HYDROGEN: A KEY CONSTITUENT IN NUCLEAR POWER PLANT DISASTER

dilip

Nuclear power holds the promise of a sustainable, affordable, carbon-friendly source of energy for the twenty-first century on a scale that can help meet the world's growing need for energy and slow the pace of global climate change. However, a global expansion of nuclear power also poses significant challenges. Nuclear power must be economically competitive, safe, and secure; its waste must be safely disposed of; and, most importantly, the expansion of nuclear power should not lead to further proliferation 1 of nuclear weapons. his report provides an overview of the proliferation ris!s of nuclear power and how they could be managed through a combination of technical, political, and institutional measures .

Introduction
he basic goal of nuclear safety is to mantain the intrigity of containment and containment to prevent the release of fission product into environments . Hence nuclear power plant is designed , constructed and operated in conformity of strignent safety standards for the protection of plant personnel, public and environment. "n case of severe accident in a nuclear he power plant,the heated #irconium metal reacts with steam produces hyrogen. combustion of this enormous amount of hydrogen can generate short term pressure or detonation forces that may exceed the ultimate strength of containment and lead to early containment failure. $efence in depth in nuclear power plant is achieved primarily by means of four successive barriers which prevent the release of radioactive material %fuel matrix, cladding, primary coolant boundary and containment&, and these barriers are primarily protected by three

levels of design measures' prevention of abnormal operation and failures %level 1&, control of abnormal operation and detection of failures %level (& and control of accidents within the design basis %level )&. "f these first three levels fail to ensure the structural integrity of the core, e.g. due to beyond the design basis multiple failures, or due to extremely unli!ely initiating events, additional efforts are made at level * to further reduce the ris!s. +or most N,,s, severe accidents lead to hydrogen release rates that exceed the capacity of hydrogen control measures at conventional design basis accident %$-.&./ocal high hydrogen concentrations can be reached in a short time, leading to combustible gas mixtures in the containment. 0oreover, a long term pressure build-up may occur due to steam generation through decay heat and1or through the generation of non-condensable gas from the interaction of the molten core with the containment basemat concrete.

he production, distribution and combustion of hydrogen in case of post accident scenario are very complex and highly plant and condition specific phenomena. Hydrogen combustion may ta!e place in

temperature increases above 71)22 6, due to rapid oxidation of 5r and the strongly exothermic nature of the reaction. 8rders of magnitude of the H ( mass assuming a complete oxidation of 1229 of the 5r mass with steam following the complete chemical reaction' 5r : (H(8 ; 5r8( : ( H( : <H <H = - >?@.@ !A1mole 5r Bhere <H is an energy released during the chemical reaction and 2.2**( !g H( per 6g 5r was oxidi#ed. . very rough order of magnitude of hydrogen created by full 5r oxidation could be up to 1222 !g of H( for a typical ,BC compared to at least ) to * time more for a -BC with the same power %around 1222 0B%e&&, and around 1122 !g of H( for a 1222 0B%e& BBDC. $uring the loss of geometry of the core, experts presently consider that the main source of released H( comes from %E-5r-8& melt oxidation. 4orrect modelling of the %E5r-8& melt oxidation is still under investigation, based on newly dedicated experimental programmes. 4rust failure and melt relocation to the lower plenum are FlatephaseG greater core than damage for the progression early phase phenomena for which the uncertainties are phenomena ."n the late core degradation phase, hot melt can drop into the lower plenum of the vessel, which may be filled with water. Huch inIection of the melt into the water, for instance in the form of a Iet, and fragmentation of the melt, would lead to an increase of the oxidation reaction surface %fragmented particles& and to a strong

variety of ways such as' mild deflagration fast or accelerated flames, deflagration to detonation transition. .n understanding of all these phenomena is crucial for planning and implementing effective hydrogen management measures. combustion "n an through hese measures use as of at

include enhancement of mixing, deliberate igniters, such recombiners, and post-accident inerting. accident situation +u!ushima where the fuel became very hot, a lot of hydrogen is formed by the oxidation of #irconium fuel cladding in steam at about 1)2234. his is beyond the capability of the normal hydrogen recombiners to deal with, and operators must rely on venting to atmosphere or inerting the containment with nitrogen. MAJOR WHILE SOURCES OF HYDROGEN TOWARDS PROGRESSION

