Transactions of the Japan Institute of Metals, Vol. 23, No. 12 (1982),pp.

780 to 787

Dissolution of Ferrous Alloys into Molten Aluminium*

By Mitsuo Niinomi**,Yoshisada Ueda*** and Masamichi Sano***

The controllingstepof dissolutionof ferrousalloysintomoltenaluminium was studied. Com-

merciallypureiron,Fe-Si,Fe-Ni,Fe-Cu, Fe-Mn and Fe-C alloyswere dippedintomoltenalumi-
nium (99.8%Al)at 973,1023 and 1073K for varioustimes.The rateof dissolution of each alloy
intomolten aluminium was examinedtheoretically from the viewpointof naturalconvectionmass
transfer.
For the dissolution
of theFe-Cr,Fe-Cu and Fe-Ni alloysat973K, theexperimental value
ofthe mass transfercoefficient iskob
nearlyequalto the theoretical
value kc.Therefore, thedissolu-
tionof thesealloysiscontrolled by the diffusion
of Fe inmolten aluminium.At 1023and 1073K,
kobdecreases withincreasing
dippingtime.Thisisdue to theincrease of theresistance
tothechemical
reactionor mass transferin the compoud layer.For the Fe-Si alloy,kobisa littlelargerthan kc.
The resistancetochemicalreaction ormass transferinthecompoud layerisnegligible. For thecom-
merciallypure iron, kob
issmallerthan kcby about 30-50%. The resistance to thechemicalreaction
or mass transferinthe compound layerisnot negligible. For theFe-Mn alloy, kobissmallerthan
kc by about 40-70%. The resistancetothechemicalreaction or mass transfer
inthealloylayerisnot
negligible.
But,furtherstudymay be necessaryforthisalloy. For theFe-C alloy, kobismuch smaller
than kc.The dissolutionof thisalloyiscontrolled by thechemicalreaction or mass transferin the
compound layer.
(Received
October
25,1982)

gated. Kosaka et al.(15)(16) studied the dissolu-

. Introduction tion of ferrous alloy into molten aluminium
mainly in a stirred bath. Little investigation
As a basicstudy on improving the resistance was carried out in an unstirred bath and on the
of ferrousalloysto the molten aluminium, Fe- effect of alloying elements in ferrous alloys. So,
Al alloylayersformed by the reactionbetween the controlling step of the dissolution of ferrous
ferrousalloys(commerciallypure iron,Fe-C, alloys into the unstirred molten aluminium was
Fe-Si, Fe-Mn, Fe-Cr, Fe-Ni and Fe-Cu studied from the viewpoint of mass transfer
alloys)and molten aluminium were examined using various ferrous alloys employed in the
and discussedin a previouspaper(1).For the previous report(1) and discussed to reduce the
purpose,moreover, itis necessaryto study on attack of ferrous alloys by molten aluminium
the dissolutionprocessof ferrousalloysinto by means of alloying elements of the base
molten aluminium in detail. Regarding the dis- metal.
solutionof solidmetal into liquidmetal, Fe
into molten Cu(2)(3),Fe intomolten Sn(4),Cu . Experimental Procedure

into molten Sn(5),Ni, Cu and Ag intomolten

Bi(6)(7),
Ni and Cu intomolten Cu-Bi and Ni- After measurements of the thickness of the

Bi(8),Fe-C alloyintomolten Fe-C(9)-(11)and alloy layer(1) (0.01m in length cut out from

othersystems(12)-(14) have so far been investi- the center of dipped samples) specimens were

polished with 800 emery paper. After weigh-

ing, these specimens were dipped for 7.2ks into
* This paper was originallypublishedin Japanese
hot solution of 1.0010-4m3 containing
in J.Japan Inst.Metals,42 (1978),549.
** School of Production Systems Engineering
, 0.04kgNaOH and 0.02kgNaNO3, and then
Toyohashi University of Technology, the adhering aluminium and alloylayerwere
Toyohashi 440, Japan. removed. Thereafter,the weight was measured
*** Department of Metallurgy
,FacultyofEngineer- again,and an averagediameterof the specimen
ing,Nagoya University,Nagoya 464, Japan.
**** Department of Iron and Steel Engineering without the adhering aluminium and alloy
,
Faculty of Engineering, Nagoya University, layerwas calculatedby the followingequation
Nagoya 464, Japan. using the densityof ferrousalloysmeasured
 Dissolution of Ferrous Alloys into Molten Aluminium 781

previously: l: density of pure liquid (kg/m3)

: viscosity coefficient (kg/ms)

