ELSEVIER Physica C 341-348 (2000) 2475-2476
www.elsevier.nl/Iocate/physc
Melting and Solidification of Y1-xYbxBa2Cu3Oy" Influences of Yb doping and Oxygen
Partial Pressure
Yuxiang Zhou and Tong B. Tang
Physics Department, H.K Baptist University,
Waterloo Road, Kowloon, Hong Kong
A comparative study was undertaken into the calcination conditions for the solid-state synthesis of pure
Yl.xYbxBa2Cu307_ ~ (x=0, 0.25, 0.5, 0.75, 1.0), the starting materials being Y203, Yb203, BaCO3 and CuO. It was
found that the calcination time should go up and the sintering temperature should lower, when the average rare
earth ionic radius decreases. Moreover, the melting and the solidification temperatures of Yt.xYbxBa2Cu3Oy rise
with decreasing Yb doping and increasing oxygen partial pressure, but depend only weakly on the particle size
distribution. These deductions will be important to the fabrication of large-grain (Y,Yb)BaCuO
1. Introduction
Recently, superconducting (RE)BCO materials
have been fabricated in large grain form via
peritectic solidification. Grains thus obtained can be
several cm in diameter with Jc a few times 10SAcra 2
at 77K [1-4]. At the peritectic temperature Tp of 900
to 1080°C, RE-123 is formed from solid RE-211,a
Ba-Cu-O based liquid phase and oxygen gas [3],
(RE)2BaCuO5+Ba3CusOr.72+0.4202
- ) 2(RE)Ba2Cu3Or.2s
Unfortunately there have been few reports on
fabricating large grain (Yb, Y)BCO [5-7]. Hence
this work, which aimed to clarify also the effects of
particle size distribution and oxygen partial pressure
on the underlying thermal events.
2. Experimental
Solid-state reaction synthesis was used to
produce Yl_xYbxBa2Cu3Oy (x=0, 0.25, 0.5, 0.75, or
1.0). Y203(99.9%), Yb203(99.9%), BACO3(99.9%)
and CuO (99.5%), all from Fluka, were thoroughly
mixed in the stoichiometric ratio, calcined in air at
880°C for 24 hours, then subjected to two
consecutive sinterings at 900 and 920°C, both for 24
h with intermediate grinding. The product was
pressed into pellets, and sintered at various
temperatures from 860 to 920°C for different x for
the same period of 24h, followed by annealing at
500°C in flowing 02 for 20h, before cooling down
to room temperature in the furnace.
The (Y,Yb)BaCuO powder thus obtained was
milled in ethyl alcohol with agate balls in an agate
jar for different periods (10, 20, 30 and 40h), dried at
130°C, then ground again in a mortar with a pestle.
Powder X-ray diffraction patterns of both as-
prepared and milled powder at room temperature,
were taken in a Rigaku D/MAX-C diffractometer,
equipped with a filter but no monochrometer. Phase
identification was achieved through searches in the
Powder Diffraction File database from JCPDS-
International Center for Diffraction Data.
For estimation of their particle size, ball milled
samples were examined in a Jeol JSM-T330A
Scanning Electron Microscope operated at 20 kV.
For simultanious thermogravimetry (TG) and
quantitative differential thermal analysis (qDTA),
a SETARAM TGA 92-16 combined thermal
analyser was used. Annealed alumina powder served
as the reference in calorimetry. Measurements
proceeded in different atmospheres as specified in
the Results section. The program was always heating
from 500 to 1100°C, isothermal for 30 minutes, then
cooling, at the same rate of 5 K/min.
3. Results and discussion
X-ray diffraction patterns showed that, for the
series of samples fabricated under the same
conditions, phase purity deteriorated as x increased.
In YbBa2Cu3Oy, lower sintering temperature and
longer calcination time reduced but could not
eliminated the impurity phases if the sintering
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