IP Library Granted Patent US 10,525,424
Granted Patent B2
US 10,525,424 · App. 15/541,260 · Granted Jan 7, 2020

Zwitterionic copolymers for fouling resistant filtration membranes

Inventors: Ayse Asatekin Alexiou (Arlington, MA); Papatya Kaner (Cambridge, MA); Chiara Vannucci (Medford, MA)
Assignee: Trustees of Tufts College
B01D71/78B01D71/76B01D71/82C08F265/06C08F297/02C08L51/06B01D71/34B01D71/40B01D2325/18
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Quick Facts
Patent No.
US 10,525,424
App. No.
15/541,260
Granted
Jan 7, 2020
Kind
B2
Abstract

A graft copolymer including zwitterionic repeat units and hydrophobic repeat units, in which the zwitterionic repeat units constitute 2-60 wt % of the graft copolymer and each of the hydrophobic repeat units is characterized in that a homopolymer formed thereof is miscible with polyvinylidene fluoride, polysulfone, poly ether sulfone, polyvinyl chloride, or polyacrylonitrile, each of the hydrophobic repeat units not being a repeat unit of polyvinylidene fluoride. Also disclosed is a filtration membrane containing such a graft copolymer or a statistical copolymer that includes the same composition of repeat units as the graft copolymer. Further disclosed are methods of preparing the graft copolymer and the filtration membrane.

Claims (47)

1. A graft copolymer, comprising:

a hydrophobic backbone, comprising a plurality of hydrophobic repeat units and a plurality of zwitterionic repeat units, wherein the number of hydrophobic repeat units is greater than the number of zwitterionic repeat units; and

a plurality of 2-50 repeat side chains, comprising hydrophobic repeat units and zwitterionic repeat units, wherein each side chain comprises more zwitterionic repeat units than hydrophobic repeat units;

wherein

the zwitterionic repeat units constitute 2-60% by weight of the graft copolymer;

each of the hydrophobic repeat units, independently, is [—O-Ph-C(CH 3 ) 2 -Ph-O-Ph-SO 2 -Ph-], [-Ph-SO 2 Ph-O-Ph-Ph-O—], [-Ph-SO 2 -Ph-O-Ph-SO 2 -Ph-O—], [-Ph-SO 2 -Ph-O-Ph-O—], or a repeat unit formed from methyl methacrylate, N,N-dimethyl acrylamide, ethyl methacrylate, acetonyl methacrylate, trifluoroethyl methacrylate, acrylonitrile, vinyl pyridine, vinyl chloride, styrene, cyclohexyl methacrylate, or propyl acrylate;

the hydrophobic repeat units are capable of forming a homopolymer that is miscible with polyvinylidene fluoride, polysulfone, poly ether sulfone, polyvinyl chloride, or polyacrylonitrile; and

each of the hydrophobic repeat units being different from a repeat unit formed from vinylidene fluoride.

2. The graft copolymer of claim 1 , wherein

the zwitterionic repeat units each comprise independently sulfobetaine, carboxybetaine, phosphorylcholine, or pyridinium alkyl sulfonate; and

each of the hydrophobic repeat units, independently, is formed from methyl methacrylate, N,N-dimethyl acrylamide, ethyl methacrylate, acetonyl methacrylate, trifluoroethyl methacrylate, acrylonitrile, vinyl pyridine, vinyl chloride, styrene, cyclohexyl methacrylate, or propyl acrylate.

3. The graft copolymer of claim 2 , wherein the zwitterionic repeat units constitute 5-45% by weight of the graft copolymer and the graft copolymer has a molecular weight of 10,000 to 3,000,000 Dalton.

4. The graft copolymer of claim 3 , wherein the zwitterionic repeat units constitute 10-30% by weight of the graft copolymer and the graft copolymer has a molecular weight of 30,000 to 1,000,000 Dalton.

