Nuclear Technology ISSN: 0029-5450 (Print) 1943-7471 (Online) Journal homepage: http://www.tandfonline.com/loi/unct20 Nanofluids for Enhanced Economics and Safety of Nuclear Reactors: An Evaluation of the Potential Features, Issues, and Research Gaps Jacopo Buongiorno, Lin-Wen Hu, Sung Joong Kim, Ryan Hannink, Bao Truong & Eric Forrest To cite this article: Jacopo Buongiorno, Lin-Wen Hu, Sung Joong Kim, Ryan Hannink, Bao Truong & Eric Forrest (2008) Nanofluids for Enhanced Economics and Safety of Nuclear Reactors: An Evaluation of the Potential Features, Issues, and Research Gaps, Nuclear Technology, 162:1, 80-91 To link to this article: http://dx.doi.org/10.13182/NT08-A3934 Published online: 10 Apr 2017. Submit your article to this journal View related articles Full Terms & Conditions of access and use can be found at http://www.tandfonline.com/action/journalInformation?journalCode=unct20 Download by: [The UC San Diego Library] Date: 18 June 2017, At: 01:07 NANOFLUIDS FOR ENHANCED ECONOMICS AND SAFETY OF NUCLEAR REACTORS: AN EVALUATION OF THE POTENTIAL FEATURES, ISSUES, AND RESEARCH GAPS THERMAL HYDRAULICS KEYWORDS: nanofluids, reactor coolant, critical heat flux JACOPO BUONGIORNO,* LIN-WEN HU,* SUNG JOONG KIM, RYAN HANNINK, BAO TRUONG, and ERIC FORREST Massachusetts Institute of Technology, Cambridge, Massachusetts 02139 Received March 23, 2007 Accepted for Publication May 12, 2007 Nanofluids are engineered colloidal suspensions of nanoparticles in water and exhibit a very significant enhancement (up to 200%) of the boiling critical heat flux (CHF) at modest nanoparticle concentrations (ⱕ0.1% by volume). Since CHF is the upper limit of nucleate boiling, such enhancement offers the potential for major performance improvement in many practical applications that use nucleate boiling as their prevalent heat transfer mode. The Massachusetts Institute of Technology is exploring the nuclear applications of nanofluids, specifically the following three: 1. main reactor coolant for pressurized water reactors (PWRs) 2. coolant for the emergency core cooling system (ECCS) of both PWRs and boiling water reactors 3. coolant for in-vessel retention of the molten core during severe accidents in high-power-density light water reactors. The main features and potential issues of these applications are discussed. The first application could enable significant power uprates in current and future PWRs, I. INTRODUCTION Addition of solid nanoparticles to common fluids such as water is an effective way to increase the critical heat flux ~CHF!. The resulting colloidal suspensions are known in the literature as nanofluids.1 Materials used for *E-mail: jacopo@mit.edu and lwhu@mit.edu 80 thus enhancing their economic performance. Specifically, the use of nanofluids with at least 32% higher CHF could enable a 20% power density uprate in current plants without changing the fuel assembly design and without reducing the margin to CHF. The nanoparticles would not alter the neutronic performance of the system significantly. A REL AP5 analysis of the large-break loss-ofcoolant accident in PWRs has shown that the use of a nanofluid in the ECCS accumulators and safety injection can increase the peak-cladding-temperature margins (in the nominal-power core) or maintain them in uprated cores if the nanofluid has a higher post-CHF heat transfer rate. The third application can increase the margin to vessel breach by 40% during severe accidents in highpower density systems such as Westinghouse AP1000 and the Korean APR1400. In summary, the use of nanofluids in nuclear systems seems promising; however, several significant gaps are evident, including, most notably, demonstration of the nanofluid thermal-hydraulic performance at prototypical reactor conditions and the compatibility of the nanofluid chemistry with the reactor materials. These gaps must be closed before any of the aforementioned applications can be implemented in a nuclear power plant. nanoparticles include chemically stable metals ~e.g., gold, silver, copper!, metal oxides ~e.g., alumina, zirconia, silica, titania!, and carbon in various forms ~e.g., diamond, graphite, carbon nanotubes, fullerene!. Nanoparticles are relatively close in size to the molecules of the base fluid and thus, if properly prepared, can realize very stable suspensions with little erosion and gravitational deposition over long periods of time. As of today, more than ten NUCLEAR TECHNOLOGY VOL. 162 APR. 2008 Buongiorno et al. NANOFLUIDS FOR ENHANCED ECONOMICS AND SAFETY OF REACTORS studies of CHF in nanofluids have been reported in the literature.2–12 The findings can be summarized as follows: 1. Significant CHF enhancement ~up to 200%! occurs with various nanoparticle materials, including silicon, aluminum, and titanium oxides. 