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Catalyst for preparing multi-carbon product by electro-reduction of carbon dioxide and carbon monoxide and preparation method and application thereof

A carbon dioxide and carbon monoxide technology, applied in the field of electrocatalysis, can solve the problems of narrow reaction window and low activity, and achieve the effects of high selectivity, high reaction activity and simple and easy preparation method.

Active Publication Date: 2020-06-05
XIAMEN UNIV
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  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

Although some copper-based electrocatalyst systems have been able to obtain higher carbon dioxide and carbon monoxide reduction selectivities by adjusting the structure, morphology, and composition of copper-based catalysts, as well as the design and control of electrolytic cells and electrolytes, the activity is generally Low, and narrow reaction window under most conditions

Method used

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  • Catalyst for preparing multi-carbon product by electro-reduction of carbon dioxide and carbon monoxide and preparation method and application thereof
  • Catalyst for preparing multi-carbon product by electro-reduction of carbon dioxide and carbon monoxide and preparation method and application thereof
  • Catalyst for preparing multi-carbon product by electro-reduction of carbon dioxide and carbon monoxide and preparation method and application thereof

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0037] 0.2mmol NH 4 HF 2 and 0.2mmol Cu(NO 3 ) 2 ·3H 2O was dissolved in 50 mL of DMF, stirred vigorously for 15 min, then transferred to a 100 mL PTFE-lined stainless steel autoclave, sealed, and heat-treated at 160 °C for 4 h; cooled, washed with deionized water and ethanol, and dried to obtain Cu(OH )F precursor, the X-ray diffraction pattern of Cu(OH)F is as follows figure 1 shown; then Cu(OH)F was loaded on the gas diffusion layer with a load of 0.5 mg cm -2 ;Finally, the fluorine-modified copper electrocatalyst (F-Cu) was obtained by electroreduction at -0.6Vvs.RHE in 1.0M KOH electrolyte for 5min. The catalyst is used as the cathode, the nickel foam is used as the anode, and the saturated Ag / AgCl electrode is used as the reference electrode, and the reaction is carried out in a flow electrolytic cell. The configuration of the flow electrolytic cell is as follows: figure 2 Shown; cathode chamber and anode chamber are 1.0M KOH electrolyte; carbon dioxide in 50mL mi...

Embodiment 2

[0039] 1.0mmol NH 4 HF 2 and 0.5mmol Cu(OAc) 2 Dissolve in 100mL DMF, stir vigorously for 15min, then transfer to a 200mL PTFE-lined stainless steel autoclave, seal, heat at 180°C for 3h; cool, wash with deionized water and ethanol, and dry to obtain Cu(OH) F precursor; then Cu(OH)F was loaded on the gas diffusion layer with a loading of 0.25 mg cm -2 ;Finally, the F-Cu catalyst was obtained by electroreduction at -0.7V vs. RHE for 5min in 2.5M NaOH electrolyte. The catalyst was used as the cathode, the nickel foam was used as the anode, and the saturated Ag / AgCl electrode was used as the reference electrode, and the reaction was carried out in a flow electrolytic cell; both the cathode chamber and the anode chamber were 2.5M NaOH electrolyte; -1 The flow rate is passed into the cathode, and different negative currents are applied for 0.5h.

[0040] Such as image 3 As shown, change the current density applied to the F-Cu catalyst from -400 to -1200mA cm -2 , the faradai...

Embodiment 3

[0042] 0.3mmol NH 4 HF 2 and 0.2mmol CuNO 3 ·3H 2 O was dissolved in 50 mL of DMF, stirred vigorously for 15 min, then transferred to a 100 mL PTFE-lined stainless steel autoclave, sealed, and heat-treated at 160 °C for 6 h; cooled, washed with deionized water and ethanol, and dried to obtain Cu(OH )F precursor; then Cu(OH)F is supported on the gas diffusion layer with a loading of 1.0 mg cm -2 ;Finally, the F-Cu catalyst was obtained by electroreduction at -1.5V vs. RHE for 5min in 0.75M KOH electrolyte. The catalyst is used as the cathode, the nickel foam is used as the anode, and the saturated Ag / AgCl electrode is used as the reference electrode, and the reaction is carried out in a flow electrolytic cell; both the cathode chamber and the anode chamber are 0.75M KOH electrolyte; carbon dioxide is passed into the cathode at different flow rates , apply -1600mA cm -2 Current response 0.5h.

[0043] Such as Figure 4 As shown, when the carbon dioxide flow rate is 20mL m...

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Abstract

The invention discloses a catalyst for preparing a multi-carbon product by electro-reduction of carbon dioxide and carbon monoxide as well as a preparation method and application thereof, and belongsto the field of electro-catalysis. The catalyst is a halogen-modified copper electro-catalyst, and halogen comprises at least one of fluorine, chlorine, bromine and iodine. The preparation method of the catalyst comprises the following steps: loading a copper halide precursor on a gas diffusion layer, and carrying out electric reduction to obtain the halogen-modified copper electro-catalyst, wherein the copper halide precursor comprises at least one of a fluorine copper hydroxide precursor and other copper halide precursors except the fluorine copper hydroxide precursor. The catalyst is applied to a reaction for preparing a multi-carbon product by electrically reducing carbon dioxide and carbon monoxide, is high in reaction activity, high in selectivity and stable in catalytic performance,and maintains very high multi-carbon product selectivity in a very wide current range.

Description

technical field [0001] The invention belongs to the field of electrocatalysis, in particular to a catalyst for electroreducing carbon dioxide and carbon monoxide to produce multi-carbon products, a preparation method and application thereof. Background technique [0002] Catalytic conversion of carbon dioxide and carbon monoxide into high value-added chemicals and fuels can not only solve the depletion of fossil energy, but also alleviate carbon emissions, which has important practical significance. On the other hand, the synthesis of multi-carbon products (such as ethylene, ethanol, acetic acid, and n-propanol, etc.) has received extensive attention due to their wide applications in chemical and energy fields. Traditional thermocatalytic carbon dioxide or carbon monoxide hydrogenation can achieve high yields of multi-carbon products under high temperature and high pressure conditions, but multi-carbon products are diverse and widely distributed, accompanied by the generatio...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J27/06B01J27/122B01J23/72C25B3/04C25B11/06C25B3/25
CPCB01J27/06B01J27/122B01J23/72C25B3/25C25B11/091B01J35/33
Inventor 谢顺吉马文超张庆红王野
Owner XIAMEN UNIV
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