56 INZHENERNO-FIZICHESKII ZHURNAL

THE MOLLIER DIAGRAM OF NORMAL HYDROGEN AT TEMPERATURES OF

16 TO I00 ~ K AND PRESSURES UP TO 500 kg/cm 2

S. A. Ulybin and S. P. Malyshenko

I n z h e n e r n o - F i z i c h e s k i i Z h u r n a l , Vol. 13, No. 1, pp. 9 0 - 9 7 , 1967

UDC 536.2

Experimental data on thermal properties are used to construct the used t h e i r own e x p e r i m e n t a l v a l u e s , as well as the
Mollier diagram of normal hydrogen at temperatures of 16--100~ K data of other r e s e a r c h e r s . A c o m p a r i s o n of the data
and pressures of 5-500 kg/cm2.
of [8] and [5, 6] showed that at some points t h e r e a r e
d i f f e r e n c e s which exceed the o v e r - a l l e x p e r i m e n t a l
The wide e m p l o y m e n t of n o r m a l h y d r o g e n in t e c h -
e r r o r . Our a n a l y s i s showed that the data of [5,6] at
nology has g i v e n r i s e to the need for a sufficiently ac-
s u b c r i t i c a l t e m p e r a t u r e s a g r e e b e t t e r with the r e s u l t s
c u r a t e M o l l i e r d i a g r a m of n o r m a l h y d r o g e n for the
of o t h e r r e s e a r c h e r s than the data of [8].
l o w - t e m p e r a t u r e r e g i o n of s t a t e v a r i a b l e s , e s p e c i a l l y
In view of this, in the c o n s t r u c t i o n of i n t e r p o l a t i o n
for the l i q u i d - p h a s e r e g i o n at high p r e s s u r e s . The
f o r m u l a s , we gave p r e f e r e n c e to the data of [5, 6] in
existing diagrams, constructed from experimental
the r e g i o n of state v a r i a b l e s f o r which data w e r e
l o w - t e m p e r a t u r e data a r e confined to p r e s s u r e s of the
a v a i l a b l e . At high p r e s s u r e s , w h e r e only the data of
o r d e r of 200 k g / e m 2. R e c e n t l y conducted e x p e r i m e n t a l
[8] a r e a v a i l a b l e , we obtained the i n t e r p o l a t i o n f o r -
i n v e s t i g a t i o n s of the d e n s i t y of n o r m a l h y d r o g e n in the
m u l a s by u s i n g t h e s e data.
liquid p h a s e have extended the r a n g e of i n v e s t i g a t e d
E x p e r i m e n t a l v a l u e s of the s a t u r a t e d v a p o r p r e s -
s t a t e v a r i a b l e s of liquid h y d r o g e n to 500 k g / c m 2.
s u r e s of n o r m a l h y d r o g e n w e r e obtained in [9] and
We a r e now c o n d u c t i n g work a i m e d at d e r i v i n g an
[10]. The data of [10] c o v e r the t e m p e r a t u r e r a n g e
equation of state of h y d r o g e n which will e n a b l e the
f r o m 13.95-24.59 ~ K and c o r r e s p o n d to the f o r m u l a
c a l c u l a t i o n of all the t h e r m o d y n a m i c p r o p e r t i e s of H 2
over a wide r a n g e of t e m p e r a t u r e and p r e s s u r e . l gp (at) = --44.368/T + 4.5331 +
Since this w o r k r e q u i r e s a g r e a t deal of t i m e it i s
worthwhile c a l c u l a t i n g a p r o v i s i o n a l M o l l i e r d i a g r a m + 0.03240 T--0,0004189 T2+0.00000484 T3. (1)
of h y d r o g e n by a s i m p l i f i e d method in the t e m p e r a t u r e
The data of [9] w e r e obtained at t e m p e r a t u r e s of
r a n g e 1 6 - 1 0 0 ~ K at p r e s s u r e s up to 500 k g / c m 2, which
