Electrochemical catalytic reduction cell for the reduction of NO.sub.x in an O.sub.2 -containing exhaust emission

• US 5,401,372 A
• Filed: 04/26/1993
• Issued: 03/28/1995
• Est. Priority Date: 04/26/1993
• Status: Expired due to Fees

• Current Assignee: Ceramatec, Inc. (Trelleborg AB)
• Original Assignee: Ceramatec, Inc. (Trelleborg AB)
• Inventors: Liu, Meilin, Zhu, Jiemin, Joshin, Ashok V.
• Primary Examiner(s): GORGOS, KATHRYN L
• Application Number:
  US08/054,159
• Time in Patent Office: 701 Days
• Field of Search: 204/89 R, 204/252, 204/265, 204/266, 204/295, 204/290 R, 204/291, 204/292, 204/128, 204/129, 204/424, 204/426, 204/431
• US Class Current: 204/265
• CPC Class Codes: B01D 53/326 in electrochemical cells
• CPC Class Codes: B01D 53/8625 Nitrogen oxides
• CPC Class Codes: C25B 1/00 Electrolytic production of inorganic compounds or non-metals
• CPC Class Codes: C25B 9/23 comprising ion-exchange membranes in or on which electrode material is embedded
• CPC Class Codes: G01N 27/4074 for detection of gases other than oxygen

Abstract

Disclosed are a process and apparatus for removing NO_x in an O₂ -containing exhaust emission based on electrochemically catalytic reduction processes. Advantages to the electrochemically catalytic reduction process include high NO_x conversion efficiency and suitability for the removal of NO_x from the O₂ -containing exhaust of mobile combustion sources due to the simplicity in construction, maintenance and operation (chemical-reducing agents are not required in the process).

Claims

1. An electrochemical cell for reduction of NOx comprising:

(a) a solid electrolyte having sides;

(b) an anode on one side of the solid electrolyte;

(c) two layers on the side of the solid electrolyte opposite that of the anode, one of said layers is a porous oxide catalyst, and the other layer is an electron conducting layer, said electron conducting layer made from a material selected from the group consisting of lanthanum strontium manganate, lanthanum strontium manganese cobalt oxide, lanthanum strontium cobalt oxide, lanthanum strontium cobalt ferride, platinum and mixtures thereof; and

(d) a circuit that applies a potential across said anode and either said porous oxide catalyst or said electron conducting layer.

2. The electrochemical cell of claim 1 wherein said electron conducting layer is sandwiched between the solid electrolyte and the porous catalyst, and serves as a cathode.

3. The electrochemical cell of claim 1 wherein said porous catalyst is sandwiched between the solid electrolyte and the electron conducting layer, and serves as a cathode.

4. The electrochemical cell of claim 1 wherein said porous oxide catalyst is made from a material selected from the group consisting of (V₂ O₅)_x (TiO₂)_1-x, (V₂ O₅)_x (SiO₂)_1-x, (V₂ O₅)_x (γ

-Al₂ O₃)_1-x, CuO₂, SnO₂, NiO, Fe₃ O₄, Nb₂ O₅, lanthanum copper ferride, lanthanum strontium manganese copper ferride, Cu_x Mo₆ S₈, and mixtures thereof, wherein x is 0.01 to 0.99.

5. An electrochemical cell for nitrogen oxide reduction comprising:

a solid electrolyte having sides;

a metallic anode positioned on one side of said solid electrolyte;

a cathode positioned on the side of the solid electrolyte opposite that of the metallic anode, said cathode comprising a porous gas-diffusion catalyst; and

a conductive layer, comprising a perovskite oxide, positioned on the cathode to enhance the conductivity of the electrochemical cell and maintain the selective absorption of nitrogen oxide.

6. The electrochemical cell of claim 5 wherein said solid electrolyte is selected from the group consisting of an yttria-stabilized zirconia, stabilized zirconia, stabilized bismuthia, stabilized ceria, and mixtures thereof.

7. The electrochemical cell of claim 5 wherein said cathode is nonstoichiometric V₂ O₅.

8. The electrochemical cell of claim 5 wherein said anode is silver.

9. The electrochemical cell of claim 5 wherein said conductive layer comprises lanthanum strontium manganate.

10. A device for the electrochemical reduction of NO_x comprising:

(a) a container;

(b) an electrochemical cell, contained within said container, said electrochemical cell comprising;

(i) a solid electrolyte having sides,

(ii) a metallic anode positioned on one side of said solid electrolyte,

(iii) a cathode positioned on the side of the solid electrolyte opposite that of the metallic anode, said cathode comprising a porous gas-diffusion catalyst, and

(iv) a conductive layer positioned on the catalyst to enhance the conductivity of the electrochemical cell and maintain the selective absorption of nitrogen oxide;

(c) a gas inlet leading into said container, said gas inlet directed to the electrochemical cell;

(d) a porous metal grid surrounding said electrochemical cell;

(e) a power source for electrifying said porous metal grid and said cathode; and

(f) a gas outlet for removing gas from said container.

11. An electrochemical cell for reduction of NOx comprising:

(a) a solid electrolyte having sides;

(b) an anode on one side of the solid electrolyte;

(c) two layers on the side of the solid electrolyte opposite that of the anode, one of said layers is a porous oxide catalyst, said porous oxide catalyst made from a material selected from the group consisting of (V₂ O₅)_x (TiO₂)_1-x, (V₂ O₅)_x (SiO₂)_1-x, (V₂ O₅)_x (γ

-Al₂ O₃)_1-x, CuO₂, SnO₂, NiO, Fe₃ O₄, Nb₂ O₅, lanthanum copper ferride, lanthanum strontium manganese copper ferride, Cu_x Mo₆ S₈, and mixtures thereof, wherein x is 0.01 to 0.99, and the other layer is an electron conducting layer; and

(d) a circuit that applies a potential across said anode and either said porous oxide catalyst or said electron conducting layer.

12. The electrochemical cell of claim 11 wherein said electron conducting layer is sandwiched between the solid electrolyte and the porous catalyst, and serves as a cathode.

13. The electrochemical cell of claim 11 wherein said porous catalyst is sandwiched between the solid electrolyte and the electron conducting layer, and serves as a cathode.