(1) kc: mass transfer coefficient (m/s)
where D: diffusion coefficient (m2/s)

d: average diameter (m), L: dipping length (m), L=0.03m in this

W: weight of specimen (kg), study.

h: height of specimen (m) This correlative eq. (2) is also consistent with
and an experimental equation by Wilke et al.(18)

s: density of specimen (kg/m3). for the aniline-water system with vertical flat

The diameter d(m) in the middle of specimen plate. In the present study, values of Sc number
can be regarded as an average diameter since are 907-908 at 973K, 647-650 at 1023K and

the diameter of dipped specimen changes 499-496 at 1073K, and values of (GrmSc) are
linearly with dipping direction. 2.7109 to 3.1109 at 973K, 3.6109 to

4.1109 at 1023K and 4.9109 to 5.1109

at 1073K. Therefore, the corelative equation
. Experimental Results and Discussion
by Ravoo(17) and Wilke et al.(18) can be

applied. These equations are both concerned

1. Correlative equation of mass transfer
with vertical flat plate, but specimens in the
under natural convection
presentstudy are cylindrical.
Therefore,the
In the case of a static specimen and an effect of curvature must be considered. This
unstirred bath as in this study and when the problem was already analyzed theoretically by
specimens are dipped vertically, the natural Ravoo et al.(17), and calculated values of the

convection due to density change in the liquid mass transfer coefficient under natural convec-
caused by the diffusion of solution atoms occurs tion for vertical flat plate and cylinder were

generally in the dipping direction and increases both almost identical and were also in good
the rate of mass transfer. The correlative agreement with experimental values of the

equation of mass transfer under vertical natural mass transfer coefficient under natural convec-
convection due to the density change at room tion for vertical cylinder at room temperature.
temperature was studied theoretically on flat Therefore, assuming that the effect of curvature

plate and cylinder by Ravoo et al.(17). Accord- can be neglected in this study, the correlative

ing to their report, when Sc number is very eq. (2) for vertical flat plate by Ravoo et al.(17)

large, an average value of Sh number can be is applied to the mass transfer under natural

obtained for a flat plate in the range of dipping convection in molten aluminium at elevated
length 0-L by the following equations: temperatures.

The distribution of velocity (V) and the

Sh=0.67(GrmSc)1/4, (2)
concentration (C) near the specimen under
where natural convection are schematically shown in

Fig. 1. As shown in this figure, the natural

Grm=gL3l(ls-s)/2, (2a)
convection due to the distribution of solute
Sc=/lD, (2b) concentration in molten aluminium occurs in

and this experiment. v and c indicate the thickness

of boundary layer of velocity and concentration,

kc=D(Sh/L). (3)
respectively.

Meanings of various symbols are given as

2. Calculation of mass transfercoefficient
follows:

Sh: Sherwood number Theoretical values of the mass transfer co-

Grm: Grashof number efficientcan be calculatedfrom eqs. (2) and (3).
Sc: Schmidt number Assuming that solid and liquid have the same
g: acceleration of gravity (m/s2) specificvolume, the density of liquid is calcu-
ls: density of saturated solution (kg/m3) lated by the equations(5)(19):
782 MitsuoNiinomi,YoshisadaUeda and Masamichi Sano

t:time (s)
kob:apparentmass transfercoefficient(m/s),
A: surfacearea per unitlength(m2/m),
Cls:saturatedconcentrationof solute(kg/m3)
and
Cb: concentrationof solute(kg/m3).
Conversionof theconcentrationfrom (mass%)
to (kg/m3) isperformed by the followingequa-
tions:

Cls=%xls ls/100,

and

Cb=%x l/100,

where

%xls: saturated concentration of eolute (mass%)

and

Fig. 1 Velocity and concentration boundary layers ls: density of liquid saturated with solute
in natural convection on a vertical flat plate. (C:
(kg/m3).
concentration, Cls: Fe saturated concentration, Cb:
The saturated concentration of solute %xls
Fe bulk concentration, c: concentration boundary
(mass%) is obtained from the concentration of
layer, v: velocity boundary layer, V: velocity,
L: dipping direction). liquidus curve at each temperature in the

phase diagram(20).
As shown in Fig. 2, denoting the distance
1/l=%x/100s+(1-%x/100)/lp, (4)
from the center of specimen to the surface of

and alloy layer by r2 (m) and that from the center

to alloy layer by r (m), W and A in eq. (5) are

%={%x0m0/100+Ls(r0-r2)}
expressed as follows:
/{m0+Ls(r20-r2)}100,

where

%x: concentration of solute (mass%)

%x0: initial concentration of solute (mass%),

m0: weight of aluminium (kg)

r0: initial radius of specimen (m),

r: radius of specimen (m) and

ls: density of pure liquid (kg/m3).