2 0 . 9 0 - 3 3 . 2 4 4 ~ K and a r e i n t e r p o l a t e d b y the equation
i s the m o s t i m p o r t a n t r e g i o n for technological appli-
c a t i o n s . This p a p e r d e s c r i b e s the p r o c e d u r e and the
1gp (at) = 3.068281--55.25642 / T - -
r e s u l t s of this c a l c u l a t i o n .
F o r the i n d i c a t e d r a n g e of t e m p e r a t u r e and p r e s - --3.1282 9 10-2 T+6.6989 - 10-4 T2. (2)
s u r e the a m o u n t of e x p e r i m e n t a l data on the c a l o r i c
The two equations a r e quite s a t i s f a c t o r y as r e g a r d s
p r o p e r t i e s of n o r m a l h y d r o g e n is e x t r e m e l y s m a l l ,
a c c u r a c y and a g r e e well with one a n o t h e r at t e m p e r -
c o v e r s a n a r r o w r a n g e of s t a t e v a r i a b l e s , and is v e r y
i n a c c u r a t e in c o m p a r i s o n with t h e r m a l data. Hence, a t u r e s c l o s e to the n o r m a l b o i l i n g p o i n t of hydrogen.
Hence, Eq. (1) was u s e d to c a l c u l a t e the s a t u r a t e d
the c a l c u l a t i o n of the M o l l i e r d i a g r a m i n this work was
v a p o r p r e s s u r e f r o m the t r i p l e p o i n t to the n o r m a l
b a s e d on the u s e of t h e r m a l data.
b o i l i n g point and Eq. (2) was u s e d f r o m the n o r m a l
E x p e r i m e n t a l v a l u e s of the specific v o l u m e s of
b o i l i n g p o i n t to the c r i t i c a l point.
n o r m a l h y d r o g e n at t e m p e r a t u r e s below 100 ~ K a r e
Values for the d e n s i t y of n o r m a l h y d r o g e n on the
g i v e n i n m a n y w o r k s . An a n a l y s i s showed that the data
s a t u r a t i o n l i n e and given in [10,11]. They a g r e e well
of [ 1 - 4 ] a r e not s u f f i c i e n t l y a c c u r a t e and they w e r e
with one a n o t h e r and c o v e r the t e m p e r a t u r e r a n g e
not u s e d i n the c a l c u l a t i o n s . Of the o t h e r w o r k s , only
f r o m the t r i p l e point to the c r i t i c a l point. To i n t e r -
two [5,6] r e l a t e to the liquid phase. In addition, J o h n -
polate the e x p e r i m e n t a l data we u s e d the equation [11]
ston and White [7] give smoothed e x p e r i m e n t a l pvT
v a l u e s for t e m p e r a t u r e s above 35 ~ K and p r e s s u r e s up
to 200 k g / c m 2. (Tr176 (3)
P--Pc
In the S c i e n t i f i c R e s e a r c h I n s t i t u t e of High T e m p e r a -
t u r e s , D. L. T i m r o t and V. E. L y u s t e r n i k m a d e m e a - where
s u r e m e n t s of the c o m p r e s s i b i l i t y of H~ on the i s o t h e r m s A=0.145985; B=4.47314.10-%
- 1 9 5 . 2 ~ C and - 1 9 5 . 5 5 ~ C up to p r e s s u r e s of 200 k g / e m 2
to v e r i f y J o h n s t o n a n d W h i t e ' s smoothed data [7]. T h e i r The c r i t i c a l c o n s t a n t s of n o r m a l h y d r o g e n w e r e
r e s u l t s a g r e e d within the l i m i t s of e x p e r i m e n t a l e r r o r . t a k e n as: T c = 33.25 ~ K, Pc = 12.568 kg/cm2; Pc - P0 =
T h u s , the data of [7] can be r e g a r d e d as quite r e l i a b l e and = 0.03067 g / c m 3.
we used them i n the c a l c u l a t i o n s . The l i t e r a t u r e at p r e s e n t does not c o n t a i n an e q u a -
