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US-20260124586-A1 - DURABLE GRAPHENE OXIDE MEMBRANES

US20260124586A1US 20260124586 A1US20260124586 A1US 20260124586A1US-20260124586-A1

Abstract

Embodiments described herein relate generally to durable graphene oxide membranes for fluid filtration. For example, the graphene oxide membranes can be durable under high temperatures non-neutral pH, and/or high pressures. One aspect of the present disclosure relates to a filtration apparatus comprising: a support substrate, and a graphene oxide membrane disposed on the support substrate. The graphene oxide membrane has a first lactose rejection rate of at least 50% with a first 1 wt % lactose solution at room temperature. The graphene oxide membrane has a second lactose rejection rate of at least 50% with a second 1 wt % lactose solution at room temperature after the graphene oxide membrane is contacted with a solution that is at least 80° C. for a period of time.

Inventors

  • Stephen Frayne
  • Michelle MacLeod
  • Brandon Ian MACDONALD
  • Lymaris ORTIZ RIVERA
  • Brent D. KELLER

Assignees

  • VIA SEPARATIONS, INC.

Dates

Publication Date
20260507
Application Date
20250612

Claims (20)

  1. 1 . A filtration apparatus, comprising: a support substrate; and a graphene oxide membrane disposed on the support substrate, the graphene oxide membrane including a plurality of graphene oxide sheets, each of the graphene oxide sheets covalently coupled to a chemical spacer, wherein: the graphene oxide membrane has a first lactose rejection rate of at least 50% with a first 1 wt % lactose solution at room temperature; and after the graphene oxide membrane is contacted with a solution that is at least 80° C. for a period of time, the graphene oxide membrane has a second lactose rejection rate of at least 50% with a second 1 wt % lactose solution at room temperature.
  2. 2 . The filtration apparatus of claim 1 , wherein the second lactose rejection rate is substantially the same as the first lactose rejection rate.
  3. 3 . The filtration apparatus of claim 1 , wherein the second lactose rejection rate is greater than the first lactose rejection rate.
  4. 4 . The filtration apparatus of claim 3 , wherein the first lactose rejection rate is less than or equal to 90%.
  5. 5 . The filtration apparatus of any one of claim 4 , wherein the second lactose rejection rate is less than or equal to 90%.
  6. 6 . The filtration apparatus of any one of claim 5 , wherein each of the graphene oxide sheets is not covalently crosslinked to the adjacent graphene oxide sheet.
  7. 7 . The filtration apparatus of any one of claim 6 , wherein the chemical spacer comprises an amine or a derivative thereof.
  8. 8 . The filtration apparatus of claim 7 , wherein the chemical spacer comprises —NH—R 1 , wherein R 1 is an aryl, which can be optionally substituted.
  9. 9 . The filtration apparatus of claim 7 , wherein the chemical spacer comprises —NH—C(O)—R 2 , wherein R 2 is C 1 -C 6 alkyl or C 2 -C 6 alkenyl, each of which can be optionally substituted.
  10. 10 . The filtration apparatus of claim 7 , wherein the amine is 4-aminophenylacetic acid or 2-(4-aminophenyl) ethanol.
  11. 11 . The filtration apparatus of any one of claim 6 , wherein the chemical spacer comprises an amide or a derivative thereof.
  12. 12 . The filtration apparatus of claim 11 , wherein the amide is acrylamide, propionamide, isobutyramide, or pivalamide.
  13. 13 . The filtration apparatus of any one of claim 12 , wherein the solution has a pH of about 7.
  14. 14 . The filtration apparatus of any one of claim 12 , wherein the solution has a pH of about 11.
  15. 15 . The filtration apparatus of any one of claim 12 , wherein the solution has a pH of about 14.
  16. 16 . The filtration apparatus of claim 15 , wherein the solution is a phosphate buffer.
  17. 17 . The filtration apparatus of claim 16 , wherein the phosphate buffer comprises Na 2 HPO 4 .
  18. 18 . The filtration apparatus of claim 17 , wherein the graphene oxide membrane is contacted with the solution at less than or equal to 100° C.
  19. 19 . The filtration apparatus of claim 18 , wherein the room temperature is about 20° C.
  20. 20 . The filtration apparatus of claim 19 , wherein the solution passes through the graphene oxide membrane.