SEVERE ACCIDENT: "n case of severe accident when core is uncovered, the heat transfer from the fuel to the steam is small compared with decay heat produced and, hence, the he fuel high temperature increases.

temperature leads to oxidation of the 5r fuel cladding and hydrogen generation and can also lead to clad ballooning and rupture. 4lad rupture is the cause of the first fission product release. he heat-up rate can increase to well above 1 61s as the local

production of steam, which can oxidi#e the available metal. "n-vessel hydrogen production coming from steel oxidation is around 129 to 1>9 of the total in-vessel hydrogen production. $uring the melting of the core, when steam comes into contact with the remaining -*4 inside the control rods, it is li!ely that any exposed - *4 will react rapidly with the steam atmosphere. . rough order of magnitude of the H( production is 2.1> to 2.)2 6g H ( per !g of -*4 oxidi#ed by steam. 4onseJuently, the Juantity of H( generated by the oxidation of -*4 remains low for ,BCs and BBDCs compared to the H( produced by the oxidation of the fuel rod cladding. Nevertheless, the strong linear !inetics of the oxidation of -*4 could contribute to local effects in the containment, such as hydrogen poc!ets. "n case of faliure of lower head of vessel uranium may come into contact with steam, uranium dioxide reacts with steam to produce E8( and hydrogen. he extent of

compartments. Dxperts generally assume that 1229 of the remaining 5r is oxidi#ed during the $4H event %or very shortly after& in the containment or the cavity pit . "n case of a reactor vessel bottom breach when the reactor coolant system is depressuri#ed, a gravitational corium drop occurs and in case of a dry cavity pit, a molten core coolant interaction %044"& starts. he 5r and 4r masses contained in the corium, coming from the remaining 5r and 4r masses in the corium at the time of the vessel lower head failure, undergo a fast oxidation in the steam and 48( environment, where the 48( is coming from the thermal decomposition of the basemat concrete. $ue to the violent gas release from the concrete into the corium at the beginning of 044", the masses of H(8 and 48( are well in excess of those of 5r and 4r and are in close contact with these. Dxperts generally assume that 1229 of these remaining 5r and 4r masses will be oxidi#ed by steam to give H( and 48 within the first hour %even less& following the beginning of 044". 8ther possible ex-vessel H( production ma occur by radiolysiss of water, corrosion reactions etc. Cadiolysis of water occurs both during normal operation and under accident conditions. "t may ta!e place in the core and in the sump. "t involves the decomposition of water molecules by radiation, which produces various radicals. he net result is the production of hydrogen and oxygen molecules in essentially a stoichiometric ratio. he phenomena are

the reaction is dependent on the partial pressures of steam and hydrogen. "n case of a reactor vessel bottom breach when the reactor coolant system is pressuri#ed %accident scenarios as loss of offsite power, small brea! /84.&, a direct containment cooling%$4H& can happen . he 5r still present in the corium at the time of the vessel breach undergoes a very fast oxidation with the available oxygen and steam. his availability depends on the design of the cavity pit and surrounding

reasonably understood for pure water at room temperature. 0ore uncertainties exist for elevated temperatures and the presence of solved matter and impurities. ,rovisions are usually already ta!en with respect to water radiolysis for post design basis accidents %e.g. /84.&. "n a containment, the only significant sources of hydrogen from corrosion are reactions of #inc and aluminium. 5inc is present in some types of paint and in galvani#ed steel. hese reactions are of importance for high and low pH values. Dvaluations have shown that the amount of hydrogen that could be produced by corrosion reactions is in the order of 122 !g in some hours, i.e. far less than from other sources. RISKS FROM HYDROGEN COMBUSTION he maIor ris!s due to combustion of hydrogen produced during sever accident are the loss of containment integrity and failure of safety systems. hese ris!s may cause increase in pressure and thermal loads manifold which can be reason for structural and components damage. be 0ild deflagrations, which occur in lean hydrogen mixtures; +ast deflagrations, which occur at higher hydrogen concentrations, or are caused by flame acceleration from flames travelling initially at lower speed, and1or Iet ignition; $eflagrations that accelerate and transit he various mode of hydrogen combustion may

to detonation %Fdeflagration to detonation transitionG, sections; /ocal detonation, at high hydrogen concentration, or as the conseJuence of a $$ process; Klobal detonation. $$ &, caused by the mechanisms described in the previous

