NUCLEAR ENGINEERING AND DESIGN 3 (1966) 365-368. NORTH-HOLLAND PUBLISHING COMP.

, AMSTERDAM

DIFFUSION

BONDING OF ZIRCALOY-2 BY SWAGING * **

E. BRUTTO, G. PERONA, R. SESINI

TO

STEEL

Laboratorio di Tecnologie , C. I. S. E . , Segrate (Milano) , Italy

G. V O L T A
Servizio di Tecnologie, C . C . R . Euratom, Ispra (Varese), Italy

Received 27 December 1965

A metallurgice,1 bond between zircaloy and steel has been obtained by hot swaging. This method, developed at first on fiat specimens and then applied to tubular joints, gives diffusion layers having a very small thickness. Mechanical, thermal and corrosion tests on tubular joints 40 mm in diameter have given satisfactory results. The application of the process to larger joints is projected.

I. INTRODUCTION
In o r d e r to obtain sound m e t a l l u r g i c a l joints b e t w e e n z i r c a l o y and s t e e l two ways can be used: cold p r o c e s s e s ( e x p l o s i v e welding [1] and u l t r a sonic welding [2]) and p l a s t i c d e f o r m a t i o n p r o c e s s e s ( c o e x t r u s i o n [3], hot r o l l i n g [4], f r i c t i o n w e l di n g [5] and swaging). The f i r s t p r o c e s s e s p r e v e n t the f o r m a t i o n of b r i t t l e i n t e r m e t a l l i c compounds by l i m i t i n g the t e m p e r a t u r e . H o w e v e r , up to the p r e s e n t not one of t h e s e p r o c e s s e s has r e a c h e d the stage of in d u s t r i a l application. The p r o c e s s e s of the second type r e d u c e the f o r m a t i o n of b r i t t l e i n t e r m e t a l l i c compounds by s h o r t e n i n g the co n t a c t t i m e at the t e m p e r a t u r e r e q u i r e d f o r the a c h i e v e m e n t of the m e t a l l u r g i c a l bond. The m e t a l s u r f a c e s a r e s h e a r e d p a s t each o t h e r so that oxides o r o t h e r f i l m s a r e b r o k e n and u n c o n t a m i n a t e d m a t e r i a l s c o m e into contact p r o v i d i n g a g r e a t quantity of diffusion nuclei. The m a i n advantage of the swaging p r o c e s s p r e s e n t e d in this p a p e r is that it is suitable f o r application to long tubes in the finished state. The s t a n d a r d conditions ( t e m p e r a t u r e , a r e a r e duction r a t i o , s u r f a c e t r e a t m e n t , etc.) f o r bonding z i r c a l o y to s t e e l by swaging have been studied on flat s p e c i m e n s u s i n g a p n e u m a t i c h a m m e r . L a t e r they w e r e adapted f o r the f a b r i * The present work was carried out in the framework of the research program under the contract no. 180.64.5-ORGI, sponsored by Euratom. ** Accepted by W. J. McGonnagle.

cation of tubular joints, 44 m m in e x t e r n a l d i a m e t e r , 2 m m in t h i c k n e s s , on a s t a n d a r d swaging machine. 2. PROCESS FOR T U B U L A R JOINTS Two types of joints have been produced: lapped and t a p e r e d joints. The f a b r i c a t i o n of tape r e d joints b et w een z i r c a l o y - 2 and S.S. AISI 304 L is d e s c r i b e d in this section. In fig. 1 an a s s e m b l y r ead y to be swaged is shown. All the S.S. c o m p o n e n t s have been p r e v i ously d e g a s s e d in a high v a c u u m f u r n a c e at 1020oc. The s u r f a c e s to be welded a r e c h e m i cal l y p i ck l ed p r i o r to a s s e m b l y : s t e e l by m e a n s of an e l e c t r o l y t i c a l bath with p h o s p h o r i c acid and g l y c e r o l ; z i r c a l o y by m e a n s of a c h e m i c a l p i c k ling with diluted n i t r i c and f l u o r i d r i c acids. At the end of this o p e r a t i o n , a l u m i n u m n i t r a t e is then u s e d as a stop solution. B e f o r e i n t r o d u c i n g the a s s e m b l y into the swaging m a c h i n e it is heated up to 960oc by an induction coil. The jacket is e v a c u a t e d and then filled with p u r e argon. The cold m a n d r e l of bond s t e e l is i n s e r t e d when the swaging o p e r a t i o n s t a r t s . The swaging t i m e m u s t be l e s s than 20 sec in o r d e r to avoid the co o l i n g effect. Some joints obtained u s i n g the d e s c r i b e d method a r e shown in fig. 2. The m a i n c h a r a c t e r i s t i c s of the m a c h i n e e m p l o y e d a r e : c o n i c a l die angle: speed: power: maximum radial force: 20 1800 p u l s e s p e r minute 10 HP 40 000 kg.

