JOURNAL OF RARE EARTHS

V o l . 2 4 , Spec. Issue, Dee. 2006, p . 3 0 6

Influence of Solidification Rate on Microstructures of Cast Strips and Cor-

responding Sintered NdFeB Magnets
Yu Dunbo (?a&),
Xu Jing (4& if9) * , Yan Shihong (Be%), Li Zongan (+$%),
I,i Shipeng (*I&&), Li Hongwei (+hsE)
(National Engineering Research Center for Rare Earth Materials, General Research Institute jbr Nonferrous Metals,
and Grirem Advanced Materials Co . Ltd. , Beijing 100088, China)

Abstract: The influences of solidification rate on the microstructures of cast strips and corresponding sintered NdFeB mag-
nets were investigated. The experimental results show that the volume fraction and size of columnar grains vary with the
wheel speed V , and the fraction is highest to more than 90% with 3.5 p m in average width at V = 2 m's-'. The reasons
for the improved magnetic performance were discussed based on the micromagnetic theory and microstructure analyses of
the strips and sintered magnets. The magnetic properties of sintered NdFeB magnets made from the (Nd,Dy)ls.o(Fe,Ga,
Al)80.5B6.5cast strip which was obtained at V = 2 rn's-' are as follows: B , = 1.15 T( 11.25 kG), iH, = 2799 kA.m-'
(35.2 kOe) and (BH),,,=242 k J ~ r n - ~ ( 3 0 . 3MGOe).
5

Key words : sintered NdFeB magnets ; solidification rate ; cast strip ; microstructure ; rare earths
CLC number: TM273 Document code: A Article ID: 1002 - 0721 (2006) - 0306 - 04

Since the NdFeB magnetic materials firstly came
into being in 1983, NdFeB sintered magnets"] have
been remarkably expanding in the global markets.
Over 20 years, Japan has been keeping leading posi-
tion in the world in its research and development.
However, Chinese NdFeB industries grow in a star-
tling speed, which arouses great concern all over the
world. Especially in recent years, a few Chinese mag-
net producers have possessed the capability of produc-
ing high-ranking NdFeB magnets such as N50,
N48M, 32AH and so on, mainly because of adopting
advanced technologies such as strip casting technique.
For conventional ingots, when the total rare earth con-
tent is lowered to a certain level, a-Fe dendrites al-
ways appear due to the peritectic nature of the hard
magnetic NdzFellB compoundrz1, which enhances the
difficulty of making powder and hinders grain align-
ments in the subsequent proce~sing'~'.In addition,
large Nd-rich regions which are much sensitive to oxi-
dation can be found in the cast ingots. There are lots
of advantages in Strip Casting (SC) technology[4v51,
such as saving RE resources, homogenizing the colum-
nar structures, suppressing the formation of a-Fe den-
drites. It is well known that formation of a-Fe, fine
columnar crystals and the Nd-rich phase of thin layer
during casting mainly depend on the solidification
rate. Therefore, controlling the solidification rate in
order to obtain sound microstructures of the cast strips
and high performance sintered magnets has become an
important issue.
1 Experimental
The material employed in this paper was ( N d ,
Dy)l,,o(Fe,Ga,A1)80.5B~.5(%, atom fraction). It was
prepared by melting corresponding elemental metals in
alumina crucible using a vacuum induction furnace
under argon gas atmosphere. After melting, the mol-
ten alloys were poured onto a rotating copper roller.
During SC process, the peripheral speed of the cooling
- - '
roller was 1 3 m s - . After hydrogen decrepitation
(HD) process, the cast strips were pulverized directly
-
into fine powders of about 3.0 4.5 p m in mean size
by jet milling. Then, the powders were compacted in
a magnetic field, sintered and annealed at optimum
temperature. The microstructures of cast strips and
corresponding sintered magnets were investigated by
scanning electron microscope ( SEM ) and optical mi-
croscope. The composition of phases was analyzed by
energy spectra. The densities of the sintered magnets
were measured by the Archimedes displacement prin-