2. The CHF enhancement occurs at relatively low nanoparticle concentrations, typically, ⱕ0.1 vol%. 3. During nucleate boiling, some nanoparticles precipitate on the surface and form a layer whose morphology depends on the nanoparticle materials. The CHF enhancement mechanism is poorly understood but appears to be related to the presence of this layer. 4. A study of nanofluid post-CHF ~film-boiling! heat transfer also reports greatly accelerated quenching of hot copper spheres in nanofluids.13 At the Massachusetts Institute of Technology ~MIT!, we are conducting basic research on nanofluid heat transfer,14,15 including pool-boiling heat transfer and CHF ~Refs. 16 and 17!, as well as flow boiling CHF ~Ref. 18!, and are also assessing the feasibility of water-based nanofluids for light water reactors ~LWRs!. The potential applications include 1. use of a nanofluid as the primary coolant in pressurized water reactors ~PWRs! to increase the power density in the core 2. use of a nanofluid in the accumulators and safety injection of the emergency core cooling systems ~ECCS! to increase margins during design-basis events 3. use of a nanofluid for reactor cavity flooding to increase safety margins during severe accidents. This paper provides an overview of the features, issues, and research gaps of these applications. The PWR coolant application is presented in Sec. II, the ECCS application, in Sec. III and the severe-accident application, in Sec. IV. II. PWR COOLANT APPLICATION Increasing the power density of operating and0or future PWRs is an effective approach to improving their economic attractiveness. Because the capital cost of a typical PWR accounts for ;65% of the levelized busbar cost of electricity, extracting more energy from an existing reactor or reducing the physical size of future PWRs may reduce the total cost of nuclear power considerably. Power uprates at LWRs have been implemented for decades. The approved, pending, and expected power uprate applications in the United States currently amount to ;5000, 1000, and 1400 MW~electric!, respectively, as reported by the U.S. Nuclear Regulatory Commission ~NRC! website. The objective of our research is to demNUCLEAR TECHNOLOGY VOL. 162 APR. 2008 onstrate that a water-based nanofluid coolant could be used to increase the power density in a PWR plant with only modest changes to plant design, coolant chemistry, and operation.a The main feasibility issues are as follows: 1. chemical and physical stability of the nanoparticle suspension in typical PWR chemistry 2. nanoparticle effects on reactivity and coolant activation 3. thermal-hydraulic performance of the nanofluids. At relatively high nanoparticle loadings ~.1 vol%!, waterbased nanofluids tend to have much higher viscosity than pure water. This would not be acceptable in nuclear systems. However, the CHF gains appear to be associated with low nanoparticle loadings. At such low loadings, the viscosity, thermal conductivity, surface tension, and specific heat of a water-based nanofluid are similar to those of pure water. This is an ideal situation in which only the CHF is affected by the nanoparticles, while other properties basically are unchanged. The nanoparticle materials initially considered are alumina, zirconia, silica, carbon, gold, platinum, and iridium. Of these materials, alumina, silica, and carbon were chosen based on the literature review, gold, platinum, and iridium for their expected stability, and zirconia based on engineering judgment. Nanoparticles made of all these materials are commercially available. II.A. Chemical and Physical Stability Particle sedimentation can occur via a variety of mechanisms, including gravity, inertia, thermophoretic and electric effects, boiling, etc.19 Agglomeration increases the size of the particles, thus greatly increasing the potential for gravity and inertial deposition. Dilute suspensions of nanoparticles ~such as those being studied in our project! tend to be more stable, because the probability of particle-to-particle collision is low. However, even in dilute suspensions, thermal agitation and flow mixing are generally not sufficient to prevent agglomeration. In nanofluids with oxide nanoparticles, agglomeration can be largely reduced by adjusting the pH to create like electric charges on the nanoparticle surface so that the nanoparticles reject each other on contact. With nonoxide nanoparticles, one typically has to resort to surfactants to keep the particles from agglomerating. However, pH is not an independent variable in PWRs; it plays an important role in managing corrosion and thus has to be a Our initial focus is on the PWR. The coolant application for the boiling water reactor ~BWR! does not seem very promising, because nanoparticle carryover to the turbine and condenser could raise erosion and fouling concerns. However, note that small quantities of zinc and noble metals in dissolved form are introduced in current BWRs for corrosion control. 