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H. Muscher, P. Kaleychev, J. Stuckert
5th International ASTEC User Club meeting, Aix, 29. Jan. - 1st Feb. 2013
Institute for Applied Materials Materials Process Technology, Programme NUKLEAR
KIT University of the State of Baden-Wuerttemberg and National Research Center of the Helmholtz Association
www.kit.edu
QUENCH-00 Oct. 9 - 16, 97 QUENCH-01 February 26, 98 QUENCH-02 July 7, 98 QUENCH-03 January 20, 99 QUENCH-04 June 30, 99 QUENCH-05 March 29, 2000 QUENCH-06 Dec. 13 2000 QUENCH-07 July 25, 2001 QUENCH-09 July 3, 2002 QUENCH-08 July 24, 2003 QUENCH-10 July 21, 2004 QUENCH-11 Dec 08, 2005 QUENCH-12 Sept 27, 2006 QUENCH-13 Nov. 7, 2007 QUENCH-14 July 2, 2008 QUENCH-15 May 27, 2009 2 29.01.2013
Water 80 g/s Water 52 g/s Water 47 g/s Water 40 g/s Steam 50 g/s Steam 48 g/s Water 42 g/s Steam 15 g/s Steam 49 g/s Steam 15 g/s Water 50 g/s Water 18 g/s Water 48 g/s Water 52 g/s Water 41 g/s Water 48 g/s
1800 K 1830 K 2400 K 2350 K 2160 K 2020 K 2060 K 2100 K 2100 K 2090 K 2200 K 2040 K 2100 K 1820 K 2100 K 2100 K 170 m 145 m 160 m, breakaway 274 m 514 m 613 m (at 850 mm) 170 m 300 m, breakaway 400 m 470 m 320 m 82 m 160 m 207 m 230 m 300 m 312 m
completely oxidized 500 m at 913 mm completely oxidized completely oxidized 280 m 420 m 670 m completely oxidized completely oxidized completely oxidized completely oxidized completely oxidized completely oxidized 750 m 840 m 630 m
Heinrich Muscher 36 / 3 20 / 140 18 / 120 10 / 2 25 / 2 32 / 4 66 / 120 60 / 400 46 / 38 48 / 5 9 / 132 34 / 24 42 / 1 34 / 6 41 / 7
commissioning test pre-oxidized cladding COBE: no additional preoxidation no additional pre-oxidation slightly pre-oxidized cladding pre-oxidized cladding OECD-ISP 45 COLOSS: B4C COLOSS: B4C, steam starvation, very high T reference to QUENCH-07 (without B4C) LACOMERA: air ingress LACOMERA: boil-off ISTC: VVER SARNET: Ag/In/Cd (aerosol) M5 cladding ZIRLO cladding
KIT IAM
Introduction/ Motivation/ Outline ASTEC 2.0 rev.1 modelling / CORA-13 + simulations of the quench exp. (level controlled by auxiliary feed water injection, afw) Validation against Q-experiments : -code to data ASTEC-ICARE-part: phenomena occurring during degradation: clad ox., rods heat up melting today (29.1.13!) a new Q-experiment is conducted at IAM/KIT (Q-debris) .. QUENCH (Q-) experiments ) still provide new data for development of models: Useful appl. of ASTEC on Q-problems such as comparing Zry-4, M5, E110 BCs, nominal s-s, (input) degradation parameters: given by PSI TG/BE+ KIT objectives/ scope of sim-s clearly outlined: radial& axial bundle profiles according to specifications (geometry of the Q-facility etc..) Chronology of main exp. events- given in quick look tables (KIT-reports)
29.01.2013
Heinrich Muscher
KIT IAM
1st steps in Q- modelling using ASTEC v.2.1/ some progress achieved contract on ASTEC usage signed 28.10.2010 (GRS) "Overview of the integral code ASTEC v2.0- ref. "Evolution of ASTEC v2.0-r1 with respect to the v2.0 (update) ASTEC principles and general modeling features, IRSN 2011 focus on the ICARE part within ASTEC Training Course material detailed ICARE user's manual; guidelines; MARCUS (web) Understanding of "quench05.dat ID: courtesy Patrick Chatelard, IRSN Q-facility real design (position of TCs, etc.) Towards a best-estimate ASTEC-ICARE ID for Q tests: Q-10, Q-13, Q-16 (SARNET-BE) : work is underway: Q-10/-13/-16 to be further simulated Participation at GRS-IRSN and OECD TG-meetings KIT ASTEC1.3 work done already 2006 by others (ID s: nodalization schemes, data fields) KIT/IAM experience with calc. on the Zry-4 cladding /steam interactions using SVECHA code: QWS 16/H2 uptake in the KIT-LORA furnace Important activities followed: our KIT internal report published on Q-14; papers Q-05 /-06 /-11 / exp. were simulated with ASTEC V2.0 rev.1, too (post- test analysis)
