IP Library Granted Patent US 9,269,963
Granted Patent B2
US 9,269,963 · App. 13/884,571 · Granted Feb 23, 2016

Solid oxide cell stack and method for preparing same

Inventors: Peter Vang Hendriksen (Hillerød, DK); Lars Mikkelsen (Rødovre, DK); Martin Søgaard (Ringe, DK); Jens Valdemar Thorvald Høgh (Copenhagen K, DK); Wolff-Ragnar Kiebach (Copenhagen N, DK); Kresten J. N. L. Jensen (Hillerød, DK)
Assignees: Technical University of Denmark; Haldor Topsoe A/S
H01M4/8846C25B9/00H01M4/9016H01M8/2425H01M2008/1293Y02E60/50Y02E60/525
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Quick Facts
Patent No.
US 9,269,963
App. No.
13/884,571
Granted
Feb 23, 2016
Kind
B2
Abstract

A method for producing and reactivating a solid oxide cell stack structure by providing a catalyst precursor in at least one of the electrode layers by impregnation and subsequent drying after the stack has been assembled and initiated. The method includes impregnating a catalyst precursor into a cathode of a solid oxide cell stack which already contains an active material (an anode reduction) for example, in the form of Ni/YSZ anodes. Due to a significantly improved performance and an unexpected voltage improvement this solid oxide cell stack structure is particularly suitable for use in solid oxide fuel cell (SOFC) and solid oxide electrolysing cell (SOEC) applications.

Claims (26)

1. A method for producing a solid oxide cell stack comprising an internal manifold, an external manifold or a combination of both, the method comprising the steps of:

assembling the solid oxide cell stack by arranging a plurality of single solid oxide cells into a stack, each of the plurality of single solid oxide cells containing electrode layers separated by an electrolyte layer;

initiating the solid oxide cell stack by undergoing anode reduction; and the method further comprising the steps of:

(a) impregnating a catalyst precursor into only a cathode of the solid oxide cell stack by introducing a solution of the catalyst precursor via the internal or external manifold, and

(b) subsequently drying the solution of the catalyst precursor,

wherein steps (a) and (b) are conducted at least once after the solid oxide cell stack has been assembled and initiated so that the electrode layers become catalytically active.

2. Method according to claim 1 , wherein the cathode in step (a) is already active.

3. Method according to claim 1 , in which catalytic active material is provided in at least one of the electrode layers of each of the plurality of single solid oxide cells via a ceramic processing technique or by an impregnation with the catalyst precursor before the solid oxide cell stack has been initiated.

4. Method according to claim 1 , comprising impregnating the catalyst precursor by means of pouring or pumping the solution of the catalyst precursor through the manifolds of the stack.

5. Method according to claim 1 , comprising providing a vacuum to the solid oxide cell stack prior to the step of subsequently drying the solution of the catalyst precursor.

6. Method according to claim 1 , comprising drying the solution of the catalyst precursor by blowing air through the stack or heating the stack at 100° C. or higher.

7. Method according to claim 1 , wherein the catalyst precursor is selected from the group of (La 1-x Sr x )MnO 3-δ , (Ln 1-x Sr x )MnO 3-δ , (Ln 1-x Sr x )Fe 1-y Co y O 3δ , (Y 1-x Ca x )Fe 1-y Co y O 3-δ , (Gd 1-x Sr x )Fe 1-y Co y O 3-δ , (Gd 1-X Ca x )Fe 1-y Co y O 3-δ (Y,Ca)Fe 1-y Co y O 3-δ , ceria, doped ceria, zirconia, doped zirconia, La(Ni,Fe)O 3 , La(Ni,Co)O 3 , La 2 NiO 4 , Ln 1-x AE 2x TmO 4 , where TM is a transition metal, Ln is a lanthanide element and AE is an alkali earth element, Pr 2 O 3 ; and mixtures thereof, and where 0≦x≦1; 0≦y≦1; and 0≦δ≦0.3.

8. A method for reactivating a solid oxide cell stack comprising an internal manifold, an external manifold or a combination of both, the method comprising the steps of:

assembling the solid oxide cell stack by arranging a plurality of single solid oxide cells into a stack, each of the plurality of single solid oxide cells containing electrode layers separated by an electrolyte layer;

initiating the solid oxide cell stack by undergoing anode reduction; and

subsequently, reactivating the solid oxide cell stack by

(a) impregnating a catalyst precursor into only a cathode of the solid oxide cell stack by introducing a solution of the catalyst precursor via the internal or external manifold, and

(b) subsequently drying the solution of the catalyst precursor,

wherein steps (a) and (b) are conducted at least once after the solid oxide cell stack has been assembled and initiated so that the electrode layers become catalytically active.

9. Method according to claim 8 , wherein the cathode in step (a) is already active.

10. Method according to claim 8 , in which catalytic active material is provided in at least one of the electrode layers of each of the plurality of single solid oxide cells via a ceramic processing technique or by an impregnation with the catalyst precursor before the solid oxide cell stack has been initiated.

11. Method according to claim 8 , comprising impregnating the catalyst precursor in step (a) by means of pouring or pumping the solution of the catalyst precursor through the manifolds of the stack.

12. Method according to claim 8 , comprising drying the solution of the catalyst precursor in step (b) by blowing air through the stack or heating the stack at 200° C. or higher.

13. Method according to claim 1 , wherein the catalyst precursor is selected from MgO, CaO, Al 2 O 3 /MgO, CaZrO 3 , SrZrO 3 , BaZrO 3 , CaO, SrO, BaO or the carbonates SrCO 3 , CaCO 3 or BaCO 3 .

14. Method according to claim 13 , wherein the catalyst precursor is provided as an aqueous solution of ceria.

15. Method according to claim 14 , wherein the aqueous solution contains a solvent and a surfactant.

Assignments (4)
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Aug 13, 2024
From: THE TECHNICAL UNIVERSITY OF DENMARK
To: TOPSOE A/S
Reel/Frame 068261/0412 →
CHANGE OF NAME Recorded Oct 3, 2023
From: HALDOR TOPSØE A/S
To: TOPSOE A/S
Reel/Frame 065108/0028 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Nov 26, 2014
From: TOPSOE FUEL CELL A/S
To: HALDOR TOPSOE A/S
Reel/Frame 034270/0044 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded May 9, 2013
From: HENDRIKSEN, PETER VANG; MIKKELSEN, LARS; SOGAARD, MARTIN; HOGH, JENS VALDEMAR THORVALD; KIEBACH, WOLFF-RAGNAR; JENSEN, KRESTEN J.N.L.
To: THE TECHNICAL UNIVERSITY OF DENMARK; TOPSOE FUEL CELL A/S
Reel/Frame 030388/0301 →
Continuity (1)
Related Publication 20130224620A1 · Aug 29, 2013