IP Library › Granted Patent US 11,512,011
Granted Patent B2
US 11,512,011 · App. 16/326,300 · Granted Nov 29, 2022

Methods and systems for electrochemical oxidation of polyfluoroalkyl and perfluroalkyl contaminants

Inventors: Qingguo Huang (Fayetteville, GA); Hui Lin (Griffin, GA); Junfeng Niu (Griffin, GA)
Assignee: University of Georgia Research Foundation, Inc.
C02F1/4672C02F1/463C02F1/46114C25B11/031H01M4/0433H01M4/664C02F1/444C02F2001/46133C02F2001/46138C02F2001/46161C02F2001/46171C02F2101/14C02F2101/36C02F2103/001C02F2103/06C02F2103/36
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Quick Facts
Patent No.
US 11,512,011
App. No.
16/326,300
Granted
Nov 29, 2022
Kind
B2
Abstract

The present disclosure provides methods, electrodes, and systems for electrochemical oxidation of polyfluoroalkyl and perfluroalkyl (PFAS) contaminants using Magnéli phase titanium suboxide ceramic electrodes/membranes. Magneli phase titanium suboxide ceramic electrodes/membranes can be porous and can be included in reactive electrochemical membrane filtration systems for filtration, concentration, and oxidation of PFASs and other contaminants.

Claims (24)

1. A method for electrochemically oxidizing polyfluoroalkyl and perfluoroalkyl substances (PFASs), the method comprising:

contacting an aqueous composition contaminated with one or more types of PFASs with a Magnéli phase titanium oxide ceramic electrode comprising one or more Magnéli phase titanium sub-oxides wherein at least one of the Magnéli phase titanium sub-oxides is Ti 4 O 7 or Ti 5 O 9 ; and

supplying electric current to the Magnéli phase titanium oxide ceramic electrode in an electrochemical cell, whereby the electrode electrochemically oxidizes the PFASs to oxidatively degrade the PFASs into mineral components, inorganic components, or both, wherein the one or more types of PFASs comprise at least one type of perfluoroalkyl acid (PFAA).

2. The method of claim 1 , wherein the Magnéli phase titanium oxide ceramic electrode comprises T 4 O 7 or a combination of Ti 4 O 7 and Ti 5 O 9 .

3. The method of claim 1 , wherein the composition contaminated with PFASs comprises wastewater and the method further comprises pre-treating the wastewater to concentrate the PFASs prior to contact with the Magnéli phase titanium oxide ceramic electrode.

4. The method of claim 3 , wherein the wastewater is pre-treated via electrocoagulation to concentrate the PFASs.

5. The method of claim 2 , wherein the Magnéli phase titanium oxide ceramic electrode comprises a plurality of micropores.

6. The method of claim 5 , wherein the plurality of micropores have a diameter from about 10 nm to 10 μm.

7. The method of claim 5 , wherein the Magnéli phase titanium oxide ceramic electrode has a porosity of about 5-75%.

8. The method of claim 1 , wherein the at least one type of PFAA is selected from: perfluorooctanoate (PFOA), perfluorooctanesulfonate (PFOS) or a combination thereof.

9. The method of claim 1 , wherein the composition contaminated with PFASs comprises contaminated wastewater, and the method further comprises:

producing at least partially decontaminated wastewater after contact with the Magnéli phase titanium oxide ceramic electrode electrochemically oxidizes the PFASs.

10. The method of claim 9 , further comprising recycling the at least partially decontaminated wastewater.

11. The method of claim 1 , wherein the Magnéli phase titanium oxide ceramic electrode comprises a plurality of pores and serves as both an anode and a membrane in a reactive electrochemical membrane (REM) filtration system.

12. The method of claim 1 , wherein the at least one type of PFAA is selected from: a perfluoroalkyl carboxylic acid (PFCA), a perfluoroalkyl sulfuric acid (PFSA), or a combination thereof.

