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Catalyst for preparing alcohol through methane electro-oxidation and preparation method and application thereof

A catalyst and electro-oxidation technology, applied in the direction of electrodes, electrolysis components, electrolysis process, etc., can solve the problems of lack of practical application value and high catalyst cost, and achieve high selectivity and the effect of inhibiting deep oxidation

Pending Publication Date: 2022-07-22
SHANGHAI SHENGJIAN ENVIRONMENTAL SYST TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0009] However, most of the above-mentioned catalysts use noble metals (Pt, Pd, Au, Ru, Rh) as the main active components or important doping aids, which makes the catalyst cost too high for the electrooxidation of methane to alcohol and lacks practical application value.
In addition, catalyst powder is usually mixed with conductive agent (carbon black, etc.), binder (Nafion solution, etc.), solvent (water, ethanol, acetone, etc.) , metal foam, conductive glass, etc.), it is impossible to avoid the performance attenuation caused by the shedding of active components

Method used

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  • Catalyst for preparing alcohol through methane electro-oxidation and preparation method and application thereof

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preparation example Construction

[0065] An embodiment of the present invention provides a method for preparing a catalyst, which can be used for the electro-oxidation of methane to alcohol, comprising the following steps:

[0066] S1. Preparation of reduced graphene oxide dispersion

[0067] The graphene oxide (GO) dispersion is mixed evenly with ammonia water and hydrazine hydrate, and the reaction is carried out at 70°C-100°C for 0.5h-4h to obtain a reduced graphene oxide (rGO) dispersion, and stirring is maintained during the preparation process.

[0068] In order to further control the sufficient reduction of graphene oxide, the concentration of graphene oxide dispersion liquid is 0.05mg / mL-0.5mg / mL (such as 0.05mg / mL, 0.1mg / mL, 0.2mg / mL, 0.3mg / mL, 0.4mg / mL) / mL, 0.5mg / mL), ammonia water is an aqueous solution with an ammonia content of 25-28wt%, hydrazine hydrate is an aqueous solution with a hydrazine hydrate content of 80-90wt%, and the volume ratio of ammonia water to graphene oxide dispersion is 1:(1...

Embodiment 1

[0096] The present embodiment provides a preparation method of a catalyst, comprising the following steps:

[0097] (1) Graphene oxide was prepared according to the Hummers method, and deionized water was injected into the prepared graphene oxide to obtain a GO dispersion with a concentration of 0.2 mg / mL. Take 100 mL of the GO dispersion and mix it with ammonia water and hydrazine hydrate. Among them, the volume ratio of ammonia water and GO dispersion liquid is 1:1000, and the volume ratio of hydrazine hydrate and GO dispersion liquid is 1:10000, and the rGO dispersion liquid is obtained by refluxing at 80 °C for 1 h.

[0098] (2) Use a syringe pump to slowly inject the zinc acetate solution into the NaOH solution. The concentration of zinc acetate in the mixed solution is 1mM, and the mass concentration ratio of zinc acetate and NaOH is 1:4. Stir evenly and heat at 80 °C for 1 h to obtain a ZnO colloidal solution. Dilute with deionized water to a target concentration of 0....

Embodiment 2

[0136] The present embodiment provides a preparation method of a catalyst, comprising the following steps:

[0137] (1) 100 mL of GO dispersion with a concentration of 0.2 mg / mL was uniformly mixed with ammonia water and hydrazine hydrate. Among them, the volume ratio of ammonia water and GO dispersion was 2.8:1000, the volume ratio of hydrazine hydrate and GO dispersion was 5.1:10000, and the rGO dispersion was obtained by refluxing at 90 °C for 0.5 h.

[0138] (2) Use a syringe pump to slowly inject the zinc acetate solution into the NaOH solution, the concentration of zinc acetate in the mixed solution is 7.5mM, and the ratio of the concentration of zinc acetate to NaOH is 1:4, stir evenly and heat at 60°C for 2h to obtain a ZnO colloidal solution, Deionized water was added to dilute to a target concentration of 0.2 mg / mL.

[0139] (3) The ZnO colloidal solution and the rGO dispersion (100 mL) were mixed in a volume ratio of 2:1, and vacuum filtered through the mixed cellu...

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Abstract

The invention discloses a catalyst for preparing alcohol through methane electro-oxidation and a preparation method and application thereof, and relates to the technical field of catalysts. The catalyst for preparing alcohol through methane electrooxidation comprises a hydrogel film formed by reduced graphene oxide and zinc oxide colloid, the zinc oxide colloid is dispersed in a film layer of the hydrogel film, zirconium oxide and nickel are loaded on the surface of the hydrogel film, and the non-noble metal catalyst is obtained. Meanwhile, the catalyst has high methanol / isopropanol selectivity at room temperature, and can effectively inhibit deep oxidation.

Description

technical field [0001] The invention relates to the technical field of catalysts, in particular, to a catalyst for producing alcohol by electrooxidation of methane, a preparation method and application thereof. Background technique [0002] There are abundant natural gas resources in the earth's crust all over the world, and the storage amount accounts for about 21% of the total energy of the earth. In recent years, unconventional natural gas resources such as shale gas and methane hydrate have been continuously explored, making natural gas an ideal substitute for petroleum resources. Methane is the main component of natural gas (about 70-90% by volume). Given the extremely high combustion enthalpy (-892kJ / mol) and energy density (>1000kWh / m) of methane 3 ), most natural gas resources are used for heating or catalytic oxidation in fuel cells to generate electricity. Carbon dioxide emissions and methane leakage from these uses will exacerbate the greenhouse effect. In ...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): C25B3/07C25B11/054C25B11/065C25B11/067C25B11/091
CPCC25B3/07C25B11/054C25B11/065C25B11/067C25B11/091Y02E60/50
Inventor 张伟明张辰栗文龙胡雪慧
Owner SHANGHAI SHENGJIAN ENVIRONMENTAL SYST TECH
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