P a p e r [8] gives smoothed pvT data for n o r m a l h y - tion of s t a t e which c a n s e r v e as a b a s i s f o r the a n a -
d r o g e n at p r e s s u r e s up to 500 k g / c m z and low t e m - l y t i c a l t r e a t m e n t of e x p e r i m e n t a l pvT data for n o r m a l
p e r a t u r e s . To obtain the smoothed data the a u t h o r s h y d r o g e n in the e n t i r e i n d i c a t e d r a n g e s of t e m p e r a -
JOURNAL OF ENGINEERING PHYSICS
t u r e and p r e s s u r e . The d e r i v a t i o n of an equation of
s t a t e p r e s e n t s s o m e difficulty and did not c o m e within
the s c o p e of the p r e s e n t i n v e s t i g a t i o n . H o w e v e r , we
r e j e c t e d a p u r e l y g r a p h i c a l m e t h o d of c o n s t r u c t i n g
the M o l l i e r d i a g r a m s i n c e this m i g h t r e d u c e its a c -
c u r a c y to s o m e extent, and we u s e d m a i n l y a n a l y t i c a l
m e t h o d s . To s i m p l i f y the a n a l y t i c a l t r e a t m e n t of the
e x p e r i m e n t a l d a t a we d i v i d e d the e n t i r e r a n g e of s t a t e
v a r i a b l e s into t h r e e r e g i o n s : the f i r s t i n c l u d e s s t a t e s
of the g a s with a s u b c r i t i c a l d e n s i t y at all t e m p e r a -
t u r e s ; the s e c o n d i n c l u d e s t e m p e r a t u r e s and d e n s i t i e s
above the c r i t i c a l ; the t h i r d i n c l u d e s t e m p e r a t u r e s
b e l o w Tc and d e n s i t i e s g r e a t e r than Pc-
In the f i r s t r e g i o n , i . e . , p <- Ps, we u s e d the e q u a -
tion of [12] for the s p e c i f i c v o l u m e s . It is one of the
m o s t a c c u r a t e e q u a t i o n s , v a l i d for a wide r a n g e of
t e m p e r a t u r e and p r e s s u r e , and s u i t a b l e for c a l c u l a -
t i o n s of c a l o r i c p r o p e r t i e s .
In t h i s w o r k we m a d e an a d d i t i o n a l c o m p a r i s o n of
the equation of [12] with the e x p e r i m e n t a l d a t a in the
l o w - t e m p e r a t u r e r e g i o n of v a r i a b l e s and c o n f i r m e d
the high a c c u r a c y of this equation.
At s u p e r c r i t i c a l d e n s i t i e s and t e m p e r a t u r e s below
100 ~ K the p u b l i s h e d equations of s t a t e for n o r m a l h y -
d r o g e n a r e b a s e d on the a s s u m p t i o n of l i n e a r i t y of the
i s o c h o r s and u s u a l l y have the f o r m
p(v, T) = A(v) + B(v)T. (4)
An e x a m p l e of such a r e l a t i o n s h i p is the equation of
[5], p r o p o s e d f o r s p e c i f i c v o l u m e s of 1 3 - 1 9 c m 3 / g at
p r e s s u r e s up to 110 k g / c m 2. T h i s e q u a t i o n w a s c o m -
p a r e d with the e x p e r i m e n t a l d a t a for the liquid s t a t e in
w i d e r r a n g e s of s p e c i f i c v o l u m e and p r e s s u r e . The
d i s c r e p a n c i e s w e r e found to i n c r e a s e s h a r p l y even
when the v a l u e s of the s t a t e v a r i a b l e s w e r e only a
l i t t l e o u t s i d e the r a n g e r e c o m m e n d e d in [5]. Within
the r e c o m m e n d e d r a n g e the equation on the a v e r a g e