13. The method of claim 1 , wherein the at least one type of PFAA comprises at least one perfluoroalkyl sulfuric acid (PFSA).

14. A method for electrochemically oxidizing polyfluoroalkyl and perfluoroalkyl substances (PFASs), the method comprising:

contacting an aqueous composition contaminated with one or more types of PFASs with an electrochemical cell comprising a first Magnéli phase titanium oxide ceramic membrane electrode configured to serve as an anode and a second Magnéli phase titanium oxide ceramic membrane electrode configured to serve as a cathode, wherein the first and second Magnéli phase titanium oxide ceramic membrane electrodes each comprise one or more Magnéli phase titanium sub-oxides wherein at least one of the Magnéli phase titanium sub-oxides is Ti 4 O 7 or Ti 5 O 9 ; and

supplying electric current to the electrochemical cell such that the first Magnéli phase titanium oxide ceramic membrane electrode electrochemically oxidizes the PFASs to oxidatively degrade the PFASs into mineral components, inorganic components, or both, and the second Magnéli phase titanium oxide ceramic membrane electrode serves as the cathode.

15. The method of claim 14 , wherein the cathode reduces chlorate to Cl − .

16. A method for electrochemically oxidizing polyfluoroalkyl and perfluoroalkyl substances (PFASs), the method comprising:

contacting an aqueous composition contaminated with one or more types of PFASs and trichloroethylene (TCE) with an electrochemical cell comprising a first Magnéli phase titanium oxide ceramic electrode configured to serve as an anode and a second Magnéli phase titanium oxide ceramic membrane electrode configured to serve as a cathode, wherein the first and second Magnéli phase titanium oxide ceramic membrane electrodes each comprise one or more Magnéli phase titanium sub-oxides wherein at least one of the Magnéli phase titanium sub-oxides is Ti 4 O 7 or Ti 5 O 9 and wherein each electrode has at least a portion of the electrode coated with activated carbon fiber (ACF); and

supplying electric current to the electrochemical cell such that the first Magnéli phase titanium oxide ceramic membrane electrode electrochemically oxidizes the PFASs to oxidatively degrade the PFASs into mineral components, inorganic components, or both, and the second Magnéli phase titanium oxide ceramic membrane electrode serves as the cathode and reduces chlorate to Cl − .

17. The method of claim 16 , wherein the first and second Magnéli phase titanium oxide ceramic electrodes have a tubular shape.

Assignments (3)
CORRECTIVE ASSIGNMENT TO CORRECT THE FIRST INVENTOR'S NAME PREVIOUSLY RECORDED AT REEL: 049101 FRAME: 0304. ASSIGNOR(S) HEREBY CONFIRMS THE ASSIGNMENT . Recorded Jan 24, 2023
From: HUANG, QINGGUO; LIN, HUI; NIU, JUFENG
To: UNIVERSITY OF GEORGIA RESEARCH FOUNDATION, INC.
Reel/Frame 062490/0111 →
CONFIRMATORY LICENSE Recorded Nov 7, 2022
From: UNIVERSITY OF GEORGIA
To: NATIONAL INSTITUTES OF HEALTH (NIH), U.S. DEPT. OF HEALTH AND HUMAN SERVICES (DHHS), U.S. GOVERNMENT
Reel/Frame 061885/0910 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded May 7, 2019
From: HONG, QINGGUO; LIN, HUI; NIU, JUFENG
To: UNIVERSITY OF GEORGIA RESEARCH FOUNDATION, INC.
Reel/Frame 049101/0304 →
Continuity (2)
Provisional Application 62377120 · Aug 19, 2016
Related Publication 20190185351A1 · Jun 20, 2019
Cited By (12)
US 12,215,044 US 12,240,772 US 12,275,661 US 12,304,850 US 12,351,492 US 12,351,498 US 12,473,222 US 12,492,137 US 12,515,974 US 12,534,390 US 12,545,601 US 12,655,051