81 Buongiorno et al. NANOFLUIDS FOR ENHANCED ECONOMICS AND SAFETY OF REACTORS controlled within a certain range, typically, 6.9 to 7.4 at room temperature. Therefore, it is necessary to find a nanofluid that is stable within the same allowable pH range, as changing the PWR water chemistry to accommodate the nanofluid is not a viable option. Furthermore, surfactants may undergo serious radiolysis when exposed to core radiation, thus not performing their intended duty. The University of Florida, an MIT partner in the nanofluid project, has obtained some initial encouraging results for carbon ~diamond! nanoparticles without surfactants in prototypical PWR water chemistry,20 but much more work in this area is clearly needed, including the investigation of radiation effects on nanofluid stability, as well as the impact of nanoparticle deposition on corrosion of the fuel cladding. II.B. Nuclear Performance Two potential issues have been analyzed in this area: neutron activation of the nanoparticles and reactivity effects. The equilibrium coolant activity A due to neutron activation of the nanoparticles was calculated by means of the well-known equation A⫽ FsNT ~e ltC ⫺ 1! e l~tc⫹toc ! ⫺ 1 , ~1! where f ⫽ neutron flux s ⫽ capture cross section Representative values of the activity for various nanoparticles are reported in Table I. All activities are calculated for 0.001 vol% nanoparticle loading, 5 ⫻ 10 13 n0cm 2 {s thermal neutron flux, an in-core transit time of 0.6 s, and an out-of-core residence time of ;16 s. Discussions with a health physicist at the Seabrook nuclear power station have established that a reasonable target for coolant activity during refueling is ,0.1 mCi0cm 3. Therefore, nanofluids with carbon nanoparticles should meet this criterion easily, even at higher loadings. Silica and alumina nanoparticles should also meet the criterion because their activity decays rapidly after shutdown. Zirconia nanoparticles are within the limit only at very low loadings, while gold, platinum, and iridium are not acceptable because their activities would remain high during an outage. Thus, the noble metals are discarded from further consideration. For a traditional 17 ⫻ 17 PWR fuel assembly with 5% enriched UO 2 fuel, the effect of the nanoparticle loading on the beginning-of-life ~BOL! reactivity is shown in Fig. 1. The calculations were performed with the popular LWR neutronic code CASMO ~Ref. 21!. It is apparent that the effect on reactivity is minimal. For example, we estimate that the boron equivalent concentration for 1 vol% Al2O 3 nanoparticles is ;3 ppm, i.e., three orders of magnitude lower than the actual boron concentration in PWRs at BOL. The void and Doppler reactivity coefficients were also calculated with CASMO and found practically unchanged from the pure water situation. II.C. Thermal-Hydraulic Performance NT ⫽ target nucleus number density The target is to uprate by 20% the core power density for existing PWR plants. In principle, even more ambitious targets could be set for new plants, as discussed in Ref. 22. For uprates in existing PWRs, the postulated constraints are as follows: l ⫽ radioactive decay constant tc ⫽ in-core transit time toc ⫽ out-of-core residence time. TABLE I Activation of Nanoparticles* Nanoparticle Material Dominant Radionuclide, Decay Half-Life Carbon Silica ~SiO 2 ! Alumina ~Al2O 3 ! Zirconia ~ZrO 2 ! Gold Platinum Iridium C, b ⫺ ~no g! b ⫺ ~g: 1.3 MeV! 28 Al, b ⫺ ~g: 1.8 MeV! 95 Zr, b ⫺ ~g: 0.7 MeV! 198 Au, b ⫺ ~g: 0.4 MeV! 197 Pt, b ⫺ ~g: 0.2 MeV! 194 Ir, b ⫺ ~g: 0.3 MeV! 5700 yr 2.6 h 2 min 64 days 2.7 days 18 h 19 h 14 31 Si, Activity ~per unit coolant volume! 0.001 mCi0cm 3 0.04 mCi0cm 3 10 mCi0cm 3 0.2 mCi0cm 3 3000 mCi0cm 3 6 mCi0cm 3 2500 mCi0cm 3 a *At 0.001 vol% loading and for 5 ⫻ 10 13 n0cm 2 {s thermal flux. a Due to its long half-life, the activity of 14 C does not reach equilibrium during irradiation, so Eq. ~1! cannot be used. The reported activity is based on 60 effective full-power years of operation. 82 NUCLEAR TECHNOLOGY VOL. 162 APR. 2008 Buongiorno et al. NANOFLUIDS FOR ENHANCED ECONOMICS AND SAFETY OF REACTORS 3. Case 3. A combination of cases 1 and 2, e.g., increase the flow and temperature rise by ;10% each. Fig. 1. The BOL reactivity in a PWR fuel assembly with nanofluid coolants. ~The curves for alumina and zirconia nanofluids overlap.! 