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E. BRUTTO, G. I~ERONA, R. SESINI, G. VOLTA

S.S. AISI 504 L

Zhca]oy-2_

," #

/ / . z v / / I / '' / / I / ~ /

/ '' "z "*" "* " / / / "Z f "# / X f / ~ "

Fig. 1. Assembly of a zircaloy-steel sample before swaging.

Fig. 2. Zirealoy-steel tapered joints obtained with the described process. 3. M E T A L L U R G I C A L CHARACTERISTICS O F THE BONDING LAYER S e v e r a l m e t a l l o g r a p h i c e x a m i n a t i o n s have b e e n made on s p e c i m e n s a f t e r d e s t r u c t i v e t e s t s . As expected, the b e s t m e c h a n i c a l p r o p e r t i e s a r e obtained with a v e r y thin and u n i f o r m diffusion layer. The o p t i m u m t h i c k n e s s is 2 to 4 ~. In a longitudinal s e c t i o n of a typical joint the t h i c k n e s s of the l a y e r f r o m one end to the o t h e r c ha ng es l e s s than 20%. The l o c a l fluctuations a r e in the l i m i t s of + 12%. The m e t a l l o g r a p h i c s t r u c t u r e of the z i r c a l o y in the welded zone is of Widmanst~tten type. Cold wo rk i n g followed by annealing at 750oc can r e s t o r e the n o r m a l s t r u c t u r e . In o r d e r to i n v e s t i g a t e the influence of the p l a s t i c d e f o r m a t i o n method on the s t r u c t u r e and c o m p o s i t i o n of the bonding l a y e r a c o m p a r a t i v e a n a l y s i s with an e l e c t r o n m i c r o p r o b e has been made on l a y e r s obtained by swaging and by static hot p r e s s i n g . Quantitative d i f f e r e n c e s have been found. In the r an g e of t h i c k n e s s of about 15 ~ the swaged bond contained c r a c k s with s e v e r a l s e g r e g a t e d g r ai n s. It does not show w e l l s e g r e g a t e d l a y e r s of fixed c o m p o s i t i o n . When the t h i c k n e s s is r e d u c e d (up to 4 ~, the s e n s i t i v i t y l i m i t of the i n s t r u m e n t being 2.5 ~) the plateau in the c o m p o s i t i o n c u r v e c o r r e s p o n d i n g to i n t e r m e t a l l i c l a y e r s tends to d i s a p p e a r .

4. TESTS ON JOINTS In o r d e r to e s t a b l i s h the e f f i c i e n c y of the d es c r i b e d p r o c e s s and the p r o p e r t i e s of the joints obtained by this, a s e r i e s of 20 joints was subm i t t e d to d e s t r u c t i v e t e s t s . No s a m p l e r e v e a l e d

DIFFUSION BONDING OF Z I R C A L O Y - 2 TO S T E E L BY SWAGING

367

Table 1
Test Results Observations

Stud

tit
k\\'~.\\N

~5

15 -: 35 kg/mm 2

Dispersion indicating brittle bonding

Bend

Internal zircaloy: no detachment up to 180o External zircaloy: rupture of zircaloy before detachment

Shear
7"#'/" / ~// //

12 -.- 14 kg/m 2

Burst Thermal cycling Corrosion

20oc 400oc-100oc 400oc steam 400oc terphenyl

Bulge in zircaloy-2 at 410 kg/cm 2 500 cycles without deterioration No preferential corrosion No preferential hydrogen pick-up
No mechanical test after cycling

