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Modified graphene oxide/Nafion composite proton exchange membrane as well as preparation method and application thereof

A proton exchange membrane, oxide stone technology, applied in electrochemical generators, climate sustainability, final product manufacturing, etc., can solve problems such as water loss, interfere with normal cathode reaction, and decline, and achieve enhanced alcohol resistance, proton resistance, etc. The effect of high conductivity enhancement

Inactive Publication Date: 2020-08-14
GUANGDONG PROVINCIAL BIOENGINEERING INST (GUANGZHOU SUGARCANE IND RES INST)
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

At present, the perfluorosulfonic acid membrane represented by Nafion is the most researched and applied, but there are two key scientific problems in the actual application of Nafion membrane: one is that Nafion membrane loses water seriously under high temperature and low humidity conditions, and the proton conductivity will decrease. Due to the collapse of the ion cluster network proton transport channels formed by sulfonic acid groups and water molecules through dynamic hydrogen bonds, the proton transport channel collapsed significantly; the second is that when the Nafion membrane is used in a direct methanol fuel cell (DMFC), fuel methanol permeates seriously, and methanol molecules are easy to follow Water molecules pass through the ion cluster network together and penetrate to the cathode, which not only causes fuel waste, but also interferes with the normal reaction of the cathode, resulting in a significant drop in DMFC efficiency
[0005] In summary, graphene oxide modified with acid-base block polymers has been applied to prepare composite proton exchange membranes, but it has not been seen that monomers containing acidic groups (sulfonic acid) and basic groups (imidazole) have been sequentially synthesized by ATRP reaction. Graft polymerization onto the surface of graphene oxide, and compound with Nafion to prepare acid-base block copolymer to modify graphene oxide / Nafion composite proton exchange membrane, strengthen the proton conduction and alcohol resistance of Nafion membrane, and solve the problem of Nafion membrane proton conductivity and methanol permeation There are common problems that restrict each other and cannot be improved at the same time

Method used

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  • Modified graphene oxide/Nafion composite proton exchange membrane as well as preparation method and application thereof
  • Modified graphene oxide/Nafion composite proton exchange membrane as well as preparation method and application thereof
  • Modified graphene oxide/Nafion composite proton exchange membrane as well as preparation method and application thereof

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Effect test

Embodiment 1

[0028] Disperse 0.5 g of graphene oxide (GO) prepared by the Hummers method by ultrasound for 30 minutes into 200 mL of ethanol and N,N-dimethylformamide (DMF) mixed solvent (volume ratio 1:1), add 40 mL of ammonia water, 40 °C Stir at low temperature for 2 hours, dissolve 2.2mL (3-aminopropyl)triethoxysilane (APTES) into 100mL ethanol solution, add dropwise to the above GO dispersion, and continue to stir and react overnight at 40°C after the dropwise addition is completed. Cool to room temperature, centrifuge, wash with absolute ethanol and acetone successively, and vacuum dry to obtain amino-modified graphene oxide (GO-NH 2 ). 0.5g GO-NH 2 Disperse into 40mL DMF by ultrasonication for 30 minutes, add 5mL triethylamine, cool to 0°C, slowly add α-bromoisobutyryl bromide 1.74mL / DMF 30mL solution dropwise under nitrogen atmosphere, after the dropwise addition, react at room temperature for 36 hours, filtered, washed with DMF, absolute ethanol, and acetone successively, and va...

Embodiment 2

[0032] Disperse 0.5 g of graphene oxide (GO) prepared by the Hummers method by ultrasound for 30 minutes into 200 mL of ethanol and N,N-dimethylformamide (DMF) mixed solvent (volume ratio 1:1), add 40 mL of ammonia water, 40 °C Stir at low temperature for 2 hours, dissolve 2.2mL (3-aminopropyl)triethoxysilane (APTES) into 100mL ethanol solution, add dropwise to the above GO dispersion, and continue to stir and react overnight at 40°C after the dropwise addition is completed. Cool to room temperature, centrifuge, wash with absolute ethanol and acetone successively, and vacuum dry to obtain amino-modified graphene oxide (GO-NH 2 ). 0.5g GO-NH 2 Disperse into 40mL DMF by ultrasonication for 30 minutes, add 5mL triethylamine, cool to 0°C, slowly add α-bromoisobutyryl bromide 1.74mL / DMF 30mL solution dropwise under nitrogen atmosphere, after the dropwise addition, react at room temperature for 36 hours, filtered, washed with DMF, absolute ethanol, and acetone successively, and va...

