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2010

Consequences of hydrogen pick-up in fuel cladding


A literature study

Kristiina Sadian, Rickard Johansson and Christian Alex Uppsala University 5/25/2010

[CONSEQUENCES OF HYDROGEN PICK-UP IN FUEL CLADDING] den 25 maj 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.

Uppsala University | Abstract

den 25 maj 2010

[CONSEQUENCES OF HYDROGEN PICK-UP IN FUEL CLADDING]

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

Cladding related problems ......................................................................................................... 8 Hydrogen pick-up ....................................................................................................................... 9


The hydrogen pick-up mechanism ...................................................................................................................... 9 Hydrogen content at different burn-ups........................................................................................................... 10 Zirconium hydride properties ........................................................................................................................... 11

Effects of hydriding .................................................................................................................. 12


Hydrogen embrittlement .................................................................................................................................. 12 Delayed hydride cracking .................................................................................................................................. 12 Blistering ........................................................................................................................................................... 13

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

Abstract | Uppsala University

[CONSEQUENCES OF HYDROGEN PICK-UP IN FUEL CLADDING] den 25 maj 2010

INTRODUCTION AND BACKGROUND


A huge part of the research conducted on nuclear power has been focused on minimizing the downtime of the reactors. A substantial part of the research conducted has been proven to be successful but there is still work to be done. One issue that can cause a reactor shut down is the phenomenon of hydrogen pick-up in the fuel cladding, which is the part of the fuel assembly as can be seen in Figure 3.The hydrogen can cause the cladding to become brittle and crack which leads to radioactive material leaking out into the reactor water and in turn cause the radiation levels outside the reactor to rise. When these radiation levels reach values that are unacceptable the fuel assembly has to be replaced which cannot be done during operation. Changing the fuel assembly thereby requires a shutdown of the reactor and the maintenance performed such as the cooling and the fuel exchange typically requires the reactor to remain inactive for a week which of course is a very expensive consequence. Other reasons for the continued research in hydriding are the power uprate of the Swedish reactors and the progress toward higher and higher burn-ups. The government has allowed uprating of Ringhals 1 and 2, Oskarshamn 2 and 3, and Forsmark 1-3 and this power uprate has already begun to some extent. This, of course, creates higher demands on the fuel cladding.

PURPOSE AND AIM OF THIS STUDY


This project is mainly a literary study with the purpose of creating an overview of the mechanisms and consequences related to hydrogen uptake as well as giving insight to current research and yet unanswered questions. It is a collaboration between Uppsala University and Vattenfall AB, with the purpose of giving students an opportunity to apply their knowledge on real problems at the same time as Vattenfall benefits from the students fresh perspectives, overall an exchange of in-depth knowledge and understanding. A visit was made to Studsvik in Nykping, together with Hans Henriksson, our supervisor, and Anna-Maria Wiberg, both from Vattenfall. At Studsvik, experts in the research field of cladding related issues; Anna-Maria Alvarez, Clara Anghel, Slava Griegoriev, held seminars as well as gave a guided tour of the laboratory facility for mechanical testing. Furthermore, interviews have been made with senior specialists at Studsvik, Anna-Maria Alvarez, at Westinghouse, Mats Dahlbck, and at the Oskarshamn power plant, Gunnar Rnnberg.

Uppsala University | Introduction and background

den 25 maj 2010

[CONSEQUENCES OF HYDROGEN PICK-UP IN FUEL CLADDING]

NUCLEAR REACTORS IN THE WORLD TODAY


There are 438 nuclear reactors in the world today (May 2010) operating in 30 countries, accounting for 15 % of the worlds total electricity production. Table 1, below, shows general information about the nuclear reactors in the world today. Worth noticing are the different types of nuclear reactors, water cooled and moderated reactors stand for 91 % of the total amount of reactors.
TABLE 1. GENERAL INFORMATION ABOUT NUCLEAR REACTORS IN THE WORLD 20081.
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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

Fuel enriched UO2

Coolant water

Moderator water

94 44

86.4 24.3

enriched UO2 natural UO2

water heavy water CO2

water heavy water graphite

UK

18

10.8

Russia

12

12.3

natural U (metal), enriched UO2 enriched UO2

water

graphite

Japan, France, Russia Russia TOTAL

4 4 441

1.0 0.05 386.5

PuO2 and UO2 enriched UO2

liquid sodium water

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%.

FIGURE 1. OWNERSHIP OF NUCLEAR POWER PLANTS IN SWEDEN 20092 .

