMBRITTLEMENT
Hydrogen embrittlement is as the name suggests a change in the mechanical properties of the zircaloy due to 9 hydrogen pick-up. Embrittlement occurs mainly in the temperature range between 100 - 300C . At higher temperatures the hydrides become ductile and are no longer hazardous as the risk for fractures decreases significantly.
FIGURE 10. A) STRESSDIAGRAM FOR DIFFERENT TEMPERATURES. B) RELATIVE DUCTILITY AS A FUNCTION OF HYDROGEN CONTENT FOR DIFFERENT TEMPERATURES9.
FIGURE 11. SCHEMATIC ILLUSTRATION OF THE DIFFUSION OF HYDROGEN TOWARDS A CRACK TIP. THE LARGER ARROWS INDICATE THE DIRECTION OF THE EXTERNAL STRESS. THE CRACK PROPAGATION DIRECTION IS NORMAL TO THE DIRECTION OF APPLIED STRESS9.
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BLISTERING
Sometimes the inside of the fuel cladding is lined with another zirconium alloy or pure zirconium, to prevent corrosion from the fission products. If the cladding wall is penetrated, perhaps by corrosion, coolant may enter the fuel chamber, where it vaporizes. The steam will now oxidize the fuel, leaving it very rich in hydrogen. If the protective layer on the inside of the cladding is defective, in the vicinity of the steam cavity, hydrides will form in large quantities. These formations are called hydride blisters (Figure 12). From these blisters, hydrogen may diffuse into the matrix creating radial hydrides. They are called radial because their direction of propagation is
radial. Thus, their crack direction is axial as is the direction of applied stress. This is dire, because it greatly 13 enhances the risk of the cladding to rupture.
13 14
(Alvarez, Banerjee och Bickel) (Rnnberg) Uppsala University | Incidents caused by hydriding in fuel claddings 13
It was shown that grit-blasting with such lances causes small stainless steel particles to be embedded at the inner guide tube surface, acting as hydrogen windows. Ni was deposited onto the cladding surface, causing hydrogen, which was added to the coolant at about 150 C, to catalytically diffuse into the cladding. It was shown during the investigation that a necessary condition for hydrogen uptake was that Ni in the coolant was high during start-up, and that hydrogen was added to the water before the creation of a protective oxide layer 15 could prevent hydrogen uptake . The problem was solved by altering the production method, i.e. the grit-blasting, the annealing etc. Other measures were also taken, for example adding hydrogen to the coolant at a later time, allowing the protective 16 oxide layers to form. No incidents have been reported since . Although primary damages caused by hydriding are no longer problems in neither BWRs nor PWRs, secondary damages are still the root of much trouble. At Oskarshamn Nuclear Power Plant, the fuel claddings in reactor 3 are much more prone to hydriding than the fuel claddings in reactors 1 and 2. Quite much time has been spent trying to understand the cause for this, and some measures have been taken to reduce a lot of the effects of hydriding in reactor 3. For example, the coolant purification system in O3 is slightly different from the coolant purification system used in O1 and O2. Therefore, it is believed that this may be the source of the problem. The water purification system has been altered, but whether or not this will solve the problem is not yet known, since these measures have been taken rather recently and some time must pass in order for sufficient statistics 16 to be built up.
Since1971, some 7000 shipments of used up nuclear fuel has been made over many millions of kilometers with no personal injury or property damages, no breach of containment and very low dose rate to the personnel involved.
15 16
(Pettersson, Bengtson and Andersson) (Rnnberg) 17 (How nuclear works) 14 Transporting used up fuel | Uppsala University
18 19
(Rnnberg) (2008 Performance Indicators) 20 (Glossary of Terms Used in Radiological Protection) Uppsala University | Fission gas release and radiation dosages 15
ONGOING PROJECTS
CLADDING MATERIAL
The nuclear fuel companies, Westinghouse in particular, continue to conduct research on ways to improve the cladding and its material to enhance its resistance to hydrogen uptake. Westinghouse is also trying to minimize the space found between the fuel and its cladding where the hydrides, which attract to lower temperatures, tend to gather up. However, this space does serve a purpose when the temperature of the fuel pellets rises and the fuel itself begins to expand.
SCIP
Since 2004 Studsvik has been the operating agent of an OECD project called SCIP, Studsvik cladding integrity program, which has just been extended to run for another 5 years last summer under the name of SCIP II. This project has addressed most hydrogen-related failure mechanisms within the fuel cladding. Many cladding materials have been tested and models have been created to simulate how the fuel as well as these materials is affected during reactor operation. The projects main focus is to increase the overall operation safety of our nuclear power plants to avoid unplanned maintenance due to fuel failure. Most failure mechanisms studied have been well-known for many years, but SCIP gives a deeper knowledge of the mechanisms as fuel conditions change now and in the future in connection with increased power extraction 21 from the fuel.
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BIBLIOGRAPHY
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