CA1319639C - Method and apparatus using a solid electrolyte in the form of a disk for the separation or pumping of oxygen - Google Patents

Method and apparatus using a solid electrolyte in the form of a disk for the separation or pumping of oxygen

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Publication number
CA1319639C
CA1319639C CA000549920A CA549920A CA1319639C CA 1319639 C CA1319639 C CA 1319639C CA 000549920 A CA000549920 A CA 000549920A CA 549920 A CA549920 A CA 549920A CA 1319639 C CA1319639 C CA 1319639C
Authority
CA
Canada
Prior art keywords
disk
oxygen
solid electrolyte
feedstock
input
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Expired - Fee Related
Application number
CA000549920A
Other languages
French (fr)
Inventor
Jerry W. Suitor
Wilbur J. Marner
C. Martin Berdahl
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
California Institute of Technology CalTech
Original Assignee
California Institute of Technology CalTech
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Priority claimed from US06/923,160 external-priority patent/US4885142A/en
Application filed by California Institute of Technology CalTech filed Critical California Institute of Technology CalTech
Application granted granted Critical
Publication of CA1319639C publication Critical patent/CA1319639C/en
Anticipated expiration legal-status Critical
Expired - Fee Related legal-status Critical Current

Links

Classifications

    • Y02E60/366

Landscapes

  • Oxygen, Ozone, And Oxides In General (AREA)

Abstract

ABSTRACT

An apparatus in the form of a disk for the separation of oxygen from gases, or for the pumping of oxygen, uses a substantially circular disk geometry for the solid electrolyte with radial flow of gas from the outside edge of the disk to the center of the disk. The reduction in available surface area as the gas flows toward the center of the disk reduces the oxygen removal area proportionally to provide for a more uniform removal of oxygen.

Description

`" 1319639 Field of the Invention This invention relates to an apparatus for the separation and/or pumping of oxygen from a feedstock containing.
Background of the Invention Many, solid oxides, such as stabilized zirconia, behave like semiconductors except that instead of conducting electrons, they conduct oxygen ions. Previously used tubular and flat plate cell geometry arrangements for removing oxygen from oxygen-containing gas, or for pumping substantially pure oxygen streams, have had very uneven oxygen removal distributions or oxygen pumping efficiencies, due to electrical current mal-distribution over the cell.
This has resulted in excessive solid electrolyte requirements and excessive power consumption. Moreover, there, has been a tendency to damage the solid electrolyte due to over depletion of the oxygen-containing gas stream.
Summaxy of the Invention According to this invention, the solution to the foregoing problem lies in the use of substantially circular disk geometry for the solid electrolyte with radial flow of feed~tock gas frcm the outside edge of the disk to the center. The reduction in available surface area as the gas ~lows toward the center of the disk reduces the oxygen removal proportionally to provide for a more uniform removal o~ oxygen through the disk.
The uniqueness of the circular disk design is in the radial feedstock gas flow inward the center of the disk. As the gas flows towards the disk center, oxygen is removed.
The lower oxygen partial pressure causes an increase in the Nernst bucking voltage. With linear flow configurations such as a tube or square plate, the ,, . .-i.;.
, . ,~".

-` 1319~39 oxygen partial pressure drops quickly producing a high Nernst bucking voltage and therefore a high power consumption. The radial flow of the circular disk subjects the gas to a reduced active area as the flow moves toward the center. Therefore the oxygen removal rate is reduced and the partial pressure of oxygen does not drop as dramatically as with linear flow arrangements.
According to one form of the invention there is provided an apparatus for the separation and/or pumping of oxygen from feedstock containing oxygen, as defined herein which includes a disk of oxygen conductive solid electrolyte adapted to be contacted with electrode means to produce a flow of oxygen ions therethrough. Means are provided to flow the feedstock radially inwardly from the circumference of the disk.
According to the method aspect of the invention a disk of oxygen conductive solid electrolyte material is provided.
A feedstock containing oxygen is supplied to a peripheral portion of the disk and said feedstock is passed radially inwardly over the input surface of the disk. A current is applied to the disk in a manner such that oxygen is removed from said feedstock through said disk.
The term "feedstock containing oxygen" includes those feedatocks which include oxygen as a component, such as air and gaseous oxides, as well as substantially pure oxygen feedstocks. In the latter case, the inventive apparatus and method ~erves to pump oxygen.
It is an ob;ect of an aspect of this invention to provide an apparatus for separating oxygen from a feedstock containing oxygen. It is a further feature of this invention to provide a method and apparatus to pump oxygen.
Another feature of this invention is the provision of a method and apparatus to obtain oxygen from air.
A still further feature of this invention is the provision of a method and apparatus of the foregoing type that can be operated efficiently and economically.

