IP Library Granted Patent US 11,148,099
Granted Patent B2
US 11,148,099 · App. 16/743,055 · Granted Oct 19, 2021

Graphene-based membrane and method of producing the same

Inventors: James Antony Prince (Singapore, SG); Sowrirajalu Bhuvana (Singapore, SG); Anbharasi Vanangamudi (Singapore, SG); Gurdev Singh (Singapore, SG)
Assignee: Ngee Ann Polytechnic
B01D67/0079B01D67/00B01D69/148B01D71/021B01D71/40B01D71/42B01D71/60B01D71/68B01D71/76B01D71/78C08F8/12C08F8/32C08F8/48C08F220/44C08F222/06C08G73/101C08G73/1075C08G73/14C08L33/24C08L73/02B01D2323/38B01D2325/36C08F2800/10C08F2810/20
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Quick Facts
Patent No.
US 11,148,099
App. No.
16/743,055
Granted
Oct 19, 2021
Kind
B2
Abstract

A graphene-based membrane and a method of producing the same are disclosed. The graphene-based membrane may include a graphene-polymer composite, wherein the graphene-polymer composite may consist of an amine functionalized graphene and a polymer containing an anhydride group as a linker for linking the amine functionalized graphene to the polymer. The graphene-based membrane may be constructed of a single-layer. A method may include reacting a polymer containing an anhydride with an amine functionalized graphene in presence of a solvent to form an intermediate product; and thermal imidizing the intermediate product to form a graphene grafted polymer composite for use in fabricating a graphene-based membrane.

Claims (32)

1. A method of producing a single-layer graphene-based membrane from a graphene-polymer composite, the method comprising:

(i) reacting a polymer containing an anhydride group with an amine functionalized graphene in presence of a solvent to form an intermediate product; and

(ii) thermal imidizing the intermediate product to form a graphene grafted polymer composite for use in fabricating graphene-based membrane,

wherein the polymer containing the anhydride group is a poly(acrylonitrile-co-maleic anhydride) and wherein the graphene grafted polymer is a graphene grafted poly(acrylonitrile-co-malemide).

2. The method according to claim 1 , wherein the thermal imidization is carried out by heating the intermediate product at a temperature ranging from 115° C. to 255° C. for a period of 1.5 to 4.5 hours.

3. The method according to claim 1 , wherein the thermal imidization is carried out by heating the intermediate product at 195° C. to 125° C. for 0.5 to 1.5 hours, followed by 180° C. to 220° C. for another 0.5 to 1.5 hours, and 245° C. to 255° C. for yet another 0.5 to 1.5 hours.

4. The method according to claim 1 , wherein the thermal imidization is carried out by heating the intermediate product at 120° C. for 2 hours, followed by 200° C. for 1 hour.

5. The method according to claim 1 , wherein the solvent is a polar aprotic solvent.

6. The method according to claim 5 wherein the solvent is N—N-dimethyl acetamide.

7. The method according to claim 1 , wherein the polymer containing an anhydride group reacts with the amine functionalized graphene at a temperature of 80° C. for 24 hours.

8. The method according to claim 1 , wherein the intermediate product is graphene grafted poly(acrylonitrile-co-maleic acid).

9. The method according to claim 1 , further comprising:

adding the graphene grafted polymer composite to a solution containing polyvinylpyrolidone, N-methyl-2-pyrolidone and diethylene glycol; and

stirring the solution to obtain a homogenous polymeric casting solution for use in fabricating graphene-based membrane.

10. The method according to claim 9 , wherein the casting solution comprises 15 to 40 wt % graphene grafted polymer composite, 2 to 15 wt % polyvinylpyrolidone, 1 to 15 wt % diethylene glycol and 40 to 80 wt % N-methyl-2-pyrolidone.

11. The method according to claim 9 , wherein the casting solution comprises 21 wt % graphene grafted polymer composite, 5 wt % polyvinylpyrolidone, 5 wt % diethylene glycol and 69 wt % N-methyl-2-pyrolidone.

12. The method according to claim 9 , wherein the solution is stirred at a speed of 250 to 350 rpm for at least 24 hours at 80° C.

13. The method according to claim 9 , further comprising:

fabricating the graphene-based membrane using phase inversion method.

14. The method according to claim 13 , wherein the graphene-based membrane is a flat sheet membrane.

15. The method according to claim 1 , further comprising:

adding a second polymer selected from the group consisting of polyethersulfone, polyvinylidene fluoride, polyacrylonitrile, cellulose acetate, polytetrafluoroethylene and polypropylene to the graphene grafted poly(acrylonitrile-co-maleimide) composite to form a mixture;

adding the mixture to a solution comprising polyvinylpyrolidone, N-methyl-2-pyrolidone and diethylene glycol; and

stirring the solution to obtain a homogenous polymeric casting solution for use in fabricating graphene-based membrane.

16. The method according to claim 15 , wherein the second polymer is polyethersulfone.

17. The method according to claim 16 , wherein the casting solution containing the modified polyethersulfone graphene grafted poly(acrylonitrile-co-maleimide) composite comprises 15 to 40 wt % polyethersulfone, 2 to 15 wt % polyvinylpyrolidone, 1 to 15 wt % diethylene glycol, 40 to 80 wt % N-methyl-2-pyrolidone and 1 to 25 wt % graphene grafted poly(acrylonitrile-co-maleimide) composite.

18. The method according to claim 16 , wherein the casting solution containing the modified polyethersulfone graphene grafted poly(acrylonitrile-co-maleimide) composite comprises 21 wt % polyethersulfone, 5 wt % polyvinylpyrolidone, 5 wt % diethylene glycol, 64 wt % N-methyl-2-pyrolidone and 5 wt % graphene grafted poly(acrylonitrile-co-maleimide) composite.

19. The method according to claim 15 , wherein the solution is stirred at a speed of 250 to 350 rpm for at least 24 hours at 80° C.

20. The method according to claim 15 , further comprising:

fabricating the graphene-based membrane using dry-wet spinning method.

21. The method according to claim 20 , wherein the graphene-based membrane is a hollow-fiber membrane.

22. The method according to claim 14 , wherein the graphene-based membrane has an average pore size of 0.04 to 0.10 μm.

Assignments (1)
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Jan 15, 2020
From: PRINCE, JAMES ANTONY; BHUVANA, SOWRIRAJALU; VANANGAMUDI, ANBHARASI; SINGH, GURDEV
To: NGEE ANN POLYTECHNIC
Reel/Frame 051519/0380 →
Continuity (2)
Division 15567956
Related Publication 20200164318A1 · May 28, 2020