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Method for electrocatalytically reducing carbon dioxide based on chip on flex (COF)-metal interface synergistic effect

A technology of synergy and carbon dioxide, applied in the direction of electrodes, electrolytic components, electrolytic processes, etc., can solve the problems of low efficiency and no selectivity, and achieve the effects of easy adjustment, improved selectivity, and guaranteed catalytic activity

Active Publication Date: 2018-11-06
WUHAN UNIV
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  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0003] However, for the metal catalytic system, due to the relatively flat energy band structure in the metal, although it has high catalytic activity, it does not have specific selectivity, especially in the electrocatalytic reduction of carbon dioxide in the water system, the hydrogen evolution reaction Compared with the carbon dioxide reduction reaction, it is better; on the other hand, for the molecular catalytic system, because its front orbital is better matched with a specific molecule (such as carbon dioxide), it has better reaction selectivity, but it is limited by the catalytic active center. Limitations, as well as the influence of the conductivity of the molecular catalytic system compound itself, make its efficiency not high

Method used

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  • Method for electrocatalytically reducing carbon dioxide based on chip on flex (COF)-metal interface synergistic effect
  • Method for electrocatalytically reducing carbon dioxide based on chip on flex (COF)-metal interface synergistic effect
  • Method for electrocatalytically reducing carbon dioxide based on chip on flex (COF)-metal interface synergistic effect

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Experimental program
Comparison scheme
Effect test

Embodiment 1

[0024] 1. Synthesis and activation of a three-dimensional covalent organic framework (COF-300) based on imine bonding

[0025] Following the method in the literature [J.Am.Chem.Soc.,2009,131,4570-4571], 100mg of tetraaminophenylmethane and 64mg of terephthalaldehyde were dissolved in 2mL of 1,4-dioxane, and then Add it into the glass tube, and exchange the atmosphere in the glass tube with argon, and seal the tube after freezing in liquid nitrogen; place the glass tube in a 120°C oven for 3 days, then filter the solid, and put the resulting solid in 1,4-dioxane and acetone were used for reflux activation in a Soxhlet extractor, followed by activation with supercritical carbon dioxide to obtain a yellow covalent organic framework material based on imine bonding, namely activated COF -300 powder.

[0026] 2. Preparation of COF-300-AR Based on Amine Bonding

[0027] Add 57.6 mg (1 equivalent) of terephthalic acid and 50 mg (1 equivalent, based on the number of imine bonds) of a...

Embodiment 2

[0028] Example 2: Preparation of COF-metal electrodes

[0029] Put 5 mg of COF-300-AR powder in a mixed solution system formed by 0.75 mL of deionized water, 0.25 mL of ethanol, and 40 μL of 5% Nafion solution, ultrasonically disperse for 5 minutes, then take 100 μL of the dispersion, and slowly drop it onto silver foil (purchased from AlfaAesar) and dried under an infrared lamp to obtain a COF-silver electrode.

Embodiment 3

[0031] The COF-metal interface on the COF-silver electrode constructed of COF-300-AR and silver foil was characterized by scanning electron microscope and EDX energy spectrum, as shown in figure 1 As shown in (C-F), it is found that the COF-metal interface is clear and the morphology is relatively uniform. The thickness of the COF-300-AR layer is about 15 microns. The schematic diagram of the interface is shown in figure 1 (A) shown.

[0032] At the same time, spectrum technology was used to characterize the interaction mode between COF-300-AR and carbon dioxide molecules, and it was found that it contained an amide-like structure, which made us believe that COF-300-AR has the function of enriching and transferring carbon dioxide in the synergistic interface. Further embodies the advantages of this cooperative interface in catalytic reactions.

[0033] The COF-300-AR is interacted with isotope-labeled carbon dioxide, and the mechanism of the COF-metal electrode catalytic syst...

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Abstract

The invention discloses a method for electrocatalytically reducing carbon dioxide based on a chip on flex (COF)-metal interface synergistic effect. A porous covalent organic framework material rich inan -NH- group and a metal electrode are compounded to form a synergistic interface, so that the electrocatalytic activity and the carbon dioxide selectivity are greatly improved without changing theFermi level of the metal electrode. According to the method, carbon dioxide can be reduced if only an electron exists on the interface formed by the metal electrode and a COF material instead of passing through the organic framework, so that the reduction efficiency of the carbon dioxide cannot be limited by the electrical conductivity of the COF material; and compared with a method for modifyingan organic amine molecule on the surface of the electrode, according to the method, the COF material has a better crystal structure and an ordered pore-channel structure so as to have a positive effect on diffusing the carbon dioxide to the surface of the electrode, the selectivity is improved, and meanwhile, an carbon dioxide molecule is not prevented from being diffused to the surface of the electrode, so that a traditional metal electrode is modified.

Description

technical field [0001] The invention belongs to the field of energy catalysis application of porous crystalline materials, and specifically relates to the application of a crystalline porous material with high chemical stability based on C-N single bond connection and a metal electrode to form a synergistic interface to jointly catalyze the electroreduction of carbon dioxide. Background technique [0002] Electrocatalytic carbon dioxide reduction is an efficient and sustainable energy conversion method, which can convert readily available electrical energy into chemical energy for conversion, storage and utilization [Chem.Rev.2010, 110, 6474; Chem.Soc.Rev .2014, 43, 631-675; Adv. Mater. 2016, 28, 3423-3452]. [0003] However, for the metal catalytic system, due to the relatively flat energy band structure in the metal, although it has high catalytic activity, it does not have specific selectivity, especially in the electrocatalytic reduction of carbon dioxide in the water sy...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): C25B1/00C25B11/03C25B11/06
CPCC25B1/00C25B11/031C25B11/057C25B11/075
Inventor 邓鹤翔庄林刘昊宇蔡欣尹征磊
Owner WUHAN UNIV
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