Another feature of this invention is the provision of an apparatus of the foregoing type which can be constructed easily and operated reliably.
In attempting to provide an apparatus for the separation of oxygen and other gases, and for the pumping of oxygen, the various features of the invention were met by providing an apparatus as previously described wherein the prior art problems in utilizing a solid electrolyte were overcome to attain a unit operating at increased efficiency.
Description of the Drawinas The invention will be more fully understood with reference to the following drawings wherein:
Fig. 1 represents a cross-section elevation of one embodiment of the apparatus according to this invention;
Fig. 2 represents a view in perspective of one of the members of the apparatus shown in Fig. l;
Fig. 3 is a view in perspective showing an alternate embodiment of the apparatus of the invention, with parts thereof broken away for illustration purposes;
Fig. 4 i8 a ~ectional view taken on line 4-4 of Fig.
3 looking in the direction o~ the arrow;
Fig. 5 is a schematic view showing the axial current operation of the apparatus of Fig. 1;
Fig. 6 is a view similar to Fig. 5 showing the radial current operation of the apparatus of Fig. 3;
Fig. 7 is a schematic view showing an arrangement of four separate stacks of individual cells of the apparatus according to the invention;
Fig. 8 is a schematic view showing the layout of a system ~or producing oxygen using the apparatus according to the invention, and;
Fig. 9, which appears on the page of drawings containing Figure 4, is a schematic view showing a preferred electrical connection for the inventive apparatus.

~' ~3~ 3 9 DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS
Referring now to the drawings, and particularly to Fig. 1, there is shown therein a disk 10 of solid electrolyte that is adapted to be contacted with electrode means (to be hereinafter described) to produce a flow of oxygen ions 5 therethrough. Gas impervious side wall members extend circumferentially around both sides of disk 10 to define an input chamber 12 and an output chamber 13 on opposite sides thereof. A central core member 14 is provided having an output passage 15 therein with said core member 14 extending axially on both sides of said disk 10. Side wall member 11 includes at least 10 one feedstock passage 16 being in fluid communication with inlet chamber 12 through ports 17. Side wall member 11 further includes at least one oxygen outlet passage 18 in fluid communication with outlet chamber 13 via ports 19.
Second disk means are provided opposite disk 10 to provide end walls for the input chamber 12 and output chamber 13. Such second disk means 20 are of 15 an electronically conducting gas impervious material.
Input and output chambers 12 and 13 respectively, can be filled with a porous packing material 21 which is electronically conductive to serve as an electrode means for disk 10. The material 21 is porous or powdered ceramic material which can be fabricated from conductive rare earth oxides and it can 20 also be a sintered material. In a preferred form of the invention such rare earth oxide is selected from the group consisting of perovskites, pseudo perovskites and spinels. In a still further preferred form of the invention such rare earth oxide is a lanthanum-strontium-manganese oxide.
As best shown in Fig. 2, the side wall members 11 are formed as a solid 25 gas impervious ring, with feedstock passage 16 and oxygen outlet passage 18 formed as circular therethrough with outlet ports 17 serving to permit the entryof feedstock into input chamber 12. Offset 90 degrees in the embodiment shown are outlet passage 18, which, in the unit illustrated in Fig. 2, do not have fluid communication ports. It will be apparent to one skilled in the art, 30 that side wall member 10 can be used as a side wall for both input and outputchambers 12 and 13 by simply rotating the unit 90 degrees when it is used as a ~' - 131~39 side wall for an outlet chamber. Thus, the ports 17 will serve as input ports for inlet chamber 12 and for outlet ports 19 when the unit is rotated 90 degreesfor output chamber 13. While the configuration shown utilizes two ports 17 and 19 for each chamber, more passages and ports can be utilized to obtain 5 desired distribution.
Extensions 22 of side wall member 11 are adapted to inter~lt with recess 23 of the next adjoining such side wall member in interfitting substantially sealing relationship. Internal groove 24 is also provided to interf~t with second disk 20, again in substantially gas sealing relationship.
Core member 14 is provided with extension 25 which is adapted to mate with recess 26 in next adjoining core member 14. In a preferred form of the invention, core member 14 and disk 10 are formed as an integral unit.
As shown in Fig. 1, a number of the disk, side wall member and core units can be assembled in a manner such that they will be connected for 15 communication with incoming feedstock in parallel and electrically connected in series by means of the electrically conductive porous packing material 21 and second disk means 20.
In an alternate preferred embodiment according to the invention as shown in E~ig. 3 and Fig. 4, a plurality of disks of oxygen conductive solid 20 electrolyte material 30 are shown in an arrangement where individual cells including such disk are in a stack arrangement. In ~ig. 3, there are shown four disks 30 in the stack, however more disks could be utilized.
The arrangement in Fig. 3 includes a gas impervious top plate 31, intermediate plate 32 and a bottom plate 33. The plates are interfitted and 25 stacked together in a manner to form air inlets 34, oxygen depleted air outlet 35, and oxygen outlet 36. Formed on the respective sides of disks are input chamber 37 and output chamber 38. Input chamber 37 communicates through inlet conduit 39 which is in fluid communication with feedstock passage 34.
Output chamber 38 communicates through outlet conduit 40 which is in fluid 30 communication with output passage 36. Inlet chamber 37 is also in fluid ~ r ~

