Solid State Ionics 36 (1989) 85-88
North-Holland, Amsterdam
MECHANISM OF OXYGEN INCORPORATION IN THE YBa2Cu306.9 SUPERCONDUCTOR
F. CROCE, B. SCROSATI
Dipartimento di Chimica, Universit~di Roma, "La Sapienza", Rome, Italy
and
C. ALVANI, S. CASADIO
ENEA/TIB/CHI, CRE-Casaccia, Rome Italy
Received 24 March 1989;acceptedfor publication 20 April 1989
It is well known that the oxygencontent exherts a critical role in determining the electrical characteristics of the perovskite
cuprate superconductors. However,the formal oxidation state of copper in the compoundsas well as the mechanism of oxygen
incorporation in their structure, are still a matter of discussion. In this work, we propose two possible disorder equilibria in the
400°C to 525°C temperature range and attempt to substantiate them by experimental evidence.
1. Introduction
It has now been certain [ 1,2 ] that oxygen is cru-
cial in controlling the electrical behaviour of the re-
cently discovered perovskite cuprate superconduc-
tors [3-5]. These compounds appear to contain
copper in a formal oxidation state greater than two,
which is controlled by the oxygen content. Thus, the
superconductivity characteristics are greatly affected
by the annealing conditions of the samples, being
particularly sensitive to oxygen partial pressure and
to temperature.
The Ba2YCu307_x type materials undergo a te-
tragonal-orthorhombic phase transition at a temper-
ature which greatly depends upon oxygen partial
pressure, varying from 530°C under 1% of oxygen to
700 ° C under 100% of oxygen [ 1 ]. In air (21% ox-
ygen) the transition temperature is of the order of
650°C. At low oxygen partial pressure (i.e. <0.01%),
a change in the electric properties of the materials
(which pass from a metallic to a semiconducting be-
haviour) has also been evidenced [ 1 ].
Therefore, it has seemed to us of importance to
further investigate the role of oxygen in the cuprate
superconductors and in this work we propose a
mechanism for the process of oxygen incorporation
in YBa2fu306.9 in the temperature range of 400 to
525 °C.
2. Experimental
The YBa2Cu306.9 compound was prepared from
mixed powders of CuO, BaO and Y203, heated at
900 ° C for a few hours. The material was then pressed
and sintered in air at 950°C for about seven hours
with a slow cooling to room temperature. The geo-
metrical density was 5.08 g/cm 3, corresponding to
the 79.4% of the theoretical values 6,4 g/cm 3. X-ray
analysis indicates that our specimens are single phase,
comparable with the best ceramic samples reported
elsewhere.
The samples, cut into bars with a rectangular base
having the dimensions of 30 × 4 X 2 ram, were kept
in a controlled environment cell situated in an oven,
in order to perform the desired resistivity test under
various atmospheres and temperature conditions. A
four-probe technique was used for the resistivity test.
Silver wire terminals were attached to the sample by
silver paste. The measurements were carried out both
under dc and ac polarizations using a Solartron Fre-
quency Response Analyser, model 1250 coupled with
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