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(World Nuclear Association) (Svensk Energi) 4 Nuclear reactors in the world today | Uppsala University

[CONSEQUENCES OF HYDROGEN PICK-UP IN FUEL CLADDING] den 25 maj 2010

GENERAL CLADDING INFORMATION


WHAT IS THE CLADDING ?
Cladding is used to keep fuel in place, which is necessary to control the reactor. It is also used to confine fission gases so that they dont escape out of the reactor core. Since the most common types of reactors are PWR, BWR and CANDU, these claddings will be shortly discussed.

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.

FIGURE 2. CANDU FUEL ASSEMBLY4.

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(Gerry d. Moan) (Nuclear Fuel) Uppsala University | General cladding information 5

den 25 maj 2010

[CONSEQUENCES OF HYDROGEN PICK-UP IN FUEL CLADDING]

FIGURE 3. THE LEFT ASSEMBLY IS A WESTINGHOUSE PWR FUEL DESIGN. THE MIDDLE ASSEMBLY IS A WESTINGHOUSE SVEA96 OPTIMA2 BWR FUEL.

DESIRED CLADDING PROPERTIES


The fuel cladding is constructed to withstand the tough conditions and the strain it faces in a nuclear reactor. A crack in the cladding could cause contamination of radioactive materials in the moderator, or worse yet, an even more damaged cladding could cause release of the fuel into the moderator, thus losing control of the fission processes. This of course creates extremely high requirements on the fuel cladding, that it should have 5 all the right properties. These attributes are: Adequate y at high T and during irradiation Resist corrosion Dimensionally stable Predictable mechanical properties High thermal conductivity Low neutron capture cross-section Easy to fabricate and install Easy to reprocess Low cost Low demand on scarce resources

(Kulcinski) 6 General cladding information | Uppsala University

[CONSEQUENCES OF HYDROGEN PICK-UP IN FUEL CLADDING] den 25 maj 2010

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.

Table 2, below shows the different additives in

zirconium based alloys and the applications of the different

alloys.

Uppsala University | General cladding information

den 25 maj 2010

[CONSEQUENCES OF HYDROGEN PICK-UP IN FUEL CLADDING]

Table 2. Different zirconium based alloys, alloying elements and application6.

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

Typical Alloying element w%


Sn 1,5 1,5 1,3 0,8 1 0 0,8 0 0 0 1,2 Nb 0 0 0 0 1 1 0 1 2,5 2,5 1 Fe 0,10-0,20 0,2 0,2-0,24 0,3 0,1 some 0,6 0 0 0 0,4 Cr 0,10-0,15 0,1 0,1 0,2 0 0 0,2 0 0 0 0 Ni 0,05 0 0 0 0 0 0 0 0 0 0 O 0,11 0,13 0,13 0 0 0,12 0,15 0,06 0 0,12 0,1

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 .

FIGURE 5. TYPICAL ALLOYING ELEMENTS IN COMMON ZIRCALOYS6,7.

FUEL CLADDING MATERIALS USED IN SWEDISH REACTORS


Swedish reactor types are boiling water reactors (BWRs) and pressurized water reactors (PWRs). In BWRs, Zircaloy-2 is the most commonly used material for fuel cladding whereas Zircaloy-4 is the preferred one in PWRs. Recently though, Zirlo is growing increasingly popular in the PWR type reactors. Zirlo is less prone to 8 hydriding than Zircaloy-4 but not as resistant to corrosion.

CLADDING RELATED PROBLEMS


There are two types of damages within the reactor of a power plant, primary and secondary. The primary damages are those which can be caused without the influence of any other damages prior to that primary damage in question. The secondary damages on the other hand cannot appear without being a result of a primary damage. The problematic issues caused by hydrogen uptake in the fuel cladding today are of the secondary type. The hydriding could also appear as a primary damage if the cladding hadn't been dried enough during its construction. This is however an extremely rare scenario in the power plants of today since the issue is now very well known among the nuclear fuel suppliers.

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(Studsvik Seminar 16) (Dahlbck) 8 (Rnnberg) 8 Cladding related problems | Uppsala University

[CONSEQUENCES OF HYDROGEN PICK-UP IN FUEL CLADDING] den 25 maj 2010


As mentioned above, there are several problems that arise in association with the cladding. The most common problems are debris damages, fretting, creep, corrosion and hydrogen uptake. Debris damages arise for example in BWRs when metal sand from the sand blasting process get stuck on the cladding and later on in the 8 reactor cause fretting on the cladding due to vibrations . In PWRs, a reoccurring issue is hydraulically induced 8 vibrations. Common to all types of reactors is creep which refers to movements or permanent deformations of solid materials that result from long term exposure to high levels of stress and often high temperatures. There are several different corrosion mechanisms of which shadow corrosion and nodular corrosion are of interest here. Galvanic corrosion, called shadow corrosion in the nuclear industry, corresponds to a localized enhanced corrosion of zircaloy when it is close to or in contact with another metallic component that is usually more noble than the zircaloy. This results in a corrosion surface on the zircaloy shaped as a mirror image of the more noble component, hence the name shadow corrosion. Figure 6 depicts this phenomenon, a cladding tube with a 9 mirror image of a control rod handle. Nodular corrosion refers to the formation of thick oxide spots on the zircaloy cladding, as shown in Figure 7. Additives, such as iron, nickel
FIGURE 6. SHADOW CORROSION OF ZIRCALOY FROM CONTROL ROD HANDLE9.

and chromium reduce these effects.