Experimental values of the mass transfer

coefficient are determined by a method de-

scribed hereafter. Assuming that the dissolution

of solid metal is controlled by mass transfer in

molten metal, the reducing rate in weight of

cylindrical specimen per unit length is ex-

pressed by the equation:

Fig. 2 Schematic illustration of r, r1, r2, and con-
-(dw/dt)/L=k
obA(Cls-Cb), (5) centration distribution.

where

W: weight of specimen (kg), Even in the case of Fe-Si alloy in which the Fe

concentration becomes pretty high, Cls in the

L: dipping length (m)
binary Fe-Al phase diagram consists with that in

the ternary phase diagram within -3%. So, in

In this study, the rectified radius r1 mentioned this study, Cls from the binary phase diagram is

later is used. used.

 Dissolution of Ferrous Alloys into Molten Aluminium 783

W=r2sL
3. Calculation of theoretical and
and
experimental values of mass transfer
A=2r2. coefficient

Therefore, the apparent mass transfer coeffi- (1) Physical properties used in calculation

cient kob is written as The density value of molten aluminium

does not change among various measure-

kob=-r s(dr/d)/(%x ls/100
ments(19)(21)-(24). Here, the value of Ref. (23)
-%x
l/100)r2. is adopted. There are a few reports(22)-(24) on

It seems to be practically more valid to calculate the effect of solute Fe on the density of molten

this value adding Fe in Fe-Al alloy layer which aluminium, but no data about the Fe saturated.

is not yet dissolved into the bath. Hence, the So, change in the density of molten aluminium

radius calculated by eq. (1) is corrected, adding with solute Fe was roughly approximated by

an approximate amount of Fe in alloy layer to eq. (4) in the same manner as those of Ko-

the measured weight of specimen. The cor- saka(19) and Kawakatsu et al.(5).

rected radius r1(m) is given as follow: Values of the viscosity coefficient of molten

aluminium are considerably scattered(22)-(29)

(6) especially at low temperature. This is considered

where to be affected mainly by Al2O3(24). The vis-

r: radius of specimen (m) cosity coefficient measured by Gehbhardt et

A : density of alloy layer (kg/m3), al.(24) under the condition that the effect of

: thickness of alloy layer (m), =r2-r and Al2O3 might be the lowest, is the smallest. The

dipping depth of specimen, in this study, is

%xA: amount of Fe (mass%) in Fe-Al alloy

layer. shallow (0.03m) and the bath may be affected

Using this corrected radius r1, kob is expressed by Al2O3. Consequently, it is not valid to use

as follow: the measured value by Gebhart et al.(24) for

the viscosity coefficient. Hence, the value by

kob=-r1 s(dr/dt)
Yao et al.(27) is used. The viscosity coefficient

/(%xls ls/100-%x l/100)r2. (7) of molten aluminium is also influenced by solute

The apparent mass transfer coefficient kob is Fe(22)(24), but, the influence is littie compared

obtained by substituting the decreasing rate of to the scattered measured values, and there is

corrected radius -(dr1/dt), %x and l calcu- no measurement about the Fe saturated con-

lated from the experimental values into eq. (7). centration. Therefore, the effect of solute Fe

On using these equations, calibration for the on the viscosity coefficient is not taken into

saturated concentration by alloy composition consideration, but there still remains room for

is necessary, when the solid metal is not pure. discussion.

In this study, however, kob calculated from the There are few reports on the diffusion coeffi-

assumption that solid Fe of density s dissolves cient of Fe in molten aluminium(19)(22)(30)(31).

into molten aluminium is in good agreement Kosaka et al.(19) analyzed the dissolution of Fe

with kob calibrated by alloy composition within into molten aluminium, discussed the effect of

experimental error. Therefore, kob was calcu- solute Fe on the measured values, and adopted

lated in this study using eq. (7) without calibra- the value of Uemura et al.(31) since the con-

tion. centration of Fe is very close to the saturated

concentration at the alloy layer/Al boundary.

Therefore, in the present study, the values by

The thickness of the alloy layer is regarded as an
Uemura et al.(31) are adopted.
average thickness, and r1 represents an average

corrected radius of the specimen.

A is calculated in the same manner as eq. (4), The values from eq . (4) are in good agreement
assuming that there is no change in specific with the measured values in the range of low Fe
volume. concentration.
 784 Mitsuo Niinomi, Yoshisada Ueda and Masamichi Sano

Table 1 shows the values of physical prop-

erties mentioned above. The values at 1023K
were taken from curves approximated by the
values at 973 and 1073K in the literature.The
densities of ferrous alloys are shown in Table 2.