1. Maintain the traditional 17 ⫻ 17 fuel assembly design to avoid certification of the new fuel design and retooling of the fuel manufacturing facilities. 2. Minimize the changes to the nuclear island components, i.e., no replacement of the reactor pressure vessel, steam generators, and main piping. Replacement of the main coolant pumps is considered tolerable. 3. Maintain the same core outlet temperature to mitigate materials concerns. The reference plant is a standard four-loop Westinghouse PWR. There are three approaches to accommodating the 20% power density uprate: 1. Case 1. Increase the core flow by 20%. 2. Case 2. Increase the core average temperature rise by 20%. A more modest 5% power upgrade, accommodated with a 5% core flow increase, is also evaluated and referred to as Case 4. The main operating parameters for the reference plant and cases 1, 2, 3, and 4 are shown in Table II. The values were calculated with RELAP5 ~Ref. 23! and verified with hand calculations. Replacement of the main coolant pumps is probably needed in cases 1 and 3. Major upgrade of the turbine-generator module is probably needed in cases 1, 2, and 3. The need to replace the pumps and upgrade the turbine-generator module in case 4 will vary from plant to plant, depending on their current margin. Since the steam generators and the core outlet temperature are left unchanged in all cases, the temperature ~and pressure! on the secondary side of the steam generators must be lowered somewhat in order to transfer the higher thermal power. The lower secondary temperature results in a small decrease in plant thermal efficiency, which we estimate to be ;1%, based on the Rankine cycle efficiencypressure curves in Ref. 24. In uprating the power density, we seek, where possible, to maintain or improve the margin to the key thermal-hydraulic limits, i.e., fuel melting during transient overpower and CHF during transient overpower, the latter typically being dominant in PWRs. To evaluate the margin to fuel melting and CHF, we have performed a subchannel analysis of the core using the VIPRE code, developed by the Electric Power Research Institute ~EPRI! for LWR core thermal-hydraulic analysis.25 The code solves the set of finite difference conservation equations for mass, momentum, and energy of the coolant in interconnected subchannels, assuming incompressible homogeneous flow, and calculates the coolant velocity, pressure, and enthalpy fields and fuel rod temperatures. A suite of CHF correlations is provided by VIPRE for the evaluation of the minimum CHF ratio ~MCHFR!, calculated for the given operating conditions. For our calculations, we used the W-3 correlation with TABLE II Operating Parameters for the Reference and Uprated Plants Parameter Reference Case 1 Case 2 Case 3 Case 4 Power @MW~thermal!# Total core flow rate ~kg0s! Effective core flow rate ~kg0s! Bypass flow rate ~kg0s! Tin ~8C! Tout ~8C! Tout ⫺ Tin ~8C! Primary system pressure ~MPa! Secondary system pressure ~MPa! 3 411 18 712 17 799 913 293.2 324.7 31.5 15.50 6.07 4 093 ~⫹20%! 22 291 ~⫹20%! 21 205 1 084 293.1 324.9 31.8 15.50 5.70 4 093 ~⫹20%! 18 979 18 050 929 286.8 324.7 37.9 ~⫹20%! 15.50 5.21 4 093 ~⫹20%! 20 689 ~⫹10%! 19 680 1 009 290.2 324.7 34.5 ~⫹10%! 15.50 5.47 3 582 ~⫹5%! 19 628 ~⫹5%! 18 670 958 293.2 324.7 31.5 15.50 5.98 NUCLEAR TECHNOLOGY VOL. 162 APR. 2008 83 Buongiorno et al. NANOFLUIDS FOR ENHANCED ECONOMICS AND SAFETY OF REACTORS Fig. 2. VIPRE subchannel model representing one-eighth of a 17 ⫻ 17 PWR fuel assembly. ~MCHFR typically occurs in subchannel 2 due to the cold-wall effect.! correction factors accounting for the cold wall ~i.e., unheated surfaces, such as the control-rod guide tubes! effect, the nonuniform axial flux, and the grid spacers. The model simulates the whole core by means of lumped channels for the peripheral fuel assemblies and a detailed subchannel description of the hot fuel assembly. Figure 2 shows the VIPRE subchannel model representing oneeighth of the hot fuel assembly with a standard 17 ⫻ 17 PWR fuel assembly geometry. This model was benchmarked successfully with previous VIPRE simulations performed at MIT ~Ref. 26!. The results of the VIPRE analysis are reported in Table III. It is no surprise that the margin to fuel melting decreases considerably in the uprated cases with respect to the reference case because the number of pins per fuel assembly is the same and the linear power is 20% higher. Since the centerline temperature mostly depends on the fuel thermal conductivity, this margin reduction could not be helped by the use of nanofluids. However, the calculated values of the