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GB2247883A - Superconducting spinel materials - Google Patents
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GB2247883A - Superconducting spinel materials - Google Patents

Superconducting spinel materials Download PDF

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Publication number
GB2247883A
GB2247883A GB9119649A GB9119649A GB2247883A GB 2247883 A GB2247883 A GB 2247883A GB 9119649 A GB9119649 A GB 9119649A GB 9119649 A GB9119649 A GB 9119649A GB 2247883 A GB2247883 A GB 2247883A
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GB
United Kingdom
Prior art keywords
time interval
making
group
superconducting material
superconducting
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Granted
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GB9119649A
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GB9119649D0 (en
GB2247883B (en
Inventor
John Henry Binks
Trevor James Cogle
John Thomas Sirr Irvine
Carlos Alexandre Sereno Mateus
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NAT RES DEV
National Research Development Corp UK
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NAT RES DEV
National Research Development Corp UK
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Publication of GB9119649D0 publication Critical patent/GB9119649D0/en
Publication of GB2247883A publication Critical patent/GB2247883A/en
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Publication of GB2247883B publication Critical patent/GB2247883B/en
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    • CCHEMISTRY; METALLURGY
    • C04CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04BLIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B35/00Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C04B35/01Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics
    • C04B35/46Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on titanium oxides or titanates
    • CCHEMISTRY; METALLURGY
    • C04CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04BLIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B35/00Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C04B35/01Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics
    • C04B35/46Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on titanium oxides or titanates
    • C04B35/462Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on titanium oxides or titanates based on titanates
    • C04B35/465Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on titanium oxides or titanates based on titanates based on alkaline earth metal titanates
    • HELECTRICITY
    • H10SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10NELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10N60/00Superconducting devices
    • H10N60/80Constructional details
    • H10N60/85Superconducting active materials
    • H10N60/855Ceramic superconductors

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  • Engineering & Computer Science (AREA)
  • Chemical & Material Sciences (AREA)
  • Ceramic Engineering (AREA)
  • Manufacturing & Machinery (AREA)
  • Materials Engineering (AREA)
  • Structural Engineering (AREA)
  • Organic Chemistry (AREA)
  • Compositions Of Oxide Ceramics (AREA)
  • Inorganic Compounds Of Heavy Metals (AREA)

Abstract

A superconducting material comprises a spinel structure crystal including an element from group II and an element from group IVB of the periodic table.

Description

Superconducting materials This invention relates to superconducting materials.
There has been much recent interest in copper oxide superconductors; however, the first oxide superconductors to be discovered with critical temperature (Tc) above 40K, Ba(Bi , Pb)09 and LiTi204, contained no copper Liti204, which has the cubic spinel structure and an average Ti valence of 3.5, exhibits a superconducting critical temperature of 13 K. Superconductivity has been observed for a range of compositions, close to x . 0, in the solid solution series Li During a recent investigation of the spinel solid solution series Mg2TiO4 - MgTi204, a resistive transition was observed at -500K for compositions with an average Ti valence close to 3.3.
This transition was reproduced in samples from several batches.
According to the present invention there is provided a superconducting material comprising a spinel structure crystal including an element from group II and an element from group IVB or the periodic table.
The invention will now be particularly described with reference to the accompanying drawings, in which: Figure 1 is a plot of resistivity versus temperature for a freshly prepared sample of Mg1#421Ti 1.57904, x.3.267, with In/Ga electrodes; and Figure 2 is a plot of resistance versus temperature for an x.3.267 sample, with In/Ga electrodes under various conditions.
Samples of composition Mg2~yTil+yO4 with average Ti valence x, XD (4-2y)/(y+l), were prepared using the following procedure. Appropriate quantities of MgO, TiO2 and Ti were weighed out, ground together with acetone in an agate mortar and pressed into pellets. The pellets were wrapped in graphite foil and placed in the centre of an alumina tube furnace under a constant flow of argon. Particular care was taken to minimise any diffusion of air into the gas stream, using metal tubing and teflon seals. Temperature was increased to 13500C over a period of 3 hours and the samples fired for 16 hours. The temperature was then reduced to room temperature over 4 hours and the samples removed from the furnace.
Phase purity was checked by powder X-ray diffraction using a Guinier-Hagg camera. Samples with average Ti valence close to 3.3, or less, were generally almost single phase. A small amount of second phase, < 5%, with an X-ray diffraction pattern similar to that for MgTiO3, was sometimes detected. Further reaction was not found to increase phase purity, instead the amount of second phase present was often observed to increase, probably due to oxidation; A systematic variation in lattice parameter with composition was observed, with a value of 8.482 ..002 A for x=3.267. The observed lattice parameters were consistent with reported values for Mg2TiO4, 8.445, and MgTi2O4, 8.502. Thermogravimetric analysis confirmed that the average Ti valence was, within errors, (t.05) unchanged from the starting value.
Four terminal dc resistance measurements were performed on samples mounted on a helium cryotip, using a Au (0.7% Fe)/chromel thermocouple to monitor temperature (t20K).
The sample was cooled to -150K, held for 30 minutes, then allowed to warm up at -20Kmin#1. Both current and voltage were monitored throughout. Either indium/gallium alloy or drfed silver paste electrodes were used. The room temperature resistivity was measured by two terminal ac impedance spectroscopy. The value obtained was then used to convert resistances at lower temperatures to resistivities.
On cooling the resistance of compositions with x > 3.3 rose sharply as temperature was decreased. For compositions with x < - 3 25, resistance also rose, though much less sharply, as temperature decreased. The behaviour of samples with average Ti valence between 3.25 and 3.3 was dependent upon sample history; however, compositions with x=3.267 and x=3.3 both showed evidence of zero resistance behaviour (Table 1). A typical resistivity temperature curve for a freshly prepared sample of x 1 3.267, shows a transition from zero resistance to semiconducting behaviour between 51.5 and 600K, Figure 1. At 150K, it was possible to pass up to 1 A cm~2 without any detectable voltage, indicating a resistivity of less than lOpohm-cm.
Figure 2 illustrates the deterioration of the zero resistance properties on standing. Curve 1 shows a resistance versus temperature plot for a sample allowed to to stand for three days in a vacuum desiccator (#10T) The 500K transition is still apparent; however, a second transition at about 450K was also observed with a low temperature tail indicative of weak link behaviour. In this condition the critical current was quite low with ohmic behaviour being observed for currents above 100 pA cm~2 at 150K.On standing for a further two days, the resistive transition could no longer be observed on cooling (curve 2), instead, for temperatures below 700K,the contact resistance became too high for the voltage source (- < 100V) to drive a significant current (1spa). On taking this sample, removing the electrodes and firing for 16 hours at 13000C under flowing argon, the original resistive behaviour was regenerated, (curve 3 figure 2). It was found that if the samples were stored in a good vacuum (#10-3T), the resistive transition could be preserved, unchanged, for several days.
When silver was used as electrode material, contact resistances were very much higher than for In/Ga alloy electrodes. Although similar resistive transitions were observed using Ag for both x=3.267 and x=3.3 (table 1), it was not possible to measure the resistance through the maximum of the transition.
The observed degradation in conducting properties on standing indicates that this zero resistance behaviour is associated with a phase or state highly sensitive to the presence of oxygen or water vapour. It may be that this behaviour is critically dependent upon the degree of oxidation of the spinel phase or of a surface layer, or it may be due to a metastable state that transforms rapidly in the presence of oxygen or water vapour. No significant changes in the X-ray powder diffraction pattern could be detected, however.
TABLE 1 Summary of Resistance versus Temperature Measurements.
x Electrode Tc,onset Tc(R=O) Resistance Sample / K / K Maximuma age / ohms 3.267 In/Ga 60 51.5 150 < 1 hour 61, 47 50b, 45 300 3 days > 600 5 days 51 62 200 < 1 hourC Ag ?60 33 > 100 1 hour 3.3 In/Ga 38 30b,d 200 1 day a. 40 ohm corresponds to -1 ohm-cm b. Extrapolated value c. After 16 hour Ar anneal at 13000C d. A constant resistance value of 0.5 ohm was observed below 380K