(2) Calculation of mass transfer coefficient

For the estimation of the apparent mass

transfer coefficient kob from eq. (7), the cor-

rected radius r1 must be calculated from eq. (6).

It is necessary to determine %xA of alloy layer.

%xA is obtained with the assumption that

Fe2Al5 occupies all alloy layers formed on each
Fig. 3 Relation between rectified diameter and
alloy, based on the previous report(1). In addi-
dipping time ( Fe-3Ni, -Fe-
tion, the density of alloy layer A was estimated
2C, ----Fe-3C).
to be 3.85103(kg/m3), in the same manner

as eq. (4). This value is valid as an approximate

value, because it is in good agreement with the is distributedin Al bath homogeneously. This
value A measured by Heuman et al.(32). Con- is considered to be reasonable, because the
sequently, the relations between the diameters natural convection based on the temperature
of various ferrous alloys corrected by eq. (6) distributionoccurs in Al bath, and the satu-
and the dipping time are shown in Figs. 3-5. rated concentration of soluteCls ismuch larger
The reducing rate of corrected radius is ob- than Cb.
tained from these relations. From these figures,

the corrected diameter for Fe-Si alloy is 4. Comparison of theoreticalvalue of mass

reduced linearly to the dipping time and transfercoefficient
with experimental
Value and discussionof controllingstep
parabolically decreases for the other alloys. So,
the relation between the corrected diameter The dissolution
of ferrousalloyintomolten
and the dipping time was approximated by a aluminium consistsof the followingprocesses;
line or a curve, and -(dr1/dt) was calculated. (a) reactionprocessat Fe/alloylayerinter-
The concentration of solute Fe (mass%) was face,
calculated on the assumption that dissolved Fe (b) diffusionprocess of Fe in alloylayer

Table 1 Values of physicalproperties.

Table 2 Density of ferrousalloy.

 Dissolutionof Ferrous Alloys into Molten Aluminium 785

Table 3 Mass-transfer coeff. kc and kob (dipped for

0.97.2ks).

Fig. 4 Relation between rectified diameter and

dipping time ( Fe-3Si, -Fe-

2Mn, ----Fe-3Mn).

Fig. 5 Relation between rectified diameter and

dipping time ( commercial pure iron,

-Fe-3Cu, ----Fe-3Cr). Table 4 Mass-transfer coeff. kc and kob (dipped for

0.97.2ks).

and formation process of alloy layer,

(c) reaction process at alloy layer/molten

aluminium interface and

(d) diffusion process of Fe into bulk

through diffusion layer in molten aluminium.

The mass transfer coefficient kc calculated

from the theoretical equation was compared

with kob obtained from the experiment, as

shown in Tables 3 and 4. In these tables,

values on the left side of arrows indicate those

of 0.9ks dipping and values on the right side

thoseof 7.2ks dipping,and valuesof 1.8ks or

In this study both of Fe and Al can be considered
3.6ks are intermediatebetween these two
as diffusion elements in tke alloy layer, and DFe values.As the measured values of physical
and DAl in the alloy layer are unknown. However,
propertiesused in the calculation
of theoretical
it is not clear which element is really a diffusion
values kc in Tables 3 and 4 are scattered
element. Anyhow, because this problem does not
considerably,accuratecomparison between kc
affect the analysis of the mass transfer of Fe in

molten Al, Fe may be regarded as a diffusion

and kobis difficult.
However, the discussionas
element. to which process of (d) or (a) to (c)controls
 786 Mitsuo Niinomi, Yoshisada Ueda and Masamichi Sano

the dissolution of ferrous alloy into molten the resistance of chemical reaction increases.
aluminium can be carried out. It can be sup-

posed as follows: If kckob, the (4) Fe-Mn alloy

process (d)
may be the controlling step of the kob issmaller than kc by about 40-70%. The
dissolution,