maximum fuel temperature appear to be well below the 28008C melting point of UO 2 at BOL, i.e., when the maximum linear power occurs. With respect to the reference case ~MCHFR ⫽1.76!, the maximum MCHFR decrease is for case 2 ~MCHFR ⫽ 1.33!. Thus, use of nanofluids with at least ~1.76 ⫺ 1.60!0 1.60 ' 32% higher CHF than pure water would enable the postulated power uprate without a reduction of the margin to CHF. Given the results of our low-pressure pool and flow-boiling CHF experiments 17,18 and the TABLE III Subchannel Analysis Results for the Reference and Uprated Cases* Parameter Reference Case 1 Case 2 Case 3 Case 4 Maximum fuel temperature ~8C! MCHFR Maximum exit quality Maximum exit void fraction Core pressure drop ~kPa! 2377 1.76 0.06 0.26 125 2704 1.60 0.06 0.26 167 2704 1.33 0.11 0.39 126 2704 1.49 0.08 0.32 145 2468 1.72 0.06 0.26 135 *Analysis assumes radial peaking factor Fh ⫽ 1.65, hot spot factor FQ ⫽ 2.5 ~chopped cosine!, ⫹12% overpower, ⫺5% flow, ⫹2.28C inlet temperature, ⫺200-kPa pressure swing. 84 NUCLEAR TECHNOLOGY VOL. 162 APR. 2008 Buongiorno et al. NANOFLUIDS FOR ENHANCED ECONOMICS AND SAFETY OF REACTORS data published so far, this target would seem reasonable. However, verification of CHF enhancement at prototypical PWR pressure, flow, and geometric conditions is clearly needed. The core pressure drop increases by 34, 16, and 8% in cases 1, 3, and 4, respectively, and does not increase in case 2 with respect to the reference case. The corresponding core pumping power increase in cases 1, 3, and 4 is 60, 28, and 13%, respectively, which would probably make it necessary to replace the main coolant pumps. III. ECCS APPLICATION Following a large-break loss of coolant accident ~LB-LOCA! in current LWRs, the primary system inventory is discharged to the containment and the core is uncovered. To prevent excessive fuel overheating in the ensuing transient, the ECCS is actuated so that vessel reflood occurs and core cooling is restored. Because the fuel can be initially very hot ~.7008C!, its rewetting occurs slowly through the development of a quench front, which advances upward in the core. The speed of the quench front and thus the peak temperature reached during the reflood transient depend on a combination of factors, including film-boiling heat transfer, wettability of the fuel surface by the coolant, and localized axial conduction within the cladding near the quench front. The use of nanofluids could afford a significant increase of the quench speed for two reasons: 1. Boiling-induced deposition of nanoparticles on the surface greatly enhances surface wettability. This has been experimentally demonstrated in our laboratory.16 2. Deposited nanoparticles of high-conductivity material ~e.g., alumina! improve localized axial conduction in the cladding near the quench front. The enhanced wettability, especially, is expected to increase the Leidenfrost temperature for the cladding and promote return to nucleate boiling. Quench experiments of small copper balls, whose surface was fouled with nanoparticles, have demonstrated that return to nucleate boiling can be greatly accelerated in nanofluids.13 If this behavior can be reproduced for cylindrical rods, the use of nanofluids in the ECCS offers the potential for enhanced safety margins or even power uprates for those LWRs whose power is limited by the fuel response during the LB-LOCA. For this application, the issue of chemical-physical stability of the nanofluids is much less important than for the PWR coolant application because the ECCS coolant spends most of its lifetime at room temperature and is not exposed to continuous irradiation. Also, the ECCS is actuated in response to seriously abnormal events during which coolant chemistry control is not a priority. NUCLEAR TECHNOLOGY VOL. 162 APR. 2008 The main figure of merit for the ECCS performance is the peak cladding temperature ~PCT!. During a LOCA, the PCT must be kept below 12008C ~22008F or 1473 K! to prevent rapid oxidation of the cladding. To evaluate the PCT during a LB-LOCA, we have used a previously developed and benchmarked RELAP5 input deck for a PWR. The model of the plant, representing the average and hot fuel assemblies in the core, the reactor vessel, the pressurizer, the steam generators and the pumps, is shown in Fig. 3. Note that the three intact loops are simulated as a single lumped loop. The accumulators and the longterm safety injection ~SI! system are also modeled. The six-group point-kinetics model with typical PWR reactivity coefficients is included. The balance of plant is represented by time-dependent junctions connected to the secondary side of the steam generators. The model was