5. The graft copolymer of claim 2 , wherein the zwitterionic repeat units are each formed independently from sulfobetaine methacrylate, sulfobetaine-2-vinyl pyridine, sulfobetaine-4-vinyl pyridine, phosphorylcholine methacrylate, carboxybetaine methacrylate, or sulfobetaine acrylamide; and the hydrophobic repeat units are each formed from methyl methacrylate.

6. The graft copolymer of claim 5 , wherein the zwitterionic repeat units constitute 5-45% by weight of the graft copolymer and the graft copolymer has a molecular weight of 10,000 to 3,000,000 Dalton.

7. The graft copolymer of claim 2 , wherein the zwitterionic repeat units are each formed independently from sulfobetaine methacrylate, sulfobetaine-2-vinyl pyridine, sulfobetaine-4-vinyl pyridine, phosphorylcholine methacrylate, carboxybetaine methacrylate, or sulfobetaine acrylamide.

8. The graft copolymer of claim 7 , wherein the zwitterionic repeat units are each formed from sulfobetaine methacrylate.

9. The graft copolymer of claim 8 , wherein the hydrophobic repeat units are each formed from methyl methacrylate.

10. The graft copolymer of claim 7 , wherein the zwitterionic repeat units are each formed from sulfobetaine-2-vinyl pyridine.

11. The graft copolymer of claim 10 , wherein the hydrophobic repeat units are each formed from methyl methacrylate.

12. The graft copolymer of claim 7 , wherein the zwitterionic repeat units are each formed from sulfobetaine-4-vinyl pyridine.

13. The graft copolymer of claim 12 , wherein the hydrophobic repeat units are each formed from methyl methacrylate.

14. The graft copolymer of claim 7 , wherein the zwitterionic repeat units are each formed from phosphorylcholine methacrylate.

15. The graft copolymer of claim 14 , wherein the hydrophobic repeat units are each formed from methyl methacrylate.

16. The graft copolymer of claim 7 , wherein the zwitterionic repeat units are each formed from carboxybetaine methacrylate.

17. The graft copolymer of claim 16 , wherein the hydrophobic repeat units are each formed from methyl methacrylate.

18. The graft copolymer of claim 7 , wherein the zwitterionic repeat units are each formed from sulfobetaine acrylamide.

19. The graft copolymer of claim 18 , wherein the hydrophobic repeat units are each formed from methyl methacrylate.

20. The graft copolymer of claim 1 , wherein the zwitterionic repeat units constitute 5-45% by weight of the graft copolymer and the graft copolymer has a molecular weight of 10,000 to 3,000,000 Dalton.

21. The graft copolymer of claim 20 , wherein the zwitterionic repeat units constitute 10-30% by weight of the graft copolymer and the graft copolymer has a molecular weight of 30,000 to 1,000,000 Dalton.

22. A filtration membrane comprising:

a base polymer, and

a zwitterion-containing copolymer,

wherein

the base polymer is polyvinylidene fluoride, polysulfone, poly ether sulfone, polyvinyl chloride, or polyacrylonitrile;

the zwitterion-containing copolymer comprises zwitterionic repeat units and hydrophobic repeat units, in which the zwitterionic repeat units constitute 2-60% by weight of the copolymer and the hydrophobic repeat units are capable of forming a homopolymer that is miscible with the base polymer, each of the hydrophobic repeat units being different from a repeat unit of polyvinylidene fluoride; and

the zwitterion-containing copolymer is insoluble in water, wherein the zwitterion-containing copolymer is a graft copolymer including a hydrophobic backbone, comprising a plurality of hydrophobic repeat units and a plurality of zwitterionic repeat units, wherein the number of hydrophobic repeat units is greater than the number of zwitterionic repeat units, and a plurality of 2-50 repeat side chains, each of which comprises more zwitterionic repeat units than hydrophobic units; wherein

the zwitterionic repeat units constitute 2-60% by weight of the graft copolymer;

the zwitterionic repeat units each comprises independently sulfobetaine, carboxybetaine, phosphorylchloline, or pyridinium alkyl sulfonate;

