IP Library Granted Patent US 11,708,641
Granted Patent B2
US 11,708,641 · App. 17/393,151 · Granted Jul 25, 2023

Copper catalysts for electrochemical CO

Inventors: G. Tayhas R. Palmore (Providence, RI); Taehee Kim (Providence, RI)
Assignee: Brown University
C25F7/00C25B3/26C25B11/061C25D11/34C25D21/12C25F3/26
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Quick Facts
Patent No.
US 11,708,641
App. No.
17/393,151
Granted
Jul 25, 2023
Kind
B2
Abstract

An electrochemical method includes performing anodic halogenation of Cu foils, performing subsequent oxide-formation in a KHCO 3 electrolyte, and performing an electroreduction in neutral KHCO 3 to generate a copper catalyst.

Claims (22)

1. An electrochemical method comprising:

performing anodic halogenation of Cu foils; wherein the anodic halogenation comprises 60-100 s at 1.1 V (vs. Ag/AgCl) for KCI, 60-90 s at 0.18 V (vs. Ag/AgCl) for KBr, or 1-10 s at −0.2 V (vs. Ag/AgCl) for KI;

performing subsequent oxide-formation in a KHCO 3 electrolyte; and

performing an electroreduction in neutral KHCO 3 to generate a copper catalyst comprising cubic structures of Cu and a surface roughness of less than 30; the catalyst capable to provide a faradaic efficiency ≥50% for C 2 H 4 generation.

2. The electrochemical method of claim 1 wherein the electroreduction in neutral KHCO 3 is by linear sweep voltammetry (LSV).

3. The electrochemical method of claim 1 wherein performing anodic halogenation of Cu foils comprises applying an oxidative potential to electropolished Cu foils immersed in an electrolyte containing halide ions.

4. The electrochemical method of claim 1 , further comprising:

prior to performing the anodic halogenation of the Cu foils;

mechanically polishing the Cu foils;

rinsing the polished the Cu foils;

electropolishing the Cu foils by chronoamperometry in 85% phosphoric acid at 1.5 V with a Cu counter electrode in a two-electrode configuration;

rinsing the electropolished Cu foils;

cutting the electropolished Cu foils into 2×0.5 cm 2 pieces;

flattening the electropolished Cu foils;

covering a back side and part of a front side of the flattened electropolished Cu foils with polyimide (PI) tape to define a geometric area of a working electrode; and

wrapping the working electrode in PTFE tape to prevent detachment of the PI tape, exposing an area of 0.35 cm 2 .

5. The electrochemical method of claim 4 , further comprising:

dissolving KCl, KBr, and KI in de-ionized (DI) water to a concentration of 0.1 M; and

performing the anodic halogenation on an electropolished Cu foil immersed in 0.1 M KCl, KBr, and KI, respectively, in a three-electrode configuration using a potentiostat.

6. The electrochemical method of claim 5 wherein a counter electrode is Pt gauze.

7. The electrochemical method of claim 6 wherein a reference electrode was Ag/AgCl (saturated KCl) electrode.

8. The electrochemical method of claim 7 wherein open circuit potentials of electropolished Cu in 0.1 M KCl, KBr, and KI are −0.115 V, −0.134 V, and −0.315 V vs. Ag/AgCl.

Assignments (3)
CONFIRMATORY LICENSE Recorded Apr 1, 2025
From: BROWN UNIVERSITY
To: NATIONAL SCIENCE FOUNDATION
Reel/Frame 070691/0255 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Jun 2, 2023
From: KIM, TAEHEE
To: BROWN UNIVERSITY
Reel/Frame 063835/0438 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded May 17, 2023
From: PALMORE, G. TAYHAS R.
To: BROWN UNIVERSITY
Reel/Frame 063663/0924 →
Continuity (2)
Provisional Application 63060213 · Aug 3, 2020
Related Publication 20220042198A1 · Feb 10, 2022