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Carbon-based ZIF (zeolitic imidazolate framework) composite catalyst as well as preparation method and application thereof in electrocatalytic reduction of carbon dioxide

A composite catalyst and carbon-based technology, applied in the field of electrocatalysis, can solve the problems of not being able to meet the application requirements, not being widely used, and having no catalytic activity, etc., and achieve excellent electrocatalytic carbon dioxide reduction performance, easy promotion, and outstanding performance

Inactive Publication Date: 2019-04-26
XI AN JIAOTONG UNIV
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  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0004] Although it has been reported that rare metals have significant activity in catalyzing carbon dioxide reduction, they cannot be widely used due to problems such as easy deactivation and high price; although non-metallic catalysts are stable, they do not have sufficient catalytic activity and cannot meet application requirements

Method used

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  • Carbon-based ZIF (zeolitic imidazolate framework) composite catalyst as well as preparation method and application thereof in electrocatalytic reduction of carbon dioxide
  • Carbon-based ZIF (zeolitic imidazolate framework) composite catalyst as well as preparation method and application thereof in electrocatalytic reduction of carbon dioxide
  • Carbon-based ZIF (zeolitic imidazolate framework) composite catalyst as well as preparation method and application thereof in electrocatalytic reduction of carbon dioxide

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preparation example Construction

[0029] The present invention selects ZIF as a precursor, uses the method of induced growth to compound it with carbon materials, and then undergoes high-temperature carbonization to form a rich mesoporous pore structure, and constructs an active center of Fe-N-C, which can convert carbon dioxide into carbon monoxide. . In order to realize the efficient catalytic carbon dioxide reduction of the catalyst, the present invention mainly optimizes the catalytic performance of the carbon dioxide reduction by selecting different transition metal salts, different binders and different carbon materials. The present invention combines ZIF with rich pore structure and carbon material to realize high-efficiency catalytic carbon dioxide conversion. The preparation method of carbon-based composite ZIF includes the following three steps: (1) purification and pretreatment of carbon material; (2) carbon dioxide The material and the binder are added to the ZIF precursor solution, and the ZIF is ...

Embodiment 1

[0051] 1. Graphene oxide pretreatment: Wash the prepared graphene oxide with a large amount of 0.1M dilute hydrochloric acid to remove impurities contained therein, and then wash it with a large amount of water until it is nearly neutral;

[0052] 2. Preparation of graphene-based ZIF composite catalyst: disperse the pretreated graphene oxide into deionized water (concentration about 7mg / mL); weigh 7.3g of zinc nitrate and 0.34g of ferrous sulfate, and dissolve them in 800mL of methanol And stir evenly, then add 0.5g polymethylpyrrolidone (PVP) and 10mL carbon material dispersion liquid, after stirring evenly again, add 8.5g 2-methylimidazole, keep stirring at 25°C for 24h. After the stirring was completed, the supernatant was separated by centrifugation, and the precipitate was washed three times with methanol, then transferred to a vacuum drying oven, and dried under vacuum at 70° C. overnight. After drying, high-temperature carbonization was carried out in an argon atmospher...

Embodiment 2

[0058] 1. Graphene oxide pretreatment: Wash the prepared graphene oxide with a large amount of 0.1M dilute hydrochloric acid to remove impurities contained therein, and then wash it with a large amount of water until it is nearly neutral.

[0059] 2. Preparation of graphene-based ZIF composite catalyst: disperse the pretreated graphene oxide into deionized water (concentration about 7mg / mL); weigh 7.3g of zinc nitrate and 0.34g of ferrous sulfate, and dissolve them in 800mL of methanol And stir evenly, then add 0.5g polyethyleneimine (PEI) and 10mL carbon material dispersion liquid, after stirring evenly again, add 8.5g 2-methylimidazole, keep stirring at 25°C for 24h. After the stirring was completed, the supernatant was separated by centrifugation, and the precipitate was washed three times with methanol, then transferred to a vacuum drying oven, and dried under vacuum at 70° C. overnight. After drying, high-temperature carbonization was carried out in an argon atmosphere, r...

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Abstract

The invention provides a carbon-based ZIF (Zeolitic Imidazolate Framework) composite catalyst as well as a preparation method and application thereof. The preparation method comprises the following steps: 1, pretreating a carbon material, namely carrying out purification and acid treatment on the carbon material; 2, carrying out double-metal ZIF inductive growth, namely putting the carbon materialpretreated in the step 1 and an adhesive into a methanol solution of a transition metal salt, zinc nitrate and 2-methylimidazole, and carrying out a stirring reaction to obtain a precursor; 3, carrying out high-temperature carbonization, namely carrying out high-temperature carbonization on the precursor obtained in the step 2 in an inert atmosphere. As polyvinylpyrrolidone or polyethyleneimine is adopted as the adhesive, on one side, the surface of the carbon material can be modified, on the other hand, more transition metal ions can be captured uniformly from the surface, and homogeneous nucleation and growth of a ZIF on the surface of the carbon material can be induced. The carbon-based composite material provided by the invention has outstanding properties, is capable of replacing conventional rare metal catalysts, and in addition, the operation is simple, the raw materials are easy to obtain and the carbon-based composite material is easy to be popularized in related fields of electro-catalysis.

Description

technical field [0001] The invention belongs to the field of electrocatalysis, in particular to a carbon-based ZIF composite catalyst and its preparation method and the electrocatalytic reduction of CO 2 React application. Background technique [0002] ZIF is a kind of MOFs (metal-organic framework compound) material, which is a kind of tetrahedral framework material formed by cross-linking organic imidazolates to transition metals. Due to its large specific surface area, adjustable pore size, and frame modification, ZIF materials have been frequently reported in the field of electrocatalysis. [0003] At present, electrocatalytic carbon dioxide reduction is a hot topic of great concern. Among them, electrocatalysts can be mainly divided into two categories: 1) metals represented by rare metals, transition metals, transition metal oxides or sulfides, etc. 2) non-metallic catalysts represented by nitrogen, phosphorus, boron, sulfur-doped graphene, carbon nanotubes, etc. ...

Claims

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Application Information

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IPC IPC(8): B01J31/22B01J37/08C25B11/06
CPCB01J31/1691B01J37/0018B01J37/084B01J2531/845B01J2531/847B01J2531/842B01J2531/26B01J2531/0241C25B11/095B01J35/33
Inventor 胡超穆野邱介山
Owner XI AN JIAOTONG UNIV
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