and if kobkc, one of (a), (b) or (c) may be the resistanceto chemical reactionor mass transfer
controlling step. In order to decide which in the alloy layer is not negligible.kob decreases
process of (a), (b) or (c) is the controlling step, with increasing dipping time, but the change is
more experiments will be necessary. the smallestexcept in the Fe-C alloy.The alloy
layer isthinner than that of commercially pure
(1) Fe-Cr, Fe-Cu and Fe-Ni alloys iron. The change in thickness with the dipping
At 973K, kob isalmost constantfor allthe time differsfrom those in other alloys,and the
dippingperiodsand equalto kc within -10%. layer becomes thinner with increasing dipping
Therefore,the dissolutionof thesealloysinto time and the structureof layer isporous(1).So,
molten aluminium iscontrolled by mass transfer further study may be necessary for this alloy.
of Fe in molten aluminium. At 1023 and
1073K, kob isequal to kc within -20% for a (5) Fe-C alloy
short dipping period,but decreaseswith in- kob ismuch smallerthan kc and about 1/3-
creasing dipping period, that is, with the 1/5 of the latter,and does not change with
growth of alloy layer(1).Differencesbetween dipping time.The dissolutionof thisalloyis
kc and kobat 1023 and 1073K are largerthan mainly controlledby the process except (d).
those at 973K. The reason is that the alloy In addition,althoughthe thicknessof the alloy
layersat 1023 and 1073K arethickerthan that layerchanges largerwith dippingtime than in
at 973K. Hence, itcan be speculatedthatthe the other alloys,kob changes little.Therefore,
alloylayerhas some resistanceto the chemical the dissolutionmay be controlledby the chemi-
reactionor mass transfer. cal reactionat the Fe/alloylayerinterface. In
the microstructures of Fe-C alloysas shown in
(2) Fe-Si alloy Photo. 1, cementiteincreaseswith increasing
At 973K, kobislargerthan kc by about 40- carbon content,and there existsneedle-like
60%, and at 1023 and 1073K, kobis equal to proeutectoidcementitein the Fe-2C alloyand
kc within 10-20%. At thesetemperatures,the more eutecticcementitein the Fe-3C alloy.
alloylayeron the Fe-Si alloygrows fasterand The structureof the Fe-C alloy is much
thickerthan that on the Fe-Cu alloy.kob different from those of the otheralloys.More-
increaseswith increasingdipping time.There- over, itwas observed that Fe3C remained in
fore,the resistanceof the alloy layer to the the alloy layer formed on the Fe-3C alloy
chemicalreactionor mass transferisnegligible. dipped at 973K(1). Therefore,the presenceof
A flakingof the alloylayermay be speculated cementite may assistthe resistanceto the
from the factthat kob islargerthan kc. How- chemicalreactionat the interfaceof the Fe-C
ever,thedegreeofitscontributionisnot evident alloywith the alloylayer.
for the accuracyof physicalpropertiesused in
the calculation
of kc. . Conclusion

(3) Commerciallypure iron The reactionbetween variousferrousalloys

kob issmallerthan kc by about 30-50%. The (commerciallypure iron,Fe-C, Fe-Si,Fe-Mn,
resistanceof the chemical reactionor mass Fe-Cr and Fe-Cu alloys)and molten alumin-
transferintheFe-Al alloylayerisnot negligible. ium was discussedfrom the viewpointof mass
kobdecreaseswith increasingdippingtime.The transfer. The resultsare as follows:
alloylayerformed on commerciallypure iron (1) For the Fe-Cr, Fe-Cu and Fe-Ni alloys
is the thickestamong all alloy layers and at 973K, the experimentalvalue of the mass
increaseswith increasingdippingtime.There- transfercoefficient kob is nearly equal to the
fore,the resistance
of mass transfercontaining theoretical value kc.Therefore,the dissolution
 Dissolutionof Ferrous Alloys into Molten Aluminium
Photo. 1 Microphotographs of (a)commercially pure iron,(b) Fe-2C alloy (as cast),and (c)
Fe-3C alloy(ascast).
is controlledby the mass transferof Fe in
molten aluminium. At 1023 and 1073K, kob
decreaseswith increasingdipping time. So,
the resistanceto the chemicalreactionor mass
transferin the alloylayersisnot negligible.
(2) For the Fe-Si alloy,kob isa little
larger
than kc and increasesslightlywith increasing
dipping time. The resistanceto the chemical
reactionor mass transferisnegligible.
(3) For the commercially pure iron,kob is
smaller than kc by about 30-50%. So, the
resistanceto the chemical reaction or mass
transferis not negligible. kob decreaseswith
increasingdippingtime,thatis,with the growth
of the alloylayers.
(4) For the Fe-Mn alloy,kobissmallerthan
kc by about 40-70%. The resistanceto chemical
reactionor mass transferin the alloy layeris
not negligible.But, further study may be
necessaryfor thisalloy.
(5) For the Fe-C alloy,kobismuch smaller
than kc and about 1/3-1/5of the latter.The
dissolution intomolten aluminium iscontrolled
by the chemicalreactionor mass transferin the
alloylayer.
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