Received date : 2006 - 07 - 25 ; revised date : 2006 - 09 - 08

Foundation item: Project supported by RE Application Engineering of National Ten-Fifth Year Plan of China (2002BA315A-1)
Biography: Xu Jing (1974 - ) , Male, Engineer; Research field: Rare earth magnetic materials
* Corresponding author (E-mail: ydbmail @yahoo. corn)
 Xu J et a1 . Microstructure of Cast Strips and Corresponding Sintered NdFeB Magnets
ciple in water. The magnetic properties were measured
by a hysteresisograph .
2 Results and Discussion
2. 1 Microstructures of cast strips pre-
pared at different solidification rate
The obtained cast strips were about 0. 6 , 0. 3 ,
0.2 mm in thickness with the increasing wheel speed
V = 1, 2 and 3 m s respectively. The optical micro-
graphs of cast strips are shown in Fig. 1. The white is
main phase, and the grey is Nd-rich phase. In addit-
ion, dendrite phase as a-Fe can only be found in cast
strip prepared at V = 1 rn's-' in Fig.2 by using scan-
ning electron microscope. Compared the three images
in Fig. 1 , it can be found that there are best micro-
structures in cast strip prepared at I/ = 2 m * s - l in
Fig. l ( b ) , where the volume fraction of the columnar
grains is over 90%, and fine and uniform columnar
grains are about 3.5 pm in average width with the Nd-
rich phase distributing uniformly along the boundaries
of main phase. However, as shown in Fig. 1( a ) , the
volume fraction of the columnar grains is less than
70% in cast strip prepared at V = 1 m e s - ' , and the
grain size are not uniform with 4. 5 pm in average
width. While, Fig. 1 ( c ) shows two kinds of micro-
'
structure in cast strip prepared at V = 3 m * s - : one is
Fig. 1 Optical micrographs of cast strips prepared at different wheel speed
( a ) Y = l m - s - ' ; ( h ) 1 / = 2 m . s - ' ; ( c ) V = 3 rn's-'
Fig.2 Scanning electron image of a-Fe in cast strip prepared
at V = 1 rn-s-'
307
some over-small isometric grains with average sizes of
about 2 . 0 pm appearing on the cooling surface of
strip, the volume fraction almost 40%, and the other
is columnar grains close to free surface of the strip that
whose the average size is about 4.0 p m . It is known
that the cooling rate of SC process is faster than that of
conventional casting, which makes the temperature
gradient in the strips higher than that in the ingots.
When the cooling rate is higher than 1 x lo3"c * s - , '
the primary crystals of 7-Fe are suppressed and the
peritectic reaction is hindered, thus Nd2Fe14B phase
precipitates directly from liquid phase and no a-Fe
forms. However, when the peripheral speed of cooling
roller was about 1 m - s - ' , the solidification rate in
cast strips is still not high enough to suppress the for-
mation of a-Fe effectively (Fig. 2 ) . On the contrary,
when the peripheral speed of cooling roller is
3 m - s - ' , the solidification rate in cast strips is so high
that over-small isometric grains appear on the cooling
surface. Commonly, the formation of columnar grain
structure is related to solidification rate and tempera-
ture gradient, both of which are related to the wheel
speed. Therefore, the wheel speed of V = 2 m * s - is '
suitable in this investigation because it provides high
and suitable cooling rate which can refine and homoge-
nize the columnar structures and make the Nd-rich
phase distribute uniformly along the boundaries of the
columnar grains. The microstructure in cast strip of
Fig. 1 ( b ) is just a good example, where the cooling
-
rate of strip is about 1 x I d 1 x 104"c.s-', which is
the main reason for the absence of a-Fe dendrite pre-
cipitation and the formation of desirable microstruc-
tull:. It is known that the Nd-rich phase is hydrog-
enized first during the HD process, which leads to an
intergranular crack, and then the Nd2Fe14B phase,
which leads to a transgranular crack. For the cast
strips, the uniform distribution of Nd-rich phase along
the grain boundaries are favorable for obtaining HD
powders composed of single grains on the whole. So,
308
by using the cast strips prepared at V = 2 m *s - l , the
final fine powders for sintering with a good particle size
distribution and less than 3.5 pm in average size are
easy to obtain.
2.2 Microstructures and magnetic proper-
ties of sintered magnets made from
cast strips
Magnetic properties of sintered magnets produced
from the cast strips mentioned above are shown in Ta-
ble 1. The optical micrographs of sintered magnets are
shown in Fig. 3. It is found that using cast strip pre-
pared at V = 2 m a s - ' as starting material for magnet