1319~39 communication wi~ second outlet conduit 41 which is in fluid comlnunication with oxygen depleted air outlet passage 35.
The passages 34, 35 and 36 are formed by manifold bushings 42 which are formed with flanges 43 and interfitting male and female connecting portions 44 and 45 respectively and internal bores 46 to form the respective passages.
Intermediate plates 32 are provided with inlet conduits 39, outlet conduits 40 and second outlet conduits 41, whereas top plate 31 is provided only with second outlet conduit 41 and bottom plate 33 is provided only with outlet conduit 40. In addition, top plate 31 is provided with a manifold bushing 42 for the purposes of installing a thermocouple chimney which is closed to gas flow by means of plug 47 or other suitable means.
Input chamber 37 and output chamber 38 are essentially circular cross-section being bounded by peripheral rings 48.
Circular disks 30 are mounted between the respective plates 31, 32 and 33 by means of platinum wire contact rings 49 which provide the electrical connection to the disks 30.
Inlet conduit 39 connects to circumferential plenum 50 which distributes the inlet feedstock around the periphery of inlet chamber 37 at a location substantially on the outer circumference of disk 30. Feedstock bleeds from the plenum 50 under ring 51 to enter input chamber 37.
It is preferred that the disks 10 and 30 be of circular con~;guration to achieve a more uniform oxygen removal by providing radial flow of gas front he outside edge of the disk towards its center. Thus, as air or oxygen enters inlet chamber 12 or 37 the gas proceeds radially toward the center of disk 10 or 30. The reduction in available surface area over disk 10 or 30 as the gas moves inwardly reduces the oxygen removal proportionally to provide for a more uniform removal of the oxygen from the feedstock. Substantially pure oxygen passing through disk 10 or 30 by electrodialysis flows through the apparatus to oxygen outlet passage 18 or 36 respectively.
Figs. 5 and 6 illustrate the mode of operation of apparatus of Figs. 1 and 3 respectively. Fig. 5 shows the axial current operation of the apparatus in 31~6~9 Fig. 1 wherein the porous packing materia1 electrode 21 distributes the electrons across the surface of disk 10 where they are directed through the diskin an axial direction. In Fig. 6, the current is distributed circumferentially around the edge of disk 30 by platinum wire contact rings 49, serving as S electrodes, and electrons are directed radially inwardly within disk 30.
ln Fig. 7, there is shown a plurality of stacks 52 of individual cells 53.
Each cell comprises a solid electrolyte disk 10 or 30 and the other components as described above to form the necessary input chambers and output chambers.
As shown in Fig. 7, the four stacks 52 and related hardware comprise a module 54 The stacks 52 are supplied with air ~rough supply air manifold 55 which coMects with feed stock passage 16 if the cells 53 are of the con~lguration shown in Figs. 1 and 2, or alternatively, feedstock passage 34 if the cells are of the configuration shown in Figs. 3 and 4. Oxygen manifold 56 is similarly connected oxygen outlet passage 18, as shown in Figs. 1 and 2 oxygen outlet passage 36 as shown in Figs. 3 and 4. Oxygen depleted air manifold 57 communicates with output passage 15 in the case of the ce11s of Figs. 1 and 2, or oxygen depleted air outlet 35 in the case of the cells of Figs. 3 and 4.
Electrical power is supplied to the module by electrical conduits 58. The power is distributed to each stack 51 by means of busher 59.
In Fig. 8, there is shown the layout for a system for producing oxygen from air using the module 54 of Fig. 7. The system includes air inlet 60, air blower 61 and conduit 62 which divides into conduit 63 to deliver the air to heat exchanger trains 64. In the heat exchanger 64, the air is preheated, extracting energy contained in gases exhausting from module 54. The air streams then pass through conduits 65 and are recombined and pass through furnace 66 which adds additional heat to permit operation at the desired elevated temperature. In module 54 itself, additional heat recovery will be made to absorb heat generated by ohmic heating in the module. After separation in the module, the oxygen depleted air and the oxygen flow by means of conduits 67 to heat exchanger train 64.