first used to generate the steady-state operating conditions reported in Table II. The following assumptions were made for the LB-LOCA analysis: 1. At t ⫽ 5 s, a 100% break occurs in the cold leg of one loop. 2. At t ⫽ ;5.1 s, the reactor scram signal is sent, based on low pressure in the pressurizer and low mass flow rate in the core 3. The SI signal is sent automatically when the pressure falls below 12.9 MPa. 4. At t ⫽ 8 to 9 s, the main coolant pumps trip. 5. The SI flow ~155 kg0s! starts 27 s after the SI signal. The behavior of the PCT during the LB-LOCA for the reference case and cases 1, 2, 3, and 4 is shown in Fig. 4, and a summary is provided in Table IV. The blowdown and reflood peaks are clearly visible in Fig. 4. The maximum value of the PCT is reached during reflood in all cases. As expected, the uprated cases have generally higher PCTs than the reference case during both blowdown and reflood. The core is successfully quenched in all cases, but the time-to-quench is longer for the 20% uprate cases ~cases 1, 2, and 3! than for the 5% uprate case ~case 4!, as expected. To quantify the effect of a nanofluid-based ECCS, RELAP5 was modified for us by the Idaho National Laboratory, to include user-specified multipliers enabling manipulation of the boiling curve. That is, the CHF and the post-CHF heat transfer coefficient can be arbitrarily increased throughout the accident to simulate the effect of a nanofluid. The results of the analysis with the manipulated boiling curve are also reported in Table IV ~bottom four rows! and Fig. 5. It is apparent that a large increase of CHF helps significantly during blowdown but not as much during reflood. On the other hand, an increase in post-CHF heat transfer is key to reducing the PCT during reflood but does not have a dramatic effect 85 Buongiorno et al. NANOFLUIDS FOR ENHANCED ECONOMICS AND SAFETY OF REACTORS Fig. 3. RELAP5 model for the cold-leg LB-LOCA analysis of the PWR. Fig. 4. The PCT history during a LB-LOCA. on blowdown. It should be emphasized that for PWR plants that are not LOCA-limited but CHF-limited, an improvement of the CHF will be sufficient to enable the power uprate. A systematic experimental study of the post-CHF heat-transfer characteristics of nanofluids at prototypical reactor conditions is clearly needed before the merit of nanofluids for the ECCS application can be fully judged. 86 IV. SEVERE-ACCIDENT APPLICATION Advanced LWR systems, such as Westinghouse’s AP1000 and the Korean APR1400, employ an in-vessel retention ~IVR! strategy to mitigate the consequences of hypothetical severe accidents in which the core melts and relocates to the bottom of the reactor vessel. The IVR strategy consists of flooding the reactor cavity and NUCLEAR TECHNOLOGY VOL. 162 APR. 2008 Buongiorno et al. NANOFLUIDS FOR ENHANCED ECONOMICS AND SAFETY OF REACTORS TABLE IV LB-LOCA Analysis Results Blowdown Peak Reflood Peak PCT ~8C! Time ~s! PCT ~8C! Time ~s! Reference Case 1 Case 2 Case 3 Case 4 674 723 853 766 687 7.1 7.7 7.4 7.0 7.0 726 951 924 966 813 85.4 185.0 130.7 122.8 105.0 Case 1 ~⫹100% CHF! Case 1 ~⫹100% post-CHF! Case 4 ~⫹100% CHF! Case 4 ~⫹100% post-CHF! 680 712 635 697 8.2 7.2 7.1 7.1 936 825 749 614 123.0 116.5 92.3 100.45 Case Fig. 5. The PCT history with enhanced CHF and post-CHF during a LB-LOCA ~20% uprate!. removing the residual heat from the molten core through the reactor vessel lower head. Heat removal is limited by the occurrence of CHF on the reactor vessel outer surface, so the use of a nanofluid instead of water can help to better mitigate the consequences of the severe accident. The AP1000 was selected as the reference plant for the analysis. Following core melting, the AP1000 operator floods the reactor cavity with water from the incontainment refueling water storage tank ~IRWST! if the IRWST has not already been drained. Therefore, we envision a system in which small tanks containing a concentrated nanofluid would inject it into the reactor cavity. The resulting diluted nanofluid would then flow along the vessel and remove the heat. The system comprises 2 ⫻100% capacity tanks located above the reactor cavity near the IRWST ~Fig. 6!. Each tank contains ;0.5 m 3 of concentrated nanofluid. A risk-informed analysis of this NUCLEAR TECHNOLOGY VOL. 162 APR. 2008 injection system design has shown that the nanofluid IVR failure probability, given an initiating event leading to core relocation, has a reasonably low value of 0.01 ~Ref. 27!. Note that in this application, there is great flexibility in selecting the type of nanofluid with little concern for its compatibility with the reactor coolant chemistry, because the nanofluid tanks are completely