Description

RELATED APPLICATIONS This application is a continuation of U.S. patent application Ser. No. 17/960,440, filed Oct. 5, 2022, and titled DURABLE GRAPHENE OXIDE MEMBRANES, which is a continuation of U.S. patent application Ser. No. 17/380,566, filed Jul. 20, 2021, and titled DURABLE GRAPHENE OXIDE MEMBRANES, now U.S. Pat. No. 11,498,034, which is a continuation of U.S. patent application Ser. No. 16/887,555, filed May 29, 2020, and titled DURABLE GRAPHENE OXIDE MEMBRANES, now U.S. Pat. No. 11,097,227, which is a continuation of International Patent Application No. PCT/US2020/033246, filed May 15, 2020, and titled DURABLE GRAPHENE OXIDE MEMBRANES, which claims priority to and the benefit of U.S. Provisional Patent Application No. 62/848,014, filed on May 15, 2019, and U.S. Provisional Patent Application No. 62/910,789, filed on Oct. 4, 2019, the disclosures of which are hereby incorporated by reference in their entireties. TECHNICAL FIELD The present disclosure relates generally to graphene oxide membranes and their use in separation processes. BACKGROUND Membranes can be used to separate a mixture by passing some components (filtrate or permeate) and retaining others preferentially with a balance of the mixture (rejects) according to any of a variety of properties of the membrane and/or of the components of the material being filtered. For example, membranes can be configured to separate rejects from a filtrate based on size exclusion (i.e., a physical barrier such as pores that are smaller than the excluded particles). Other examples include membranes that are configured to separate rejects from a filtrate based on chemical, electrochemical, and/or physical binding with one or more components of the material being filtered. Polymer membranes are a common type of membrane. They have been used commercially for water softening, desalination, and for the concentration, removal, and purification of different salts, small molecules, and macromolecules. However, in certain environments (e.g., oxidizing conditions, high pH, high temperatures, or in some solvents), polymer membranes can become damaged or fail due to swelling, oxidation reactions, degradation, or softening of the polymer. Accordingly, there is a need in the art for new membranes that address one or more deficiencies of polymer membranes. SUMMARY Embodiments described herein relate generally to durable graphene oxide membranes for fluid filtration. For example, the graphene oxide membranes can be used for concentration, removal, and purification of different salts. For the membranes described herein, each of the graphene oxide sheets is not covalently crosslinked to the adjacent graphene oxide sheet. One aspect of the present disclosure relates to a filtration apparatus comprising: a support substrate, and a graphene oxide membrane disposed on the support substrate. The graphene oxide membrane includes a plurality of graphene oxide sheets, each of the graphene oxide sheets covalently coupled to a chemical spacer. The graphene oxide membrane has a first lactose rejection rate of at least 50% with a first 1 wt % lactose solution at room temperature. The graphene oxide membrane has a second lactose rejection rate of at least 50% with a second 1 wt % lactose solution at room temperature after the graphene oxide membrane is contacted with a solution that is at least 80° C. for a period of time. In some embodiments, the second lactose rejection rate is substantially the same as the first lactose rejection rate. In some embodiments, the second lactose rejection rate is greater than the first lactose rejection rate. In some embodiments, the first lactose rejection rate is less than or equal to 90%. In some embodiments, the second lactose rejection rate is less than or equal to 90%. In some embodiments, the chemical spacer comprises an amine or a derivative thereof. In some embodiments, the chemical spacer comprises —NH—R1, wherein R1 is an aryl, which can be optionally substituted. In some embodiments, the amine is 4-aminophenylacetic acid or 2-(4-aminophenyl) ethanol. In some embodiments, the chemical spacer comprises an amide or a derivative thereof. In some embodiments, the chemical spacer comprises —NH—C(O)—R2, wherein R2 is C1-C6 alkyl or C2-C6 alkenyl, each of which can be optionally substituted. In some embodiments, the amide is acrylamide, propionamide, isobutyramide, or pivalamide. In some embodiments, the solution has a pH of about 7. In some embodiments, the solution has a pH of about 11. In some embodiments, the solution has a pH of about 14. In some embodiments, the solution is a phosphate buffer. In some embodiments, the phosphate buffer comprises Na2HPO4. In some embodiments, the room temperature is about 20° C. In some embodiments, the solution passes through the graphene oxide membrane. In some embodiments, the period of time is about 2-6 hours. One aspect of the present disclosure relates to a filtration apparatus comprising: a support substra