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

FIGURE 7. NODULAR CORROSION ON ZIRCALOY CLADDING9.

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.

THE HYDROGEN PICK -UP MECHANISM


What is known, is that the oxidation of zirconium liberates hydrogen ions as shown by the chemical reaction below: 2 H2O+Zr ZrO2+4H
- 9

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.

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(Rnnberg) (Studsvik AB) 10 (Gerry d. Moan) Uppsala University | Hydrogen pick-up 9

den 25 maj 2010

[CONSEQUENCES OF HYDROGEN PICK-UP IN FUEL CLADDING]

FIGURE 8. HYDROGEN CONTENT IN ZIRCALOY AS A FUNCTION OF TEMPERATURE9.

HYDROGEN CONTENT AT DIFFERENT BURN-UPS


As time goes, more and more hydrogen will gradually diffuse into the zircaloy. Therefore, it is important to investigate hydrogen concentrations as a function of burn-up, as it has become desirable with higher and 11 higher burn-ups. Burn-up is by definition the amount of energy, expressed in MegaWatt days, per unit mass fuel, expressed in kg pure Uranium, and measures the amount of thermal energy generated in the reactor in that time period. In Sweden, the burn-up is 45 MWd/kgU and progressing towards a burn-up of 50 MWd/kgU. Germany, Switzerland and USA are the countries with the highest burn-ups in the world at the moment, with about 50 MWd/kgU and progressing towards 55 MWd/kgU. In the long run, the goal is to reach burn-up values 8 of 70-75 MWd/kgU. Table 3 below shows the hydrogen content depending on burn-up.
TABLE 3. HYDROGEN CONTENT AS A FUNCTION OF BURN-UP9.

Low burn-up (20-40 MWd/kgU) BWR PWR 20-100 ppm 20-200 ppm

High burn-up (50-75 MWd/kgU) 100-500 ppm 100-1000 ppm

Temperature [C] 300-340 360-400

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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(Rnnberg) (About fuel burn-up rates) 10 Hydrogen pick-up | Uppsala University

[CONSEQUENCES OF HYDROGEN PICK-UP IN FUEL CLADDING] den 25 maj 2010

ZIRCONIUM HYDRIDE PROPERTIES


Depending on hydrogen content and temperature, the hydrides will form in different phases which in theory might affect what kind of effects the precipitates might cause on the cladding. Figure 9 below shows the 9 different existing hydride phases, however, only the -phase has been observed.

FIGURE 9.PHASE DIAGRAM FOR ZIRCONIUM HYDRIDES9.

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.

Phase -Zr (ZrH) (ZrH1,6) (ZrH2)

Crystal structure hcp fct fcc fct

Latticeconstants [nm] a c 0,323 0,46 0,478 0,498 0,515 0,497 0,445

Density [g/cm ] 6,51 5,82 5,64 5,61

Mean interatomic distance [nm] 0,322 0,334 0,338 0,339

(Studsvik AB) Uppsala University | Hydrogen pick-up 11

den 25 maj 2010

[CONSEQUENCES OF HYDROGEN PICK-UP IN FUEL CLADDING]

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.

DELAYED HYDRIDE CRACKING


A well-known property of Zirconium and its alloys is that it has a low solubility for hydrogen. When a sufficient amount of hydrogen has been solved into the Zirconium matrix, precipitation of the hydrogen commences, forming platelets consisting of hydrides. If such a platelet is formed sufficiently close to a notch or crack tip in the material, a diffusion of hydrogen, from the platelet towards the crack tip, occurs (Figure 11). As more and more hydrogen is gathered at the crack tip, the yield stress there reduces, until it reaches the actual applied stress, causing material failure. This process is called delayed hydride cracking or DHC.

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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Effects of hydriding | Uppsala University

[CONSEQUENCES OF HYDROGEN PICK-UP IN FUEL CLADDING] den 25 maj 2010


The reason for the migration of hydrogen, from the platelets to the crack tip, is that the chemical potential of the hydrogen at the crack tip differs from the chemical potential of the hydrogen in the platelets. The chemical potential depends on the local hydrostatic stress field: an increase in stress causes the chemical potential to reduce. Hence, since the hydrostatic stress field is reduced in the platelets, the chemical potential is greater there, inducing a diffusion of hydrogen towards the crack tip. The crack velocity is determined by the chemical potential as well. The greater the chemical potential in the matrix, the higher the driving force and the larger velocity is a consequence.