d e f e c t s which might have effected the u s e of the material. A b r i e f d e s c r i p t i o n of the t e s t s c a r r i e d out is given in the following p a r a g r a p h s . R e s u l t s a r e shown in table 1. 4.1. Mechanical tests A d e t a c h m e n t t e s t by t e n s i l e s t r e s s was s e t up, which c o r r e s p o n d s to the "stud t e s t " g e n e r ally u s e d in o r d e r to check plating adhesion. A s m a l l disk is r e m o v e d f r o m the m e t a l l i c joint; the welding s u r f a c e :is n o r m a l to the axis of the disk itself. A s p e c i m e n as shown in table 1 is r e m o v e d f r o m the disk. The v a l u e s thus obtained a r e on the a v e r a g e 20% l o w e r than t h o s e which would be obtained with s t a n d a r d t e n s i l e s p e c i mens. Another c o n t r o l p e r f o r m e d on s e v e r a l s a m p l e s is the bend test; though it does not p r o v i d e n u m e r i c a l v a l u e s , it g i v e s an indication of the w e l di n g a c c e p t a b i l i t y in the s i m p l e s t way. It cons i s t s in bending a s t r i p (longitudinal s e c t i o n f r o m the joint) around a b a r having a p r e - e s t a b l i s h e d d i a m e t e r . The welding is c o n s i d e r e d good when the s t r i p bends at a definite angle without detachment. A n o t h er s i g n i f i c a n t t e s t was that of s h e a r r e s i s t a n c e . The s t r e s s obtained with this t e s t i s s i m i l a r to the w o r k i n g s t r e s s . A r i n g is d e r i v e d f r o m the c y l i n d r i c a l joint w h e r e s t e e l p r o t r u d e s on one side and z i r c a l o y on the other. The r i n g

is p l a c e d u n d e r a p r e s s acting ax i al l y up to d e tachment. Some joints w e r e s u b m i t t e d to " b u r s t t e s t " by i n t e r n a l p r e s s u r e without axial s t r e s s , as el o n gation is p r e v e n t e d . In all s a m p l e s p r e s s u r e was b r o u g h t to 410 k g / c m 2 , c o r r e s p o n d i n g in the m a t e r i a l to a s t r e s s of 47 k g / m m 2. Only in one c a s e bulging was o b s e r v e d on welding without s e p a r a t i o n , in all the o t h e r s it o c c u r r e d only in the z i r c a l o y tube. 4.2. T h e r m a l t e s t s F o u r joints w e r e t h e r m a l c y c l e d in a i r for 500 t i m e s (each c y c l e l a s t i n g 1 hr) b e t w e e n 100 and 400oc. Subsequently it was d e t e r m i n e d that the welding was not d a m a g e d by m e a n s of h e l i u m leak t e s t s . In o r d e r to a s c e r t a i n the st ab i l i t y f o r i n t e r m e t a l l i c diffusion, s a m p l e s obtained f r o m joints w e r e kept f o r 100 h r at 600oc. T h i s is a much h i g h e r t e m p e r a t u r e than that c o n s i d e r e d as w o r k i n g conditions. The diffusion l a y e r t h i c k n e s s r e m a i n e d unchanged. 4.3. Corrosion t est s C o r r o s i o n t e s t s c a r r i e d out in s t e a m at 400oc and 100 k g / c m 2 r e v e a l e d n e i t h e r a c c e l e r a t e d c o r r o s i o n in the welding zone nor an indication of l o c a l i z e d c o r r o s i o n s . T e s t s at 400oc in t e r p h e n y l did not r e v e a l a h y d r o g e n p r e f e r e n t i a l a b s o r p t i o n in the diffusion

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E. BRUTTO, G. PERONA, R. SESINI, G. VOLTA REFERENCES [1] V. Philipchuck, Explosive welding, ASD-TR-61-24 (August, 1961). [2] E. Gebhardt et C., Reaktorwerkstoffe (Teubner V e r lag, 1964). [3] W. B. Tuffin, A.R. Gilman and S. Isserow, Tubular s t a i n l e s s steel - zircaloy t r a n s i t i o n joints p r e p a r e d by tandem extrusion, NMI 7216. [4l H. W. Boessenkool, G. Durst and S. Siegel, Proc6d6 perfectionn~ de liaison de m~taux en phase solide, B.F. No. 1.176.904 (1952). [5] S. Paprocki and S. P o r e m b k a , Joining z i r c a l o y s t a i n l e s s steel and SAP alloys by friction rolling and explosive techniques, BMI-1594.

l a y e r a f t e r a s o a k i n g i n a u t o c l a v e of 400 h r . After corrosion bend tests provided results perfectly comparable with those previoulsy performed. 5. C O N C L U S I O N S The process, in the development stage has given promising results, and an application on i n d u s t r i a l s c a l e i n t h e f r a m e of t h e d e v e l o p m e n t of a n O R G E L t y p e r e a c t o r i s f o r e s e e n in t h e near future. ACKNOWLEDGEMENTS A u t h o r s a r e g r e a t l y i n d e b t e d to t h e i r c o - o p e r a t o r s f o r t h e e f f i c i e n t c o n t r i b u t i o n s u p p l i e d to the research development.