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A nickel-nitrogen codoped carbon electrocatalyst and a preparing method and application thereof

An electrocatalyst, co-doping technology, applied in chemical instruments and methods, physical/chemical process catalysts, electrodes, etc., to achieve the effect of improving selectivity, easy industrial production, and high specific surface area

Inactive Publication Date: 2019-05-21
ZHEJIANG UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0005] However, there are various forms of co-doped catalysts. Researchers have tried to obtain more selective catalytic materials by changing the synthesis method and selecting different precursors. However, how to significantly improve the selectivity of electrocatalytic CO generation is still an urgent need. solved problem

Method used

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  • A nickel-nitrogen codoped carbon electrocatalyst and a preparing method and application thereof
  • A nickel-nitrogen codoped carbon electrocatalyst and a preparing method and application thereof
  • A nickel-nitrogen codoped carbon electrocatalyst and a preparing method and application thereof

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0031] The preparation steps of nickel-nitrogen co-doped porous carbon nanosheets are:

[0032] Step 1. Add 5.5mol sodium benzoate (C 7 H 5 O 2 Na), 1.56mol nickel acetate (Ni(CH 3 COO) 2 ) And 6.24mol manganese acetate (Mn(CH 3 COO) 2 ) Add 60mL N,N-dimethylformamide (DMF), the molar ratio of nickel acetate to manganese acetate is 1:4, magnetically stir until it dissolves;

[0033] Step 2. Add 11 mol of terephthalic acid (BDC) and magnetically stir to dissolve to obtain a mixed solution;

[0034] Step 3. Add the mixed solution to the hydrothermal reaction kettle and react at 180° C. for 12 hours to obtain a mixed solution for generating metal organic framework compounds;

[0035] Step 4. Centrifuge the mixed solution in step 3, wash with DMF and absolute ethanol, and then vacuum dry at 80°C for 12 hours;

[0036] Step 5. Baking again at 700°C, the heating rate is 2.5°C / min, the baking time is 2h, and the obtained product includes a nickel-nitrogen doped carbon layer and manganese oxide...

Embodiment 2

[0046] The preparation steps of nickel-nitrogen co-doped porous carbon nanosheets are:

[0047] Step 1. Add 5.5mol sodium benzoate (C 7 H 5 O 2 Na), 0.39mol nickel acetate (Ni(CH 3 COO) 2 ) And 7.41mol manganese acetate (Mn(CH 3 COO) 2 ) Add 60mL N,N-dimethylformamide (DMF), the molar ratio of nickel acetate to manganese acetate is 1:9, magnetically stir to dissolve;

[0048] Step 2. Add 11 mol of terephthalic acid (BDC) and magnetically stir to dissolve to obtain a mixed solution;

[0049] Step 3. Add the mixed solution to the hydrothermal reaction kettle and react at 180° C. for 12 hours to obtain a mixed solution for generating metal organic framework compounds;

[0050] Step 4. Centrifuge the mixed solution in step 3, wash with DMF and absolute ethanol, and then vacuum dry at 80°C for 12 hours;

[0051] Step 5. Baking again at 700°C, the heating rate is 2.5°C / min, the baking time is 2h, and the obtained product includes a nickel-nitrogen doped carbon layer and manganese oxide;

[005...

Embodiment 3

[0055] Like the nickel-nitrogen co-doped porous carbon nanosheets provided in Example 1, the molar ratio of nickel acetate to manganese acetate is 1:1.5. The heating temperature of the mixed solution B is 120°C, and the baking temperature is 600°C. The prepared nickel-nitrogen The BET specific surface area of ​​the co-doped porous carbon nanosheets is 300m 2 / g.

[0056] As in Application Example 1, the nickel-nitrogen co-doped porous carbon nanosheets prepared in Example 3 are used as a catalyst to electrocatalyze CO reduction 2 The maximum Faraday efficiency for CO is about 85% (starting voltage is -0.5V).

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Abstract

A nickel-nitrogen codoped carbon electrocatalyst is provided and is nickel-nitrogen codoped porous carbon nanosheets. The invention also provides a preparing method of the electrocatalyst. The methodincludes a step of adding sodium benzoate, nickel acetate and manganese acetate into DMF, dissolving the materials, and then adding terephthalic acid to obtain a solution mixture; a step of heating the solution mixture to generate a metal-organic framework compound adopting Ni<2+> and Mn<2+> as center metal ions and the terephthalic acid as an organic ligand, and performing separation; a step of roasting the metal-organic framework compound in an ammonia atmosphere so that the terephthalic acid in the metal-organic framework compound is carbonized, the Ni<2+> and N form a coordinate bond and the Mn<2+> is converted into manganese oxide; and a step of removing the manganese oxide through acid washing to obtain the nanosheets. The provided electrocatalyst has high selectivity and high catalytic activity when applied for electrocatalytic reduction of CO2 into CO. The preparing method is easy to operate and reaction conditions are mild.

Description

Technical field [0001] The present invention relates to the technical field of energy and chemical industry, in particular to a nickel-nitrogen co-doped carbon electrocatalyst, and a preparation method and application thereof. Background technique [0002] Electrocatalytic CO 2 The reduction reaction is to convert CO 2 One of the most promising technologies for reduction and conversion into high value-added fuels. These high value-added products include methane, formic acid, CO and so on. Among these products, CO is an important chemical raw material, which is used in industrial production such as Fischer-Tropsch synthesis process and has received extensive attention in recent years. However, the development and application of this technology is limited by the low selectivity and low activity of the catalyst. [0003] In the past few years, scholars have devoted themselves to the research and development of highly selective CO 2 The electrocatalysts converted into CO mainly includ...

Claims

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Application Information

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IPC IPC(8): B01J27/24B01J35/02C25B1/00C25B11/06
Inventor 侯阳王馨悦杨彬李中坚雷乐成
Owner ZHEJIANG UNIV
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