Y. Wang et al. / Journal of Alloys and Compounds 646 (2015) 626e631
627
difficulty in sintering densification, more internal pores and flaws
and a lot of dust, which bring about environmental pollution and
damage to people's physical health.
In view of a lot of advantages by the co-precipitation method,
such as the uniform material chemical composition, good purity
and good crystal structures and low sintering temperatures, it be-
comes the research and development focus of the preparation of
ceramic nuclear fuel and material in the world [11]. As an advanced
technology to produce ceramic materials, however, there are rare
stirred and then heated to the reaction temperature in the pre-
cipitation tank. Then saturated (NH CO solution was added into
4
)
2
3
the tank at a certain flow rate (5 ml/min). When the feeding
finished, a certain volume (60e80 ml) of anhydrous ethanol was
added. After a period of time (0.5e1 h) the precipitation reaction of
the mixed solution finished and the solution lost liquidity. After
sediment filtering, the filter cake was washed three times with
ꢀ
anhydrous ethanol and dried at 65 C for 15 h to get precursor. The
ꢀ
precursor was kept at 600 C for 2.5 h, cooled and ground to pro-
ꢂ2
research reports on the preparation of CaO-doped UO
Gd fuel pellets by co-precipitation reaction method.
(NO , Gd(NO and Ca(OH) were adopted as the initial
experimental materials in this paper. UO -10 wt% Gd fuel with
different contents of CaO (the mass fraction of 0, 0.3%, 0.5% and
.6%, respectively) were prepared by co-precipitation reaction
2
-10 wt%
2 2 3
duce UO eGd O eCaO powder, which was pressed by 4 ton cm
2
O
3
pressure into cylindrical powder bulks with the diameter of about
8 mm and the height of about 10 mm. The pressed powder bulks
UO
2
3
)
2
3
)
3
2
2
2
O
3
were sintered in the reducing atmosphere into CaO-doped UO
10 wt% Gd ceramic fuel pellets. The sintering atmosphere was
, the sintering temperature was 1650 C, and the hold time was
3.5 h.
In order to study the effect of CaO doping on UO
respectively, UO -1 wt% CaO and Gd -1 wt% CaO samples were
2
-
2 3
O
ꢀ
0
H
2
method and sintered in different sintering process conditions. The
paper studied the effects of sintering temperatures and CaO con-
tents on the sintered density, densification dynamics, grain sizes
and crushing strength. In addition, its microstructure and phase
structure were analyzed. The research results provided techno-
2
2 3
and Gd O ,
2
2 3
O
prepared by the above-mentioned method, which were sintered at
ꢀ
1100, 1200, 1300, 1400, 1500 and 1600 C in the sintering atmo-
logical base for the preparation and application of CaO-doped UO
0 wt% Gd
safety for advanced nuclear power use.
2
-
sphere of H
2
with the hold time of 3 h.
1
2 3
O burnable poison fuel with high burn-up and inherent
2.2. Characterization and measurement
ꢀ
2
. Experimental method
After the cylindrical powder bulks was heated up to 1650 C in
2
, its shrinkage was measured by a lever dilatometer. The densities
H
2
.1. Fuel preparation
of fuel pellets are measured with water immersion method. The
Optical microscope (OM) is used to observe the metallurgical
structures of fuel pellets. Line intercept method is adopted to test
the average grain sizes of pellets. The phase structures of fuel pel-
lets are tested with D/max22400X X-ray diffractometer (XRD).
Electronic universal testing machine was used to measure the
crushing strength of cylinders with height-diameter ratio of 1:1.
The specific measurements were as follows: (1). The pressure sur-
faces sizes of tested samples were measured and the areas were
calculated. The samples for each group are not fewer than 3; (2).