separated from the primary coolant and the ECCS. Therefore, we have selected an alumina nanoparticle nanofluid at 20 wt% concentration, which exhibits excellent colloidal stability. When diluted in the ;2500-m 3 vessel cavity water, this nanofluid gives a target concentration of ;0.001 vol%. To ensure reliable and effective nanofluid injection into the vessel cavity, the tanks are kept at slight overpressure with inert gas accumulators, and the injection lines are equipped with radial spargers. Moreover, effective mixing occurs in the cavity due to the 87 Buongiorno et al. NANOFLUIDS FOR ENHANCED ECONOMICS AND SAFETY OF REACTORS Fig. 6. Schematic of the nanofluid injection system for severe-accident management. coolant flow induced by boiling on the vessel surface. Finally, the time available for mixing is of the order of tens of minutes. Computational Fluid Dynamics ~CFD! simulations using AP1000 as a reference case suggest that nanofluid mixing in the reactor cavity can be realized within a few minutes. The nanofluid tank discharge signal is automatically tied to the operator’s action of manually flooding the vessel cavity, but it can also be actuated independently if the cavity has already been flooded. During normal operating conditions, the nanofluid in the tanks is stagnant and at room temperature, so sampling for quality control is straightforward. To guarantee long-term stability of the nanoparticle suspension in the tanks, the pH is adjusted to ;4 by adding nitric acid to the nanofluid. Given the acidity of the concentrated nanofluid and the presence of nitrates, the material of choice for the injection tanks is titanium grade 2 ~Ref. 28!. Once the nanofluid is diluted in the vessel cavity, the pH shifts toward neutral and nanoparticle stability may become an issue; however, under these circumstances, good stability is needed for only ,1 day, that being the typical timescale of severe accidents. To evaluate the nanoparticle stability when pH changes, we have conducted dilution experiments and measure nanoparticle size changes as a function of time. Large increases in nanoparticle size would indicate agglomeration. The results are shown in Table V. It is apparent that the size changes are minimal, i.e., within the experimental uncertainty ~620 nm! of the dynamic-light-scattering particle sizer chosen for these measurements. Other factors that need to be considered before making a final selection of a nanofluid are ~a! the response of the nanofluid to the dose of radiation it would be exposed to during IVR and ~b! the response of the nanofluid to the coolant chemistry it would encounter in the reactor cavity. Preliminary re88 TABLE V Average Nanoparticle Diameter in Dilution Experiments with Alumina Nanofluids* Time After Dilution ~h! Concentration 20 wt% 0.01 vol% 0.001 vol% 0 1 6 24 37.8 nm n0a n0a n0a n0a a 42.6 nm 32.6 nm 46.7 nm n0a 52.3 nm 33.4 nm 46.7 nm *The experimental uncertainty is 620 nm. a Not applicable. sults of experiments conducted at MIT suggest that Nyacol alumina nanofluid is stable when exposed to doses of radiation it would encounter in IVR ~Ref. 29! but might be unstable when combined with trisodium phosphate ~which would be present in a flooded reactor cavity!. More work is needed in this area. In AP1000 IVR, the coolant boils in a gap between the vessel outer surface and the vessel thermal insulation. The resulting two-phase mixture creates a density difference between the gap and the flooded vessel cavity, which drives a natural circulation flow. A one-dimensional model for the two-phase flow and heat transfer on the vessel outer surface has been developed and used to quantify the residual heat that can be removed by using a nanofluid. This model defines the gap between the reactor vessel outer surface and the thermal insulation as the rising portion coolant flow path ~riser!. The falling portion of the flow path ~downcomer! is outside this gap in NUCLEAR TECHNOLOGY VOL. 162 APR. 2008 Buongiorno et al. NANOFLUIDS FOR ENHANCED ECONOMICS AND SAFETY OF REACTORS TABLE VI Key Input for the IVR Heat Transfer Model Parameter Value Vessel inner diameter Vessel height Lower head height Vessel0insulation gap Inlet temperature Inlet pressure 4.02 m 6.14 m 2.31 m 0.076 m 1008C 0.157 MPa a a Corresponding to a depth of ;15 m from the water level in the reactor cavity. the reactor cavity. Table VI shows several key parameters used in the model. The Levy correlation 30 is used to determine the flow quality in the heated section, and the EPRI correlation 31 is used to determine the void fraction. The momentum equation, including the gravity, acceleration, and wall friction terms, is solved to provide the