hermal loads can be intermittent %free flames& or continuous %diffusion1standing flames&. +ree flames occur after ignition in a gas cloud; they typically last seconds. Htanding flames may occur at a location where the hydrogen from the source mixes with air. . typical example is a -BC suppression pool surface, where standing flames can occur when hydrogen is driven from the drywell through the water of the suppression pool. .t low H( concentrations, typically *L?9 H(, deflagrations produce only slow flames, and loads are Juasi-static. hey are basically calculated from the energy balance, the !ey parameter being the number of hydrogen moles that react with oxygen. 4ombustion is often not complete, i.e. not all hydrogen will burn. +or structural response, it can be assumed that the loads are static, i.e. no dynamic response needs to be ta!en into account. .bove about ?9 H( concentration, flames may accelerate and larger loads may result. "n addition, combustion is more complete, so that loads also increase due to the fact that more hydrogen is burned. Note that flame acceleration is a complex process, and does

not

depend

Iust

on

the

hydrogen

codes, often of the type of finite elements, is available to investigate the response of the structure to the dynamic load. HYDROGEN CONTROL AND MITIGATION Containm nt atmo!"# $ In $ti%ation P$ &in $ti%ation hese are the counter measures which are basically used for the -BC having a small containment which is not accessible during normal operation. "n this case an inerti#ation with nitrogen during normal operation did not endanger the staff and disturb the operation. Hince the containment free volume is not too large the inerti#ation and deinerti#ation can be done in hours and the costs are bearable. he hydrogen is produced during a severe accident by oxidation of the cladding and other metallic materials. "f there is practical no oxygen in the containment %M>9& the ris! of hydrogen combustion is near #ero. +or inerti#ation of the containment, e.g. after outage, the cold stored nitrogen is heated by an air heated vapori#er. "t is fed into the containment by using the existing ventilation system Po!t&in $ti%ation +or -BC having large containment which is easily accessible, the inerti#ation during normal operation is not practicable. +or these some investigations for a postinerti#ation were made. ,ost-inerti#ation %post-accident inerti#ation& involves inIection of non-combustible or combustion-inhibiting gases into the containment atmosphere, following the onset of an accident that has the potential of producing significant

concentration, but also on the amount of bloc!age, the degree of confinement, the presence of diluent gases %steam, 48(&, etc. .ccelerated flames produce pressure spi!es, characteri#ed by a high pressure which lasts a very short time. Bhere flames accelerate in a confined volume L typically a reactor containment or its subcompartments L the pressure developed depends on the si#e of the H( gas region, the H( concentration, the si#e of the enclosure and the configuration of obstacles. $etonations produce shoc! waves, resulting in high pressures, with a very rapid decay after the pea! value. "f the detonation results from a transition from deflagration to detonation, these loads can even be higher. ,ea! pressures of (>2 bar have been observed in reflected shoc! waves, in an experiment initially at 1 bar pressure. "n order to obtain the actual ris! from these loads, the structural response of the containment %or other endangered Higher structure&, pea! loads must do be not obtained.

necessarily result in higher structural loads' the pea! pressure alone is insufficient to determine the vulnerability of a structure. ,ressure records associated with $$ or a stable detonation display a sharp pressure rise followed by the decay, which is relatively rapid for $$ . Hlow and fast deflagrations, on the other hand, display a more gradual pressure rise and decay. he details of the pressure histories can be very important in assessing the response of a particular structure. . variety of structural analysis

Juantities of hydrogen. .n early and rapid inerting has to be decided and introduced by the plant personnel before exceeding the flammability limits of the gas mixture in the containment. Nitrogen and carbon dioxide have been considered as candidate noncombustible %diluent& gases. 4omplete inerting %i.e. combustion suppression at all hydrogen concentrations& is possible only when the carbon dioxide or steam concentration exceeds approximately @2 vol9 in air; inerting with nitrogen reJuires in excess of N> vol-9. "t should be noted that inerting by dilution assumes that the diluent is thoroughly mixed with the atmosphere in the containment by an appropriate diluent distribution system. Po!t&a''i( nt (i)*tion , "n this a relatively small mass of inert gas, inIected in the vicinity of hydrogen release can significantly reduce the detonability of gas mixtures in the region. ,ost-accident dilution is essentially a strategy for purging selected local volumes identified by mixing analysis as trouble spots for accumulation of hydrogen. "nert gas purging used in this way could contribute to eliminating potential flammable or detonable poc!ets that arise prior to complete mixing. However, there exists uncertainty regarding combustioninduced redistribution of gas volumes and the feasibility of maintaining the inerted condition locally, after the first combustion occurs. 8ne more benefit flame is that it decrease1suppresses Ea$)+ , nti)ation acceleration