The samples were put in the center of the pressure plate of the
(
1) The preparation of mixed solution of UO
and Ca(NO
2
(NO
3
)
2
, Gd(NO
3
)
3
3 2
)
First, in accordance with the traditional approach to the prep-
aration of nuclear fuel for pressurized water reactors, UO pellets
2
with the ration of O/U ¼ 2.10 are prepared with the raw material of
2
35
ammonium diuranate (ADU,
pellets are broken into UO
U content ¼ 0.2 at%). The UO
2
2
powder with the particle size
ꢀ
ꢁ
1e2
m
m.The UO
2
powder was dried at 350 C for 2.5 h and 99.9%
2
Gd
2
O
3
powder with the particle size ꢁ1
m
m (Ganzhou holmium xin
tester. Load was added at a rate of 2 ꢃ 10 N/s until the sample was
ꢀ
new materials co.,LTD) was dried at 550 C for 2 h. Based on the
destroyed. The maximum load was recorded during that moment;
(3). The test results were put in the following formula to calculate
mass fractions of Gd
amount of dry powder (90 g UO
put into the dissolving tank together with a certain amount
2
O
3
in UO
2
-10 wt% Gd
2
O
3
fuel pellets, a certain
2
powder, 10 g Gd
2
O
3
powder) was
the crushing strength. R
MPa, P is failure load, N, and S is stressed area.
C
¼ P/S, where R
C
is the crushing strength,
(
(
450e500 ml) of deionized water. By rapid stirring, moderate
95e105 ml) concentrated nitric acid was added into the dissolving
3. Results and discussion
tank. After complete dissolution, insolubles were filtered out and
the remaining clear filtrate was mixed solution of UO
Gd(NO
The mass fractions of CaO in doped UO
pellets were 0, 0.3%, 0.5% and 0.6%, respectively calcium hydroxide
was weighed according to the proportion of CaO and stirred with
2
(NO
3
)
2
and
3.1. Phase analysis of CaO-doped UO
2 2 3
eGd O fuel pellets
3 3
) .
2
-10 wt% Gd
2
O
3
fuel
Fig. 1 is XRD diffraction pattern of UO
different CaO contents after sintering at 1600 C in H
time of 3.5 h at the heating rate of 4 K min . There were few dif-
2
eGd
2
O
3
fuel pellets with
with the hold
ꢀ
ꢂ1
2
5
ml water. 1e2 ml concentrated nitric acid was added and dis-
solved to get stable Ca(NO solution. By rapid stirring, Ca(NO
was slowly dropped into the mixed solution of UO
ferences among the XRD diffraction patterns of UO
pellets with different CaO contents as shown in Fig. 1. Almost all
were UO phase diffraction peaks, demonstrating that substitu-
tional solid solution formed in UO -Gd fuel pellets with
different contents of 10 wt% Gd . Fig. 1 shows that when 0.3 wt%
CaO was added into UO eGd fuel pellets, there were not other
2 2 3
-Gd O fuel
3
)
2
3 2
)
and
2
(NO
3
)
2
2
Gd(NO
Gd(NO
3
)
)
3
3
. In the end, uniform mixed solution of UO
and Ca(NO was prepared.
2
(NO
3
)
2
,
2
2 3
O
3
3
)
2
2 3
O
O
2 3
2
(
2) The preparation of saturated (NH
4
)
2
CO
3
solution
peaks in the XRD diffraction pattern, indicating that CaO solved into
the fuel pellets and uniform solid solution formed. And when 0.5%
2
2 g analytically pure solid ammonium carbonate was put into a
CaO was added into UO
showed weak CaO diffraction peaks. When CaO content increased
to 0.6%, the precipitated CaO from UO eGd fuel pellets also
2 2 3
eGd O fuel pellets, the XRD pattern
beaker together with 100 ml deionized water. In the condition of
rapid stirring, saturated (NH
4
)
2
CO
3
solution was prepared.
2
2 3
O
increased. The XRD pattern showed the increase of CaO diffraction
peaks.
(
3) The preparation of fuel pellets
From Fig. 1, the diffraction peaks in XRD diffraction pattern
showed tiny changes with the increase of CaO content. XRD
The mixed solution of UO
2
(NO
3
)
2
, Gd(NO
3
)
3
and Ca(NO
3
)
2
was