w a s s a t i s f a c t o r i l y a c c u r a t e as r e g a r d s t h e r m a l p r o -
p e r t i e s , but d i d not p r e d i c t the a c t u a l b e h a v i o r of the
i s o c h o r s of n o r m a l h y d r o g e n , which have a v e r y p r o -
\ i
~'}
p(Yz,
F i g . 1. D i a g r a m i l l u s t r a t i n g i n t e r p o l a t i o n of e x p e r i m e n t a l
p v T d a t a f o r T -< T c (a) and T --> T c (b).
57
nounced c u r v a t u r e . H e n c e , equations of s t a t e b a s e d on
the a s s u m p t i o n of l i n e a r i t y of the i s o c h o r s a r e not
s a t i s f a c t o r y for the p r e d i c t i o n of the p r o p e r t i e s of
n o r m a l h y d r o g e n in a wide p r e s s u r e r a n g e .
The i n t e r p o l a t i o n f o r m u l a which we u s e d f o r s u b -
c r i t i c a l t e m p e r a t u r e s h a s the f o r m
p(v, T) = p(Tc, v)+pITe, v'(T)] + p s ( T ) +3p(v, T). (5)
The m e a n i n g of the t e r m s c o n t a i n e d in this equation is
i l l u s t r a t e d in F i g . l a .
F o r s u p e r c r i t i c a l t e m p e r a t u r e s and p - Pc the i n -
t e r p o l a t i o n f o r m u l a h a s the f o r m
p(v, T)=p(vc, T)+p(Tr v)--pc+Sp(v, T). (6)
The m e a n i n g of the t e r m s contained in the equation is
i l l u s t r a t e d in F i g . l b . The p r e s s u r e on the c r i t i c a l
i s o c h o r P(Vc; T) was c a l c u l a t e d f r o m the equation of
[12]. We obtained a n a l y t i c a l r e l a t i o n s h i p s f o r all the
t e r m s c o n t a i n e d in E q s . (5) and (6).
F o r m u l a s (5) and (6) a g r e e w e l l with one a n o t h e r on
the c r i t i c a l i s o t h e r m and with the equation obtained in
[12] on the c r i t i c a l i s o c h o r ( f r o m the f i r s t d e r i v a t i v e
of the t h e r m a l q u a n t i t i e s ) . A c o m p a r i s o n of the e x -
p e r i m e n t a l and c a l c u l a t e d p r e s s u r e s i s shown in F i g s .
2 and 3.
The a b s o l u t e d i f f e r e n c e s b e t w e e n the c a l c u l a t e d and
e x p e r i m e n t a l p r e s s u r e s at s o m e p o i n t s a r e e x t r e m e l y
high. It should be b o r n e in mind, h o w e v e r , that in the
l i q u i d - p h a s e r e g i o n the d e r i v a t i v e (~p/3v) T is l a r g e
and, h e n c e , an a p p r e c i a b l e d i f f e r e n c e in p r e s s u r e h a s
h a r d l y any e f f e c t on the s p e c i f i c v o l u m e . In addition,
the d i f f e r e n c e s b e t w e e n the c a l c u l a t e d v a l u e s and the
d a t a of [5] and [6] a r e of o p p o s i t e s i g n s in m o s t c a s e s .
The s t r u c t u r e of the i n t e r p o l a t i o n f o r m u l a s (5) and
(6) is such that the m a i n c u r v a t u r e of the i s o t h e r m s in
the p v - d i a g r a m is due to the t e r m p ( T c , v ) . The t e r m
5p(v, T) h a s an i n s i g n i f i c a n t c u r v a t u r e on the i s o t h e r m s .
H e n c e , h a v i n g an e x p r e s s i o n for p ( T c , v) v a l i d up to
high p r e s s u r e s , we can obtain the p r e s s u r e s at high
d e n s i t i e s by e x t r a p o l a t i o n of the t e r m 6p(v, T) to the
W Iv~ b*
58 INZHENERNO-FIZICHESKII ZHURNAL