Referring now to Fig. 9, there is shown schematically electrical connection for the inventive apparatus wherein power is supplied to either platinum wire contact rings 49 or to porous electrode material 21. In the rearrangement shown, the cells 53 of a stack 52 are shown connected in series 5 to resu1t in identical current through each cell.
The invention may be embodied in other specific forms without departing from the spirit or essential characteristics thereof. The present embodiments are therefore to be considered in all respects as illustrative and not restrictive, the scope of the invention being indicated by the appended lO claims; and all changes which come within the meaning and range of equivalency of the claims are therefore intended to be embraced therein.

Claims (14)

1. An apparatus for the separation and/or pumping of oxygen from a feedstock containing oxygen comprising:
a. a disk of oxygen conductive solid electrolyte positioned such that an input side thereof is adapted to be in fluid contact with a feedstock containing oxygen and an output side thereof is in contact with an oxygen removal means, said disk being adapted to be contacted with electrodes to produce a flow of oxygen ions therethrough;
b. means to supply said feedstock containing oxygen to a peripheral portion of the input side of said disk; and, c. means to provide flow of said feedstock containing oxygen from points around the peripheral portion of said disk to a center portion thereof.
2. An apparatus according to Claim 1 further comprising oxygen depleted feedstock removal means located adjacent the input side of said solid electrolyte.
3. An apparatus according to Claim 1 further comprising an oxygen removal means located adjacent the output side of said solid electrolyte.
4. An apparatus according to Claim 1 comprising input and output chambers formed on the input and output sides of said disk.
5. An apparatus according to Claim 4 wherein said input and output chambers are formed with said disk and by top and bottom plate means respectively.
6. An apparatus according to Claim 5 wherein conduit means are incorporated in said top plate means to supply said feedstock to a peripheral section of the input side of said disk of solid electrolyte.
7. An apparatus according to claim 6 wherein said conduit means comprises a circumferential plenum located adjacent the periphery of said disk of solid electrolyte, said plenum being in fluid communication with said input chamber.
8. An apparatus according to Claim 5 comprising a plurality of said disks of solid electrolyte arranged to form a stack of cells.
9. An apparatus according to Claim 8 wherein at least one of said cells other than the top and bottom cells of said stack has said top and bottom plate means defined by a single gas impervious plate, said single gas impervious plate defining a top plate means for a cell in the stack and said plate also defining a bottom plate means for the next adjacent higher cell in the stack.
10. An apparatus according to Claim 1 further comprising electrode means positioned to contact said disk at the periphery thereof.
11. An apparatus according to Claim 2 further comprising electrode means in the form of an electronically conductive porous material spread over the input side of said disk.
12. A method of removing oxygen from a feedstock containing oxygen comprising:
a. providing a disk of oxygen conductive solid electrolyte material;

b. contacting a peripheral portion of said disk with a feedstock containing oxygen in a manner such that said feedstock moves radially inwardly from points around the periphery toward the center of said disk; and c. applying a current to said disk in a manner such that oxygen is removed from said feedstock containing oxygen through said disk to an output side thereof.
13. A method according to Claim 12 wherein said current is applied to the periphery of said disk whereby electrons are directed radially inwardly within said disk.
14. A method according to Claim 13 wherein said current is applied across the input surface of said disk whereby electrons are directed axially within said disk.
CA000549920A 1986-10-24 1987-10-22 Method and apparatus using a solid electrolyte in the form of a disk for the separation or pumping of oxygen Expired - Fee Related CA1319639C (en)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
US923,160 1986-10-24
US06/923,160 US4885142A (en) 1985-10-28 1986-10-24 Apparatus in the form of a disk for the separation of oxygen from other gases and/or for the pumping of oxygen and the method of removing the oxygen

Publications (1)

Publication Number Publication Date
CA1319639C true CA1319639C (en) 1993-06-29

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Family Applications (1)

Application Number Title Priority Date Filing Date
CA000549920A Expired - Fee Related CA1319639C (en) 1986-10-24 1987-10-22 Method and apparatus using a solid electrolyte in the form of a disk for the separation or pumping of oxygen

Country Status (1)

Country Link
CA (1) CA1319639C (en)

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