29.01.2013
Heinrich Muscher
KIT IAM
ASTEC activities concerning simulation of Q-tests at KIT The aim is to present here results of modeling Q- 5, -6, -11, -14, using ASTEC (Q-10,-16,-13 will follow later); testing the applicability of ASTEC for simulation of Q- exp.-s both the H2-source term (uncovered core..) and the HT-transient behavior of structure mat Q-debris pre- test calc.-s done by others (using different code tools, other experience..) Appl. of ASTEC to Q-exp.-s, ASTEC code validation: Water quench: Q-06 (ISP-45) Q-11 (Q-L2); Q-14 - done ; air ingress Q-10/ Q-16 follow Assessment of core degradation/ delayed core reflood Preparation of Q-10/ Q-16 IDs /SARNET BE: KIT being the only one ASTEC participant Preliminary work done so far KIT ASTEC 1.3 IDs rewritten, updated, for the purposes of ASTEC 2.0 rev2p2 (done for Q-06/Q-11/Q-14): New ID-work is in progress for Q-10; Q-16
Revision according to BE specifications MESHING: 6 radial fuel rings; 20 axial meshes /Inconel grids added
29.01.2013
Heinrich Muscher
KIT IAM
Q-test section/ ASTEC modeling axial meshes, representative simulated fuel rods standard and improved Ar/O2 ox kinetics
6 29.01.2013 5th Int. ASTEC Users` Club Meeting
KIT IAM
KIT_ASTEC
Cathcart-Pawel (low temp. range) Prater-Courtright (high temp. range)
T > 2300 K and < 0.3 mm; T > 2500 K and > 0.3 mm
For (10731673)K, the M5 ox. kinetics (KIT-SET results) was taken; for (1674-2050K) existing data for Zry-4 were used instead of -missing- M5 values Power of two circuits of FRS were adopted according to the exp. The exp. data for temp-s were changed as they were presented in ASTEC for exp. data for 3 types of rods one central, one from the internal & one from the outer group, respectively The exp. data points for H2 prod. were incorporated graphs added into the new Q-14 ID: H2 prod. rate [kg/s]; cladding layer thickness vs. & vs. elevation; sim.-s exhibited lower ox. rates of M5 for T<1650K & lower H2 gen. in phases before q-ing compared to Zry-4.
Visu8 29.01.2013
KIT IAM
Q-05
as an album
-runs at KIT-
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Heinrich Muscher
Q-06
with ASTECv2.0r1 -runs at KIT-
10
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Heinrich Muscher
ID v.1.3: W. Hering
KIT IAM
Q-11
ID: LEE ASTECv2r1
C1/2: rods degradation clear visible! -runs at KIT-
11
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Heinrich Muscher
Q-14
with ASTECv2r1 -runs at KITID: P. Kaleychev, S. Bertusi et.al.
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Heinrich Muscher
KIT IAM
1) CR (U); heated rods: inner, outer rings H1/H2; CRs (C1/C2); SH; insulation. In the end of the calc. (7600s) the highest temp. are over the insulation and the CJ the height ca. 750 mm 2) At the the height of the max. calc. ox. thickness which was at 950mm, evolution of clad layer thickness was obtained. At 7600s the fraction of [ZrO] becomes the largest one. On the 2nd place the fraction of ZrO2 and at the 3rd-the Zr contribution. In the case of inner ring rod (IRR/H1) ox. the visu showed, that the according thicknesses ([ZrO] & ZrO2) are larger than in the cases of the CR (U)-rod & outer ring rod (ORR/H2): see: yellow fig.-s, transparency 13 No.12 29.01.2013 -ASTEC viewgraph+discussion: P. KaleychevKaleychev- KIT IAM
1) Calc. extrema: (peak) clad temp.-s Tpct (Fig. A) are close to the exp. data at hottest elevation 950mm but the max. calc. value just before q-ing was ca. 2000K in comparison to 2150K in the exp. The difference to be explained with the ox. correlation for Zry-4/ not M5 used for the HT-region. 2) The calculated integral H2 prod. by ASTECv2.0R2p2 is about 32g (40g in the exp). The ASTEC results are close to exp. ones in the phases before quench. At (1674-2050)K existed data for Zry-4 were used the obtained results for H2 prod at quench are underestimated.