"n this process the containment is vented deliberately when the calculated combined pressure hydrogen of steam, combustion air and possible the exceeds

containment pressure limits

his controlled

opening of the containment in an early stage of the accident over a certain period of time is assumed to prevent the total loss of containment function by a large crac! or the failure of structures. D )i- $at i.nition $eliberate ignition system is to initiate combustion hydrogen by wherever slow and whenever while flammable mixtures arise, removing the deflagration distributing the energy release spatially and temporally. he rationale for employing intentional ignition contains the assumption that eventual ignition by a random source is inevitable and that the potential damaging effects of combustion %i.e. combustion temperature and overpressures& increase with increasing penetration of the flammable range of compositions. I.nit $! O G)o/ ")*. i.nit $! Klow plug igniters are simple electrical resistance heaters that produce a surface temperature of ?22 to P2234, which is a positive ignition source for flammable mixtures of hydrogen air steam. Klow plug igniters are reliable, robust and are the most energetic of candidate ignition sources for containment, producing ignition at very near the absolute limits of flammability. 0 S"a$1 i.nit $! Hydrogen is particularly suited to spar!

and hence reduces loads.

ignition, having the lowest spar! ignition energy of any combustible fuel. Hpar! igniters are effective ignition sources. "t is important that the freJuency of spar!ing is commensurate with the time scale of local combustible mixture formation %hydrogen release, mixing and steam condensation rates&. 0 Cata)+ti' i.nit $! 4atalytic igniters employ the heat of H( L 8( reactions at a spatial catalytic element to produce surface ignition temperatures high enough to cause ignition. 4atalytic igniters are self-actuating, self powered and continuously Juestion available. regarding he catalytic practical igniter

depleted air and drawing fresh gas from below. power reJuires hus, ,.Cs do not need external or operator to action. ,.C "nstallation units at only place

appropriate locations within the containment to obtain the desired coverage. Cata)+ti' $ 'om-ination an( "o!t&CO2 In3 'tion 4arbon dioxide is inIected in such an amount transition prevented that and while deflagration-detonation detonation catalytic onset are recombiners

remove the hydrogen over time. Hence, the containment structures and eJuipment have only to withstand the static loading caused by %accidental& deflagration. However, the inIection of incondensable gases provides a higher initial pressure for deflagration. hus, it is important that the inIection of carbon dioxide be limited to such an extent that the combined pressure load from carbon dioxide and hydrogen combustion does not exceed the containment pressure capability. he nature of the hydrogen threat to containment and the choice of measures to

performance are related to the range of mixture that can be ignited, the response time and their availability in terms of poisoning, fouling or mechanical damage. he range of operation is a particular concern in rich-limit mixtures where the margin mixtures. Cata)+ti' $ 'om-ination 4atalytic recombiners use catalysts to oxidi#e %recombine& the hydrogen and are operable outside the limits of flammability. ,.Cs are simple devices, consisting of catalyst surfaces arranged in an open-ended enclosure. "n the presence of hydrogen %with available oxygen&, a catalytic reaction occurs spontaneously at the catalyst surface and the heat of reaction produces natural convection flow through the enclosure, exhausting the warm, humid hydrogen between flammability and detonability is narrower than in lean-limit

mitigate

the

hydrogen

threat

depend

strongly on the containment design. here is not one single strategy or techniJue that is universally appropriate for all designs and accident scenarios, or even, for all phases of an accident in a particular design. $ifferent measures may be more appropriate at different locations and at different times during an accident. . completed safety assessment for the particular plant is the only valid context for Iudging the adeJuacy

of safety systems and accident management measures, countermeasures. Ceferences 1. ".D.- D4$84-1@@1 0itigation of Hydrogen Ha#ards in Hevere .ccidents in Nuclear ,ower ,lants ".D.- D4$84-1@@1 (. ritium Ha#ard Ceport' ,ollution and Cadiation Cis! from 4anadian Nuclear +acilities -y $r. "an +airlie Aune (22N ).".D.- D4$84-1>P* .nalysis of Hevere .ccidents in ,ressuri#ed Heavy Bater Ceactors including hydrogen