each of the hydrophobic repeat units, independently, is [—O-Ph-C(CH 3 ) 2 -Ph-O-Ph-SO 2 -Ph-], [-Ph-SO 2 Ph-O-Ph-Ph-O—], [-Ph-SO 2 -Ph-O-Ph-SO 2 -Ph-O—], [-Ph-SO 2 -Ph-O-Ph-O—], or a repeat unit formed from methyl methacrylate, N,N-dimethyl acrylamide, ethyl methacrylate, acetonyl methacrylate, trifluoroethyl methacrylate, acrylonitrile, vinyl pyridine, vinyl chloride, styrene, cyclohexyl methacrylate, or propyl acrylate;

the hydrophobic repeat units are capable of forming a homopolymer that is miscible with polyvinylidene fluoride, polysulfone, poly ether sulfone, polyvinyl chloride, or polyacrylonitrile; and

each of the hydrophobic repeat units being different from a repeat unit formed from vinylidene fluoride.

23. The filtration membrane of claim 22 , wherein the membrane is an ultrafiltration membrane or a microfiltration membrane.

24. The filtration membrane of claim 22 , wherein each of the hydrophobic repeat units is different from a repeat unit of polyacrylonitrile; and the zwitterion-containing copolymer constitutes less than 50 wt % of a mixture of the base polymer and the zwitterion-containing copolymer.

25. The filtration membrane of claim 22 , wherein the zwitterionic repeat units are each formed independently from sulfobetaine methacrylate, sulfobetaine-2-vinyl pyridine, sulfobetaine-4-vinyl pyridine, phosphorylcholine methacrylate, carboxybetaine methacrylate, or sulfobetaine acrylamide; and each of the hydrophobic repeat units, independently, is formed from methyl methacrylate, N,N-dimethyl acrylamide, ethyl methacrylate, acetonyl methacrylate, trifluoroethyl methacrylate, acrylonitrile, vinyl pyridine, vinyl chloride, styrene, cyclohexyl methacrylate, or propyl acrylate.

26. The filtration membrane of claim 22 , wherein the zwitterionic repeat units constitute 5-45% by weight of the graft copolymer and the graft copolymer has a molecular weight of 10,000 to 3,000,000 Dalton.

27. The filtration membrane of claim 22 , wherein the membrane is a flat sheet membrane or a hollow fiber membrane.

Assignments (4)
CORRECTIVE ASSIGNMENT TO CORRECT THE CONVEYING PARTY NAME PREVIOUSLY RECORDED AT REEL: 43831 FRAME: 210. ASSIGNOR(S) HEREBY CONFIRMS THE ASSIGNMENT. Recorded Apr 4, 2019
From: TRUSTEES OF TUFTS COLLEGE
To: NATIONAL SCIENCE FOUNDATION
Reel/Frame 049785/0972 →
CORRECTIVE ASSIGNMENT TO CORRECT THE RECEIVING PARTY ADDRESS PREVIOUSLY RECORDED AT REEL: 48456 FRAME: 825. ASSIGNOR(S) HEREBY CONFIRMS THE ASSIGNMENT. Recorded Apr 4, 2019
From: ALEXIOU, AYSE ASATEKIN; KANER, PAPATYA; VANNUCCI, CHIARA
To: TRUSTEES OF TUFTS COLLEGE
Reel/Frame 048799/0402 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Feb 27, 2019
From: ALEXIOU, AYSE A.; KANER, PAPATYA; VANNUCCI, CHIARA
To: TRUSTEES OF TUFTS COLLEGE
Reel/Frame 048456/0825 →
CONFIRMATORY LICENSE Recorded Sep 21, 2017
From: TUFTS UNIVERSITY
To: NATIONAL SCIENCE FOUNDATION
Reel/Frame 043931/0210 →
Continuity (2)
Provisional Application 62098195 · Dec 30, 2014
Related Publication 20180001278A1 · Jan 4, 2018