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

FIGURE 12. A PHOTOGRAPH OF A HYDRIDE BLISTER. COURTESY OF STUDSVIK9.

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.

INCIDENTS CAUSED BY HYDRIDING IN FUEL CLADDINGS


Nowadays, primary damages caused by hydriding are almost completely extinct in BWR and PWR type 14 reactors . However, there have been some occurrences. For example, during the 1990 outage at Ringhals nuclear power plant, two guiding tubes broke during insertion of control rods in the pool. Investigation showed high hydrogen contents in the Zircaloy-4 guide tubes. Hot cell examination revealed that the average hydrogen content was about 3000 ppm, which may be compared to normal hydrogen contents of about 200 300 ppm. This was a clear indication that hydrogen uptake was stemming from a different source than ordinary corrosion. These particular guide tubes had been grit-blasted on the inner surfaces with a stainless steel lance.

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(Alvarez, Banerjee och Bickel) (Rnnberg) Uppsala University | Incidents caused by hydriding in fuel claddings 13

den 25 maj 2010

[CONSEQUENCES OF HYDROGEN PICK-UP IN FUEL CLADDING]

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.

TRANSPORTING USED UP FUEL


When transporting radioactive materials, security is a very important issue. High demands are made on the package in which the material is being stored. Depending on the potential hazard posed by the transported material, different packages are utilized. There are three types of packages: type A, type B and type C, where type C is the most secure one. Nuclear waste is transported in B type packages, which are designed to maintain 17 shielding from gamma and neutron radiation, even under extreme conditions.

FIGURE 13. LOADING OF A SHIPMENT OF NUCLEAR WASTE PRODUCTS IN A TYPE B PACKAGE17.

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

[CONSEQUENCES OF HYDROGEN PICK-UP IN FUEL CLADDING] den 25 maj 2010

TRANSPORTING DAMAGED FUEL CLADDINGS


One might think that even though there are very little risks involved in transporting unspoiled fuel claddings, there might be many risks involved in transporting burnt up fuel, if a fuel cladding has cracked open. But protocols have been developed to maximize safety. For example, at the Oskarshamn nuclear facility, damaged fuel claddings are removed from the fuel element and gathered in a bundle. The bundle is then put in a leak proof container suitable for transport, i.e. a B type package. If a cladding has been completely ruptured, it must be put inside a security container of its own, before it is put into the bundle. Thus, transporting damaged fuel claddings does not appear to be a tougher issue than transporting intact 18 ones .

FISSION GAS RELEASE AND RADIATION DOSAGES


As mentioned earlier, a negative consequence to cracks in the cladding is fission gas release into the moderator. This is an undesirable effect since these fission products are often radioactive and thus increase 19 radiation levels in the moderator and therefore also to the personnel working at the power plants. The figures below show the collective radiation exposure, i.e. the average effective dose multiplied by the number 20 of people exposed to the radiation . Measures are taken to decrease these values further.

FIGURE 15. COLLECTIVE RADIATION EXPOSURE, BWR19.

FIGURE 14. COLLECTIVE RADIATION EXPOSURE, PWR19.

FIGURE 16. COLLECTIVE RADIATION EXPOSURE, CANDU19.

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(Rnnberg) (2008 Performance Indicators) 20 (Glossary of Terms Used in Radiological Protection) Uppsala University | Fission gas release and radiation dosages 15

den 25 maj 2010

[CONSEQUENCES OF HYDROGEN PICK-UP IN FUEL CLADDING]

CURRENT RESEARCH AND DEVELOPMENT


Since the phenomenon of hydrogen uptake in the fuel cladding was discovered several measures to prevent this have been taken. One of these measures has been changing the material of which the cladding is constructed. The alloys used have always been based on zirconium due to its beneficial properties such as resistance to corrosion and its low cross-section values for neutron capture. Even though changing to these new alloys have proven to be a very effective way to reduce the hydrogen uptake there is still a rather extensive demand on more research within the area. The reason for this demand is that many of the reactors currently active today are being upgraded to newer models with extended fuel burnups, increased cycle lengths and elevated energy output. These upgrades lead to higher core temperatures and an increased strain on the materials.

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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(Studsvik Group) 16 Current Research and Development | Uppsala University

[CONSEQUENCES OF HYDROGEN PICK-UP IN FUEL CLADDING] den 25 maj 2010

BIBLIOGRAPHY
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