Method of fabricating proton-conducting electrolytic membrane

Patent metadata

Field	Value
Publication number	US-9705146-B2
Application number	US-201414583868-A
Country	US
Kind code	B2
Filing date	Dec 29, 2014
Priority date	Dec 29, 2014
Publication date	Jul 11, 2017
Grant date	Jul 11, 2017

Abstract

A method is provided to fabricate an electrolyte membrane. The membrane has an asymmetric structure and is a polybenzimidazole membrane doped with phosphoric acid. The asymmetric structure comprises a dense layer and a porous layer. The content of phosphoric acid introduced into the polybenzimidazole membrane reaches 20 phosphoric acid molecules per polymer repeating unit. The proton conductivity of the polybenzimidazole membrane reaches 5×10 −2 siemens per centimeter (S/cm). An electrode made with the polybenzimidazole membrane can be smoothly operated in a proton exchange membrane fuel cell.

First claim

What is claimed is:

1. A method of fabricating a proton-conducting electrolytic membrane, comprising steps of:
(a) through a template-leaching method, obtaining an ionic liquid in the form of a salt compound containing imidazolium as a template to be mixed with a polybenzimidazole solution to obtain an asymmetric-structure polybenzimidazole membrane after leaching out a porous layer,

wherein said ionic liquid and said polybenzimidazole solution are immiscible; and
(b) through being soaked in phosphoric acid, introducing phosphoric acid into said polybenzimidazole membrane to obtain a proton-conducting electrolytic membrane,
wherein step (a) comprises the following steps:
said polybenzimidazole solution and said ionic liquid are mixed with a first organic solvent; said first organic solvent simultaneously dissolves said polybenzimidazole solution and said ionic liquid to obtain a mixture; said first organic solvent is removed to obtain a solid membrane with said polybenzimidazole solution and said ionic liquid; said solid membrane is soaked in a second organic solvent; said second organic solvent dissolves said polybenzimidazole solution but not said ionic liquid so that said ionic liquid is extracted from said solid membrane to be filtered off; and said solid membrane is hot-dried to remove excess solvent to obtain said asymmetric-structure polybenzimidazole membrane,

wherein, said first organic solvent is selected from a group consisting of dimethylacetamide (DMAc), N-Methyl-2-pyrrolidone (NMP), dimethyl-formamide (DMF), dimethyl sulfoxide (DMSO) and m-cresol; and said second organic solvent is selected from a group consisting of methanol and ethanol.

2. The method according to claim 1 ,
wherein step (b) comprises the following steps:
said asymmetric-structure polybenzimidazole membrane is soaked in an aqueous phosphoric-acid solution having high concentration; after being soaked until said polybenzimidazole membrane is not increased in weight, a content of phosphoric acid thus introduced is saturated and residual part of said phosphoric-acid solution on surface of said polybenzimidazole membrane is wiped off; and said polybenzimidazole membrane is hot-dried to remove residual water to obtain said proton-conducting electrolytic membrane,
wherein said aqueous phosphoric-acid solution has a concentration at least 11 molars (M).

3. The method according to claim 1 ,
wherein said ionic liquid has a weight ratio of content at least 50 phr relative to that of said polybenzimidazole solution.

4. The method according to claim 1 ,
wherein said asymmetric-structure polybenzimidazole membrane comprises a dense layer and a porous layer; and said dense layer and said porous layer have the same main material of polybenzimidazole.

5. The method according to claim 4 ,
wherein said material of polybenzimidazole is obtained through condensation polymerization with benzene-ring structured di-acid and benzene-ring structured tetra-amine.

6. The method according to claim 1 ,
wherein said asymmetric-structure polybenzimidazole membrane together with gas diffusion electrodes is processed through hot-pressing to obtain a membrane electrode used in a high-temperature proton exchange membrane fuel cell (PEMFC).

7. The method according to claim 6 ,
wherein said gas diffusion electrode is a carbon substrate; and said carbon substrate is coated with a catalyst on surface and has a hydrophobic microporous layer.

Assignees

• Univ Nat Cheng Kung

Inventors

• Hsu Steve Lien-Chung
• Jheng Li-Cheng

Classifications

• Y02P70/56

  Cross-Sectional Technologies · mapped topic

• H01M8/1053

  consisting of layers of polymers with at least one layer being ionically conductive · CPC title

• H01M2300/0082

  Organic polymers · CPC title

• H01M8/04197

  Preventing means for fuel crossover · CPC title

• H01M8/1048

  Ion-conducting additives, e.g. ion-conducting particles, heteropolyacids, metal phosphate or polybenzimidazole with phosphoric acid · CPC title