sintering leads to higher magnetic properties: B , =
1.15 T , coercivity H , = 2799 kA * m - , maximum en-
ergy product ( B H ) , , = 242 k J * m - 3 . In addition, the
sintered density of the magnet with optimum perfor-
mance reached 7.56 g *cm-3 at a lower sintering tem-
perature of 1060 "c . Using the other two strips as star-
ting material, the sintered density of the magnet
reached 7 . 5 3 and 7 . 51 g * cm-3 respectively at the
same sintering temperature of 1060 "c . Generally, ac-
cording to the micromagnetic theoryL6], H , can be ex-
pressed as
2Kl
IHC= -ff k f f 4ffex - N e f f M ~ (1)
M,
where K 1 is the anisotropy constant, M , the saturation
magnetization, a k a factor related to uniformity of K ,
in main phase, a Qa factor related to alignment of ma-
in phase crystals, aeXa factor related to uniformity of
Nd-rich phase, and NeIIeffectively separated magnetic
field factor proportional to the size of crystals. Com-
paring the three kinds of cast strips, the strip prepared
Table 1 Magnetic properties of sintered magnets in three
samples
Preparation velocity for B,l i H,l (BH),l
starting dloy I / / ( m * s - ' ) T (kASm-l) (kJam-3)
v = 1 m-s-1 1.13 2245 238
V=2 m.s-' 1.15 2799 242
V =3 m*s-' 1.11 1276 230
Fig.3 Optical micrographs of magnets made from cast strip prepared at V = 1 rn*s-'(a), V = 2 m - s - ' ( b ) , and V = 3 m * s - ' ( c )
JOURNAL OF RARE EARTHS, Vol. 2 4 , Spec. Issue, Dec . 2006
at V = 2 m - s - ' has many advantages: firstly, the mi-
crostructure of fine and uniform columnar crystals
made it possible for the strip to possess bigger value of
a kand less NSff.Secondly, for the fine powder pre-
pared from the cast strips, the Nd-rich phase distrib-
utes uniformly on the surfaces of powder particles,
which leads to a higher aeXin the sintered magnets.
Thirdly, the powders having no a-Fe which deterio-
rates the magnetic alignment, as well as being made
up of single crystal particles are favorable for magnetic
alignment, which leads to a higher in the sintered
magnet. Therefore, using the cast strip prepared at
optimum solidification rate, a sintered Nd-Fe-B mag-
net with higher i H , is expected to obtain. According to
analysis above, it can be found that the microstructure
of sintered magnets plays an important role in deter-
mining their H , . Namely, a uniform fine microstruc-
ture and good distribution of the Nd-rich phase lead to
a high H , .
From Fig. 3( c ) , extremely big grains can be seen
in the microstructure of sintered magnet made from the
strip prepared at V = 3 m - s - ' , It is because of grains
aggregation and the growth of Nd-Fe-B permanent
magnet alloy in the process of sintering. In other
words, some bigger grains eat the smaller grains
around to form the preternatural big grains. So the
Nd2Fe14Bmain phase grain abnormally grows up to 70
- 80 pm in long axis direction during the sintering
process, which greatly decreases the coercivity of the
magnet to 1276 kA * m - ' . Therefore, it is necessary
for preparing high coercivity magnets to reduce the
number of over-small isometric grains in cast strips
and fine powers in jet milling.
3 Conclusions
1. When the cooling roller speed is 1 rn * s - , the
dl solidification rate is too low, which leads to the in-
(g.m-3) creasing of the thickness of the columnar grains of the
7.53 main phase. At the same time, the formation of a-Fe
7.56
can not be completely suppressed.
7.51
 Xu J et a1 . Microstructure of Cast Strips and Corresponding Sintered NdFeB Magnets
'
2 . When the cooling roller speed is 2 m s , the
solidification rate is suitable, and the main phase
grain of cast strip possesses fine and uniform columnar
crystal strurture with thickness of 3.5 pm separated by
Nd-rich phase of thin layer dispersing uniformly along
the boundary of main phase, which is favourable to
prepare high performance sintered magnets.
3 . When the cooling roller speed is 3 m - s - I , the
solidification rate is too high, which leads to the de-
creasing of the thickness of the columnar grains of the
main phase and the appearing of over-small isometric
grains on the cooling surface of strip. It tends to make
the Nd,Fe,,B main phase grain abnormally grow during
the siritering process, which greatly decreases the co-
ercivity of the magnet.
4. Uniform fine microstructure and good distribu-
tion of the Nd-rich phase lead to a high H , . It is nec-
I
309
essary for preparing high coercivity magnets to reduce
the number of over-small isometric grains in cast strips
and fine powders in jet milling.
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