! J .

.f ll-2
li - ,,~
e--/#

20 z/O 60 60 lO0 120 0 2O O0 60 80 I00 p

F i g . 2. C o m p a r i s o n of e x p e r i m e n t a l pvT d a t a with d a t a
c a l c u l a t e d f r o m Eq. (5) [Ap = (Pexp - Pcalc) kg/cm2]: a)
d a t a of [5] (1--20.34 ~ 2--22.96 ~ 3--25.81 ~ 4--30.11 ~ K);
b) d a t a of [6] (5--16.66 ~ 6--17.909 ~ 7--20.42 ~ K).

c o r r e s p o n d i n g d e n s i t i e s . It is unlikely that such an [15]. F o r t h i s r e a s o n we u s e d v a l u e s f o r the h e a t of

e x t r a p o l a t i o n w i l l l e a d to l a r g e e r r o r s . M o r e o v e r , a
c o n s i d e r a b l e p a r t of the e r r o r will b e s y s t e m a t i c ,
which w i l l h a v e l i t t l e effect on the e n t h a l p y and e n t r o p y
increments.
To d e t e r m i n e the enthalpy and e n t r o p y of n o r m a l
h y d r o g e n we u s e d the following t h e r m o d y n a m i c r e l a -
tionships
vo IJo
7J
s(v, T)=so(T )+ A ~ ( Op ~ dr. (7)
vo
We took the t e m p e r a t u r e d e p e n d e n c e of the e n t h a l p y
i0 and the e n t r o p y s~ in the i d e a l - g a s s t a t e f r o m [13,
14]. T h e s e d a t a a r e the m o s t r e l i a b l e at p r e s e n t .
E q u a t i o n s (7) in e a c h of the t h r e e r e g i o n s of s t a t e
v a r i a b l e s w e r e i n t e g r a t e d in a c c o r d a n c e with the c o r -
r e s p o n d i n g a n a l y t i c a l r e l a t i o n s h i p f o r the t h e r m a l
properties.
In the r e g i o n of s u b c r i t i c a l d e n s i t i e s the d e r i v a t i v e s
(Op/~T)v and (l~p/Ov)T and the i n t e g r a l s f r o m t h e m
w e r e d e t e r m i n e d by d i f f e r e n t i a t i o n and i n t e g r a t i o n of
the equation obtained in [12]. On the b a s i s of t h e s e
c a l c u l a t i o n s we found the enthalpy and e n t r o p y in the
r a n g e up to the c r i t i c a l d e n s i t y at T -> T c and up to the
c o r r e s p o n d i n g v o l u m e s of d r y s a t u r a t e d v a p o r v" at
T -< T c. We a l s o found the s p e c i f i c v o l u m e s on the
r i g h t b o u n d a r y c u r v e of v" f r o m the equation f r o m [12]
by u s i n g known v a l u e s of the s a t u r a t e d v a p o r p r e s s u r e .
The e n t h a l p y i t and the e n t r o p y s ~ on the left b o u n d -
a r y c u r v e w e r e found f r o m the c o r r e s p o n d i n g v a l u e s of
i" and s" and the h e a t of v a p o r i z a t i o n r . E x p e r i m e n t a l
v a l u e s of the h e a t of v a p o r i z a t i o n f o r n o r m a l h y d r o g e n
i r e a v a i l a b l e only f o r p r e s s u r e s below a t m o s p h e r i c
v a p o r i z a t i o n c a l c u l a t e d f r o m the C l a p e y r o n - C l a u s i u s
equation [9].
In the c a l c u l a t i o n of the enthalpy and e n t r o p y in the
s i n g l e - p h a s e r e g i o n at v < Vc the a n a l y t i c a l e x p r e s -
s i o n s obtained for ( S p / ~ T ) v and ( a p / ~ v ) T and the i n t e -
g r a l s f r o m t h e m w e r e v e r y c o m p l i c a t e d and u n s u i t a b l e
f o r c a l c u l a t i o n s . In addition, the i n t e r p o l a t i o n r e l a -
t i o n s h i p s for pvT a r e a l t e r n a t i n g s e r i e s and, h e n c e ,
the c a l c u l a t e d v a l u e s of the d e r i v a t i v e s ( a p / a T ) v and
(0p/~v)T m i g h t show s o m e undulation on the i s o c h o r s
and i s o t h e r m s . To avoid t h i s and to s i m p l i f y the c a l -
c u l a t i o n s we found the d e r i v a t i v e s by the n u m e r i c a l
m e t h o d . F o r the whole r e q u i r e d d e n s i t y r a n g e we u s e d
the i n t e r p o l a t i o n f o r m u l a s to c o m p i l e a c o m p r e h e n s i v e
t a b l e of r e f e r e n c e v a l u e s for the t h e r m a l q u a n t i t i e s .
The t a b u l a t e d d a t a w e r e d i f f e r e n t i a t e d n u m e r i c a l l y by
m e a n s of a L a g r a n g e i n t e r p o l a t i o n p o l y n o m i a l . E a c h
v a l u e of the d e r i v a t i v e s (~p/DT)v and (3p/Ov)T on the
i s o c h o r o r i s o t h e r m was c a l c u l a t e d by u s i n g four a d -
j a c e n t p o i n t s (two on e a c h side). The n u m e r i c a l v a l u e s
of the d e r i v a t i v e s found in this w a y w e r e g r a p h i c a l l y
s m o o t h e d on the i s o t h e r m s and i s o c h o r s and t h e i r net
w a s then c o n s t r u c t e d .
E q u a t i o n s (7) w e r e i n t e g r a t e d n u m e r i c a l l y f r o m the
s m o o t h e d v a l u e s of the d e r i v a t i v e s within the r a n g e of
s p e c i f i c v o l u m e s f r o m the c o r r e s p o n d i n g s p e c i f i c
v o l u m e on the left b o u n d a r y c u r v e at T < TC o r on the
c r i t i c a l i s o c h o r at T >- Tc to the r e q u i r e d s p e c i f i c
v o l u m e . We thus c o n s t r u c t e d ip, iv, sp, sv, and T s
diagrams.
In all t h e s e d i a g r a m s the e n t h a l p y and e n t r o p y w e r e
s m o o t h e d . T h i s w a s f a i r l y e a s y within the l i m i t s of
a c c u r a c y of the e x p e r i m e n t a l d a t a and c o n s t r u c t i o n of
the d i a g r a m s . The M o l l i e r d i a g r a m w a s d r a w n f r o m
the s m o o t h e d v a l u e s . On i t we p l o t t e d the i s o c h o r s ,
i s o b a r s , and i s o t h e r m s , and in the t w o - p h a s e r e g i o n ,