Claims (11)

  1. CLAIMS 1. A superconducting material comprising a spinel structure crystal including an element from group II and an element from group IVB or the periodic table.
  2. 2. A superconducting material as claimed in claim 1 wherein the group II element is magnesium.
  3. 3. A superconducting material as claimed in either claim 1 or claim 2 wherein the group IVB element is titanium.
  4. 4. A superconducting material as claimed in claim 1 wherein the crystal comprises a solid solution series Mg2TiO4 - MgTi2O4.
  5. 5. A superconducting material as claimed in claim 1 comprising samples of composition Mg2~yTil+yO4 with average Ti valence x, x . (4-2y)/(y+l)
  6. 6. A superconducting material as claimed in claim 6 wherein the average valence of Ti is substantially equal to 3.3.
  7. 7. A method of making a superconductor material comprising the steps of mixing together appropriate quantities of an oxide of a group II metal, and oxide of a group IVB metal and a group IVB metal and forming pellets thereof, heating said pellets over a first time interval to an elevated temperature, holding said pellets at said elevated temperature for a second time interval and reducing said pellets to room temperature over a third time interval.
  8. 8. A method of making a superconductor material as claimed in claim 7 wherein said elevated temperature is 13500C.
  9. 9. A method of making a superconductor material as claimed in claim 8 wherein the first time interval is three hours.
  10. 10. A method of making a superconductor material as claimed in claim 8 wherein the second time interval is sixteen hours.
  11. 11. A method of making a superconductor material as claimed in claim 8 wherein the third time interval is four hours.
GB9119649A 1990-09-14 1991-09-13 Superconducting materials Expired - Fee Related GB2247883B (en)

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
GB909020115A GB9020115D0 (en) 1990-09-14 1990-09-14 Superconducting materials

Publications (3)

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GB9119649D0 GB9119649D0 (en) 1991-10-23
GB2247883A true GB2247883A (en) 1992-03-18
GB2247883B GB2247883B (en) 1994-10-05

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GB909020115A Pending GB9020115D0 (en) 1990-09-14 1990-09-14 Superconducting materials
GB9119649A Expired - Fee Related GB2247883B (en) 1990-09-14 1991-09-13 Superconducting materials

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EP (1) EP0549657A1 (en)
JP (1) JPH06503796A (en)
KR (1) KR930702246A (en)
FI (1) FI931147L (en)
GB (2) GB9020115D0 (en)
WO (1) WO1992005125A1 (en)

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0296893B1 (en) * 1987-03-28 1995-02-08 Sumitomo Electric Industries Limited Superconducting material and a process for preparing the same

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WO1992005125A1 (en) 1992-04-02
JPH06503796A (en) 1994-04-28
FI931147A7 (en) 1993-03-15
FI931147A0 (en) 1993-03-15
FI931147L (en) 1993-03-15
EP0549657A1 (en) 1993-07-07
GB9020115D0 (en) 1990-10-24
GB9119649D0 (en) 1991-10-23
GB2247883B (en) 1994-10-05
KR930702246A (en) 1993-09-08

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732 Registration of transactions, instruments or events in the register (sect. 32/1977)
PCNP Patent ceased through non-payment of renewal fee

Effective date: 19950913