Methods for co-producing hydrocarbon products and ammonia

Patent metadata

Field	Value
Publication number	US-11731920-B2
Application number	US-201916532276-A
Country	US
Kind code	B2
Filing date	Aug 5, 2019
Priority date	Aug 6, 2018
Publication date	Aug 22, 2023
Grant date	Aug 22, 2023

Abstract

A method of a hydrocarbon product and ammonia comprises introducing C2H6 to a positive electrode of an electrochemical cell comprising the positive electrode, a negative electrode, and a proton-conducting membrane between the positive electrode and the negative electrode. The proton-conducting membrane comprising an electrolyte material having an ionic conductivity greater than or equal to about 10−2 S/cm at one or more temperatures within a range of from about 150° C. to about 600° C. N2 is introduced to the negative electrode of the electrochemical cell. A potential difference is applied between the positive electrode and the negative electrode of the electrochemical cell. A system for co-producing higher hydrocarbons and NH3, and an electrochemical cell are also described.

First claim

What is claimed is:

1. A method of forming a hydrocarbon product and ammonia, comprising:
introducing ethane (C 2 H 6 ) to a positive electrode of an electrochemical cell comprising:
the positive electrode;
a negative electrode comprising one or more of a Ru/perovskite cermet, a RuNi/perovskite cermet, a RuCe/perovskite cermet, and a RuNiCe/perovskite cermet; and
a proton-conducting membrane between the positive electrode and the negative electrode, the proton-conducting membrane comprising an electrolyte material having an ionic conductivity greater than or equal to about 10 −2 S/cm at one or more temperatures within a range of from about 150° C. to about 600° C.;

introducing N 2 to the negative electrode of the electrochemical cell; and
applying a potential difference between the positive electrode and the negative electrode of the electrochemical cell while the C 2 H 6 interacts with the positive electrode so that hydrogen (H) atoms of the C 2 H 6 release electrons (e − ) to produce C 2 H 4 , hydrogen ions (H + ), and the e − at the positive electrode through non-oxidative deprotonation of the C 2 H 6 at the one or more temperatures, to transport the H + through the proton-conducting membrane, and to produce NH 3 at the negative electrode.

2. The method of claim 1 , further comprising selecting the proton-conducting membrane to comprise at least one perovskite material having a H + conductivity greater than or equal to about 10 −2 S/cm at one or more temperatures within a range of from about 400° C. to about 600° C.

3. The method of claim 2 , wherein selecting the proton-conducting membrane to comprise at least one perovskite material comprises selecting the at least one perovskite material to comprise one or more of a yttrium- and ytterbium-doped barium-zirconate-cerate (BZCYYb), a yttrium- and ytterbium-doped barium-strontium-niobate (BSNYYb), yttrium-doped BaCeO 3 , yttrium-doped BaZrO 3 , Ba 2 (YSn)O 5.5 , and Ba 3 (CaNb 2 )O 9 .

4. The method of claim 1 , further comprising selecting the proton-conducting membrane to comprise one or more of a yttrium- and ytterbium-doped barium-zirconate-cerate (BZCYYb), and a yttrium- and ytterbium-doped barium-strontium-niobate (BSNYYb).

5. The method of claim 1 , further comprising selecting the proton-conducting membrane to comprise a yttrium- and ytterbium-doped barium-zirconate-cerate (BZCYYb).

6. The method of claim 1 , further comprising selecting the proton-conducting membrane to comprise a yttrium- and ytterbium-doped barium-strontium-niobate (BSNYYb).

7. The method of claim 1 , further comprising selecting the proton-conducting membrane to comprise Ba 2 (YSn)O 5.5 .

8. The method of claim 1 , further comprising selecting the proton-conducting membrane to comprise Ba 3 (CaNb 2 )O 9 .

9. The method of claim 1 , further comprising selecting the negative electrode to comprise the Ru/perovskite cermet, the Ru/perovskite cermet selected from a Ru/yttrium- and ytterbium-doped barium-zirconate-cerate (Ru-BZCYYb) cermet and a Ru/yttrium- and ytterbium-doped barium-strontium-niobate (Ru-BSNYYb) cermet.

10. The method of claim 1 , further comprising selecting the negative electrode to comprise the RuNi/perovskite cermet, the RuNi/perovskite cermet selected from a RuNi/yttrium- and ytterbium-doped barium-zirconate-cerate (RuNi-BZCYYb) cermet and a RuNi/yttrium- and ytterbium-doped barium-strontium-niobate (RuNi-BSNYYb) cermet.

11. The method of claim 10 , wherein catalyst material of the RuNi/perovskite cermet comprises one or more of:
RuNi alloy particles; and
composite particles individually comprising:
a core comprising one of Ru, Ni, and an RuNi alloy; and
a shell partially coating the core and having a different material composition than the core, the shell comprising one other of the Ru, the Ni, and the RuNi alloy.

12. The method of claim 1 , further comprising selecting the negative electrode to comprise the RuCe/perovskite cermet, the RuCe/perovskite cermet selected from a RuCe/yttrium- and ytterbium-doped barium-zirconate-cerate (RuCe-BZCYYb) cermet and a RuCe/yttrium- and ytterbium-doped barium-strontium-niobate (RuCe-BSNYYb) cermet.

13. The method of claim 12 , wherein catalyst material of the RuCe/perovskite cermet comprises one or more of:
RuCe alloy particles; and
composite particles individually comprising:
a core comprising one of Ru, Ce, and a RuCe alloy; and
a shell partially coating the core and having a different material composition than the core, the shell comprising one other of the Ru, the Ce, and the RuCe alloy.

14. The method of claim 1 , further comprising selecting the negative electrode to comprise the RuNiCe/perovskite cermet, the RuNiCe/perovskite cermet selected from a RuNiCe/yttrium- and ytterbium-doped barium-zirconate-cerate (RuNiCe-BZCYYb) cermet and a RuNiCe/yttrium- and ytterbium-doped barium-strontium-niobate (RuNiCe-BSNYYb) cermet.

15. The method of claim 14 , wherein catalyst material of the RuNiCe/perovskite cermet comprises one or more of:
RuNiCe alloy particles; and
composite particles individually comprising Ru, Ni, and Ce.

Assignees

• Battelle Energy Alliance Llc

Inventors

• Ding Dong
• Wu Wei
• Ding Hanping
• Hua Bin

Classifications

• C07C2/24 Primary

  with metals · CPC title

• B01J31/26

  containing in addition, inorganic metal compounds not provided for in groups B01J31/02 - B01J31/24 · CPC title

• C01C1/0411 Primary

  characterised by the catalyst · CPC title

• C25B1/27

  Ammonia · CPC title

• C25B3/03

  Acyclic or carbocyclic hydrocarbons · CPC title