14 29.01.2013 KIT IAM
unheated central fuel rod (TCRC13), one heated rod from the inner ring of 8 rods (TFS4/9) one heated rod from the outer ring of 12 rods (TSH5/0). the maximum of ca. 1900K ( at TCRC13), was found just before quench. Corresponding temp. of TFS4/9 being ca. 1500K and of rod TSH5/0 - 900K. An acceptable difference vs. exp. data of about 100K for all of the rods. At the beginning of Q-phase temp.-s of the rods start to decrease due to rapid changes in the water level. .
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Axial Zr-profiles exhibiting a pronounced thinning of the metallic phase (2nd raw)
Axial temp. profiles from the beginning of the calc. to the Q-phase similar for all rods & the SH- being higher in comparison to the temp. of the CJ. The highest T-values at ca. 950 mm
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Zr ox. by steam/ a lit. overview (ZrN )/ CODEX-AIT- simulations done at IRSN Zr Nitride formation: correlation of Hollands/ (~MATPRO) often used different reaction rates paths with/ without pre-ox. (PO) possible cases without PO or with PO both can lead to wrong behavior (too high rates for lower temp-s; too low rates for higher temp-) Limitation of the calc. reaction rates to max. 2.010-4 (T>1800 K) Eact of ZrN formation: up till now modeled only for cases, where pO2/p < 1.010-2; full rate could be calc. if only pO2/p < 1.010-3
The - dependence of the O2 consumption: calc. in agreement with exp. data using Steinbrck correlation with a shift; O2 starvation reaches lower bundle elevations ( 350 mm), too; AIT (Core Degradation Exp. / Air Ingress Test) - case study: The - dependence of the N2 consumption can be calc. in agreement with exp. data with the correlation derived from SETs, T. Ziegler, KIT; the rate without PO was used calc. with leak simulation was consistent with the measured liq. levels (Q-fronts) CODEX-AIT bundle was cooled down to Tmin within 670s after start of Q-fronts (11350 12020s) Max. oxide layer of ~ 200m after pre-ox (7000 s) for rods at 850 / 950 mm Max. oxide layer of 670 m at end of simulation at 750 mm Max. ZrN layer of 200 m at end of simulation (15000 s) at 650 / 750 mm
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Gilles
Nitride phases: ZrN, Zr3N4 Oxonitride phases (stoichiometry between ZrO2 and ZrN4/3 i.e. ZrO2-2xN4x/3) :Zr7O11N2: 21% mol ZrN4/3 i.e. x= 3/14 :Zr7O8N4: 43% mol ZrN4/3 i.e. x= 3/7 : Zr2ON2: 75% mol ZrN4/3 i.e. x=3/4 Phase ZrO2 ZrN ZrON rG [kJ/mol] at 2300K -675 [THERMODATA] -151 [THERMODATA] 1071 [Gutzov]
-M. Steinbrck, Tina Ziegler
In case of simultaneous ox. & nitriding of Zr [Powers] : ZrO2 being most stable; if nitriding takes place, the product will react with O2 Nitride will be detected only if the ox. rate becomes very slow compared to the nitride rate But lack of data above kinetics of O2 reaction with Zr- nitride products Me creep area exposed to air/ further propagation to the whole sample spatial non uniformity of the ox process local init. of the breakaway transition;
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KIT IAM
Nitridation of ZrO2 (SET at KIT) ZrO2 can be nitrided directly at T > 1400 C in N2 [M. Lerch et al.]