Embodiment 3

[0036] Disperse 0.5 g of graphene oxide (GO) prepared by the Hummers method by ultrasound for 30 minutes into 200 mL of ethanol and N,N-dimethylformamide (DMF) mixed solvent (volume ratio 1:1), add 40 mL of ammonia water, 40 °C Stir at low temperature for 2 hours, dissolve 2.2mL (3-aminopropyl)triethoxysilane (APTES) into 100mL ethanol solution, add dropwise to the above GO dispersion, and continue to stir and react overnight at 40°C after the dropwise addition is completed. Cool to room temperature, centrifuge, wash with absolute ethanol and acetone successively, and vacuum dry to obtain amino-modified graphene oxide (GO-NH 2 ). 0.5g GO-NH 2 Disperse into 40mL DMF by ultrasonication for 30 minutes, add 5mL triethylamine, cool to 0°C, slowly add α-bromoisobutyryl bromide 1.74mL / DMF 30mL solution dropwise under nitrogen atmosphere, after the dropwise addition, react at room temperature for 36 hours, filtered, washed with DMF, absolute ethanol, and acetone successively, and va...

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Abstract

The invention discloses a modified graphene oxide / Nafion composite proton exchange membrane as well as a preparation method and application thereof. The preparation method comprises the following steps: introducing an ATRP initiator to the surface of graphene oxide, and sequentially carrying out ATRP reaction to graft-polymerize monomers containing acidic groups and basic groups to the surface ofthe graphene oxide, thereby obtaining acid-base block copolymer modified graphene oxide; and uniformly mixing the dispersion liquid of the acid-base block copolymer modified graphene oxide with a Nafion solution, and preparing the modified graphene oxide / Nafion composite proton exchange membrane by a solution casting method. According to the preparation method, a novel proton transfer site is formed at a Nafion-graphene oxide interface by utilizing an acid-base group; a continuous proton transfer channel is constructed, the proton conductivity of the proton exchange membrane in a high-temperature and low-humidity environment can be improved, the graphene oxide with a two-dimensional nano layered structure can block the diffusion of methanol molecules, and the methanol permeability of the proton exchange membrane is reduced.

Description

technical field [0001] The invention relates to a fuel cell proton exchange membrane and a preparation method thereof, in particular to a modified graphene oxide / Nafion composite proton exchange membrane and a preparation method and application thereof. Background technique [0002] With the increasingly prominent energy and environmental issues, proton exchange membrane fuel cells (PEMFC) have become a hot spot in new energy research due to their high efficiency and environmental protection advantages. Proton exchange membrane (PEM) is the core component of PEMFC, which directly determines the energy conversion efficiency and service life of PEMFC. Among them, proton conductivity and alcohol resistance are two key performance indicators of PEMFC. At present, the perfluorosulfonic acid membrane represented by Nafion is the most researched and applied, but there are two key scientific problems in the actual application of Nafion membrane: one is that Nafion membrane loses wat...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): C08J5/22C08J7/12C08J7/14C08F293/00C08F292/00C08L27/18C08L53/00H01M8/1009H01M8/1041H01M8/1069
CPCC08J5/2237C08J5/2293C08J7/12C08J7/14C08F293/005C08F292/00H01M8/1069H01M8/1041H01M8/1009C08J2327/18C08J2453/00C08F2438/01Y02E60/50Y02P70/50
Inventor 李发勇陈骏佳高旭华谢东李圆
Owner GUANGDONG PROVINCIAL BIOENGINEERING INST (GUANGZHOU SUGARCANE IND RES INST)