O.6 o --2 9 ~ 5
0.#
0.2 ", ~l'~t--7.
0 -0.: ,.i
"" lib
-O.2 -0.r
/80200 250 300 350 O~ 0 50 /00 /50 200 p

F i g . 3. C o m p a r i s o n of e x p e r i m e n t a l p v T d a t a with t h o s e c a l -
c u l a t e d f r o m Eq. (8) (Sp = [(Pexp - P c a l c ) / P c a l c ] " 100%):
a) D a t a of [17,18] ( 1 - - a t 113.6 ~ 2--103.16~ 3--98.16 ~ K); b)
d a t a of [7] (4--40 ~ 5--50 ~ 6--60 ~ 7--75 ~ K).
 9

>
9

b
g .f
350

9
h~
300
c~

250

200

/50

2~

100
7 0 ,9 /0 H [,2 3
0.3

50 L
! 2 3 ~ 5 6

Fig. 4. Mollier diagram of n o r m a l hydrogen f r o m 16 to 98 ~ K and from 5 to 500 kg/em2: 1) T =16~ 2) 20~ 3) 24~
4) 26~ 5) 28~ 6) 30~ 7) 32~ 8) 33.26~ 9) 43~ 10) 53~ 11) 73~ 12) 98~ a) p =0.5; b) 1; c) 5; d) 10; e) 20; f) 40;
g) 60; h) 100; i) 200; j) 300; k) 400; l) 500 k g / c m 2.

O1
60
the lines of constant d r y n e s s at steps of 0.1. The in-
v e r s i o n curve obtained in this d i a g r a m a g r e e s well
with the i n v e r s i o n curve in [6].
The a c c u r a c y of the p r e s e n t e d M o l l i e r d i a g r a m
(Fig. 4) depends mainly on the accuracy and amount of
initial e x p e r i m e n t a l data. Unfortunately, at low t e m -
p e r a t u r e s , and e s p e c i a l l y in the region of high p r e s -
s u r e s , the e x p e r i m e n t a l data a r e e x t r e m e l y m e a g e r
and a r e not v e r y a c c u r a t e . According to our e s t i m a t e s ,
the e r r o r of the d i a g r a m is 2.25 k c a l / k g for enthalpy
at v >- 14 cm3/g. At s m a l l e r specific volumes the e r -
r o r is g r e a t e r and attains values of about 5 k c a l / g at
the g r e a t e s t p r e s s u r e s and d e n s i t i e s . In the c a s e of
entropy the average e r r o r is about 0.05 k c a l / k g 9 deg.
NOTATION
T is the t e m p e r a t u r e , ~ p is the p r e s s u r e , k g / c m 2;
p is the density, g/cm3; v is the specific v o l u m e ,
cm3/g; i is the enthalpy, kcal/kg; s is the entropy,
k c a l / k g 9 deg; i0, s o a r e the enthalpy and entropy in
i d e a l - g a s state; r is the specific heat of vaporization.
Subscripts: c is the c r i t i c a l state; s is the saturation
state; the single p r i m e denotes the s a t u r a t e d l i q u i d -
s a t u r a t e d vapor line; the double p r i m e denotes the
g a s - s a t u r a t e d vapor line.
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IN ZHENERNO- FIZICHESKII ZHURNAL
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11 August 1966 Institute of High T e m p e r a t u r e s ,
Moscow