IP Library Granted Patent US 11,668,012
Granted Patent B2
US 11,668,012 · App. 16/196,283 · Granted Jun 6, 2023

Methods for producing hydrocarbon products and hydrogen gas through electrochemical activation of methane

Inventors: Dong Ding (Idaho Falls, ID); Ting He (Idaho Falls, ID); Wei Wu (Idaho Falls, ID); Yunya Zhang (Idaho Falls, ID)
Assignee: Battelle Energy Alliance, LLC
C25B3/00C25B1/02C25B9/19C25B11/077C25B11/081C25B13/04
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Quick Facts
Patent No.
US 11,668,012
App. No.
16/196,283
Granted
Jun 6, 2023
Kind
B2
Abstract

A method of forming a hydrocarbon product and hydrogen gas comprises introducing CH 4 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 comprises 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. A potential difference is applied between the positive electrode and the negative electrode of the electrochemical cell to produce the hydrocarbon product and the hydrogen gas. A CH 4 activation system and an electrochemical cell are also described.

Claims (19)

1. A method of forming a hydrocarbon product and hydrogen gas, comprising:

introducing methane (CH 4 ) to a positive electrode of an electrochemical cell comprising:

the positive electrode, the positive electrode comprising a catalyst-doped material including composite particles individually comprising:

one of silicon dioxide (SiO 2 ) and silicon carbide (SiC); and

one or more of Ru, Rh, Ni, Ir, Mo, Zn, and Fe;

a negative electrode comprising an additional cermet material comprising nickel and one or more of a yttrium- and ytterbium-doped barium-zirconate-cerate (BZCYYb) and a yttrium- and ytterbium-doped barium-strontium-niobate (BSNYYb); and

a proton-conducting membrane between the positive electrode and the negative electrode and comprising one or more of further BZCYYb and further BSNYYb, the proton-conducting membrane 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.; and

applying a potential difference between the positive electrode and the negative electrode of the electrochemical cell while the CH 4 interacts with the positive electrode so that hydrogen (H) atoms of the CH 4 release electrons (e − ) to produce methyl radicals (CH 3 + ), hydrogen ions (H + ), and the e − through non-oxidative deprotonation of the CH 4 at the one or more temperatures.

2. The method of claim 1 , further comprising selecting the proton-conducting membrane to comprise the further BSNYYb.

3. The method of claim 1 , wherein the composite particles individually comprise one of:

Fe and SiO 2 (Fe@SiO 2 );

Mo and SiO 2 (Mo@SiO 2 );

Fe and SiC (Fe@SiC); and

Mo and SiC (Mo@SiC).

4. The method of claim 3 , wherein the composite particles individually comprise the Fe@SiO 2 .

5. The method of claim 1 , further comprising selecting the proton-conducting membrane to comprise the further BZCYYb, the further BZCYYb comprising BaZr 0.3 Ce 0.5 Y 0.1 Yb 0.1 O 3-δ .

6. The method of claim 1 , further comprising selecting the proton-conducting membrane such that the proton-conducting membrane substantially intervenes between opposing surfaces of the positive electrode and the negative electrode.

7. The method of claim 1 , wherein introducing CH 4 to the positive electrode of the electrochemical cell comprises introducing one or more fluid streams comprising the CH 4 to the positive electrode of the electrochemical cell.

8. The method of claim 1 , further comprising selecting the proton-conducting membrane to be substantially homogeneous.

Assignments (2)
CONFIRMATORY LICENSE Recorded Apr 28, 2020
From: BATTELLE ENERGY ALLIANCE/IDAHO NAT'L LAB
To: UNITED STATES DEPARTMENT OF ENERGY
Reel/Frame 052510/0735 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Nov 20, 2018
From: DING, DONG; HE, TING; WU, WEI; ZHANG, YUNYA
To: BATTELLE ENERGY ALLIANCE, LLC
Reel/Frame 047553/0445 →
Continuity (2)
Provisional Application 62597004 · Dec 11, 2017
Related Publication 20190177861A1 · Jun 13, 2019