ZrO2 +
2x N 2 ZrO2 2 x N 4 x / 3 + xO2 3
KO=128 m/s Zr alloys ox
Contrary to this ZrON-case above, detailed Zry-ox kinetic data are available mechanisms are well understood/incorporated in ASTEC Zry-ox. : correlations such as Cox,1976, Schanz/Leistikow1981: c either based on the assumption that the transition is linked with transformation of t- to m- ZrO2 or Arrhenius-kinetics: C air ox model in ASTEC Ttr/ t-m = 1150 towards validation of the Q air ingress exp.-s N2/O2
Conclusions/1 ASTEC have the potential to simulate Q- exp.-s (via aft-injection) giving good results for Q-5,Q-6,Q-11,Q-14. Reference IDs being adopted.. sim. evidence was given for ex. in our reports to Zry-4/ E110/ M5 mat. comparison/ Q-14(!!) Q-5/ Q-6/ Q-11 and especially Q-14 ASTEC outputs (such as Tpct, H2 prod., FRS -behavior of CR(U), IRR(H1,H2); ORR(C1,C2); SH; CJ; insulation, axial oxide thicknesses are satisfactory results (transients, distributions) are dependent on the imposed BC/IC in the right manner: ASTEC: description of our facility (nodes) & Q-tests conduct as specified scenarios done (IDs), Captured Q-10,-16 trends/profiles must also have been consistent with the (intuitive) expectation, as it was the case of all Q-14 - dependences visualized. ASTEC should have the same potential to simulate special Q- air ingress exp.-s, as well, but HT thermodyn. data like Hf (T) of ZrN etc. still not known; nitradation as such- a kin. problem ! the incorporation of N2-modeling will (would) be a special ASTEC v2.x strength ASTEC in SARNET2 (WP5): nitradation: ASTEC modeling is not at the current State of the Art compared to the Zr-ox. modeling status Developing new skills / further insight into the philosophy behind ASTEC + its source code Q-10/Q-16 exp.-s addressed air ingress into an overheated core following earlier PO in steam:
Q-10 performed with extensive PO, moderate-high air flow rate and high temp-s at onset of flooding (max Tpct = 2200K), while Q-16 was performed with limited PO, low air flow rate and relative low temp-s at flooding init. (max. Tpct = 1870K). The expected ASTEC results in near future should exhibit these differences
20 29.01.2013 5th Int. ASTEC Users` Club Meeting Heinrich Muscher KIT IAM
Conclusions/2 lessons learned from the SETs/ Q- AIT exp. and simulations
Clad Zry-4 [600-1000 C] ox kinetics can not be described only by parabolic law, as in in pre-breakaway regime- because of breakaway-transition to fast kinetics Above 800 C, this transition is associated with nitriding. The ZrN formation begins because of a high xN2 following O2 starvation Once nitriding has begun, a porous ZrO2 grows under the influence of a self-sustained ZrN + O2 ZrO2 + 1/2N2 sequence (N2 trapped in the cladding) leading to fast degradation Breakaway transition: correlation: critical weight gain = f(T). Hyperbolic law. Assumption: linkage with a t- to m- ZrO2 transformation. Post-breakaway: to be modeled by an accelerated law, scaling rate increasing linearly difficulties linked to the pre-ox phase/ limits of the models reached in Olivia`s C. AIT simulations, modeling of the pre-breakaway by a sub-parabolic law error in clad temp prediction Kp coeff. is strongly temp dependent at low temp: modeling of the post-breakaway by an accelerated law whereas a lin kinetics observed at 850C Underestimation of the Ka coeff. (Arrhenius). Simed scaling rate too high: 900-950 C total ox in 150-80min kinetic transition too early: determination of tbreak difficult, due to the non-uniformity= =inhomogeneneities of the ox process (under starvation) oxide layer thicker close to air inlet, where breakaway occurs at first Nitradation: preliminary lit. study done, also for ZrON - O. Coindreau`s remark: temp rises too quickly during the air ingress in the simulations: - Protective oxide layer not thick enough, - T correlations used up till now (especially those used for non PO cladding) overestimate the mass gain (and so the Hr of the chemical reaction) Not enough N2 taken from the gas phase: Criterion to switch from ox. to nitridation based on an inappropriate critical starvation coeff. Not enough H2 generated during reflood: -Specific models for reflood and shattering should be used incl. ox. after nitridation ( = the re-ox.)
Lacks in ICARE modeling identified, consulted with P. Chatelard (currently underway: ASTEC source code changes concerning nitradation to be finished 2014 as a part of ASTEC v2.1 info IRSN): suitable criterion to switch from ox to nitradation needed (probable influence of the th-hydraulics ) model for reox of ZrN for scale thicknesses at the end of the PO phase, where re- ox. is quite low
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Perspectives (future prospects) further validation of the nitridation models on Q-10/ Q-16
Acknowledgement: thank you P. Chatelard, S. Bertusi, P. Kruse, W. Hering, thank you all.
22 29.01.2013 5th Int. ASTEC Users` Club Meeting Heinrich Muscher
-Olivia Coindreau-
KIT IAM