flow rate for a given heat-removal rate. Finally, the SULTAN CHF correlation,32 which accounts for the effect of the channel inclination, is used to determine the CHF ratio. This model reproduces the power-flow curve of the University of California at Santa Barbara experiments within 2% ~Ref. 33!. A multiplier is used to account for the CHF enhancement effect in a nanofluid. Experimental results at MIT found that a 0.001 vol% alumina nanofluid enhances the pool-boiling and flow-boiling CHFs by 50 and 30%, respectively, compared to the pure water case.17,18 So, heuristically, the value of the multiplier was assumed to be an intermediate 1.4. The results are summarized in Fig. 7. The curve that shows the flow rate as a function of power has a peak, which is due to the conflicting effects of increased density head and increased two-phase pressure loss in the gap. Figure 7 shows the minimum CHF ratio for pure water and nanofluid. It is apparent that if the margin to CHF must be retained, the maximum allowable power that can be removed from the vessel outer surface with a nanofluid is ;26.8 MW, or some 42% higher than water. In determining the maximum operating power, the stability of the system was also considered as large flow oscillations could cause premature CHF. Three types of instability were considered: ~a! flow excursion ~static!, ~b! density-wave oscillation ~dynamic!, and ~c! pressuredrop oscillations ~dynamic!. The criteria developed by Rohatgi and Duffey 34 were used to calculate the onset of flow excursions. Operation at the higher heat-removal rate attained with nanofluids was found to be stable ~with a good margin! against this type of instability ~see the 32-MW line in Fig. 7!. Using Saha et al.’s 35 criteria, it was determined that the system would be stable against density-wave instabilities at heat-removal rates up to 47 MW. Dynamic instabilities of the pressure-drop oscillation type may occur if the curve that shows the pressure drop as a function of mass flow rate displays a negative slope.36 That slope was inspected and found positive at all power levels up to the 32-MW static instability limit and beyond. Therefore, flow excursion Fig. 7. Operating range of the IVR system. @Departure from nucleate boiling ratio ~DNBR! is the same as CHF ratio.# NUCLEAR TECHNOLOGY VOL. 162 APR. 2008 89 Buongiorno et al. NANOFLUIDS FOR ENHANCED ECONOMICS AND SAFETY OF REACTORS seems to be the most limiting type of two-phase flow instability in this application. V. CONCLUSIONS AND FUTURE WORK Three nuclear reactor applications have been explored for nanofluids. The findings are as follows: 1. PWR coolant application: The use of nanofluids with at least 32% higher CHF could enable a 20% power density uprate in existing plants without changing the fuel assembly design and without reducing the margin to CHF. The nanoparticles would not alter the neutronic performance of the system significantly. Of the seven nanoparticle materials considered, silica, alumina, and carbon would result in acceptable coolant radioactivity during shutdown, while gold, platinum, and iridium would not. Zirconia is borderline. 2. ECCS application: A RELAP5 analysis of the LB-LOCA in PWRs has shown that the use of a nanofluid in the ECCS accumulators and safety injection can increase PCT margins ~in the nominal-power core! or maintain them in uprated cores if the nanofluid has a higher post-CHF heat transfer rate. 3. Severe accident application: Use of nanofluids could enable a more than 40% heat removal rate increase on the outer surface of the vessel during severe accidents with core relocation to the bottom of the vessel. This would result in higher margins for IVR in state-of-theart systems such as AP1000 or APR1400, or enable IVR for higher power density reactors. Among the three reactor applications considered, this one seems to present the fewest constraints and thus is likely to be implemented first. Although this exploratory study has shown that nanofluids are indeed promising, major uncertainties remain: 1. The heat transfer gains observed in nanofluid poolboiling and flow-boiling experiments at low pressure must be demonstrated at prototypical conditions. For example, CHF tests in bundle geometry at high pressure, temperature, and mass flux will be needed for the PWR coolant application. Also, CHF tests for nanofluids flowing on the outer surface of a hemispherical heater will be needed for the severe-accident application. 2. The chemical-physical stability of the nanoparticle suspension in PWR chemistry will have to be tested over long periods of time, including the effects of radiation. 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