Catalyst for producing formic acid by electroreduction of carbon dioxide and preparation method thereof

A technology of carbon dioxide and electrocatalyst, which is applied in the field of electrocatalysis, can solve the problems of difficult breakthrough of formic acid generation rate, reduction of formic acid Faradaic efficiency, sensitivity of current and potential, etc., and achieves the advantages of simple preparation method, high selectivity and high reactivity Effect

Active Publication Date: 2020-04-10
XIAMEN UNIV
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  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

Although some catalysts have been able to obtain higher carbon dioxide reduction selectivity by adjusting the structure, morphology and composition of the catalyst, the high selectivity is very sensitive to the applied current and potential.
Due to high current density (>60mA cm -2 ) competition reaction hydrogen evolution reaction activity increases, the faradaic efficiency of formic acid is significantly reduced, thus making it difficult for the formation rate of formic acid to exceed 1000 μmol h -1 cm -2

Method used

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  • Catalyst for producing formic acid by electroreduction of carbon dioxide and preparation method thereof
  • Catalyst for producing formic acid by electroreduction of carbon dioxide and preparation method thereof
  • Catalyst for producing formic acid by electroreduction of carbon dioxide and preparation method thereof

Examples

Experimental program
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Effect test

Embodiment 1

[0032] 16μmol thioacetamide and 0.4mmol InCl 3 Dissolve in 15mL DMF, stir vigorously for 15min, then transfer to a 25mL Teflon-lined stainless steel autoclave, and place in a clean 1×3cm 2 Carbon paper, sealed, heat-treated at 150°C for 12h; after cooling, the carbon paper was taken out, washed with deionized water, and dried to obtain S-doped In 2 o 3 Precursor; final in 0.5M KHCO 3 Electroreduction at -0.98V vs.RHE in the electrolyte for 5min yields a carbon paper-supported 4.9mol% S-doped In metal electrocatalyst (S-In), such as figure 1 Shown is a scanning electron microscope image of a 4.9% sulfur-doped metal indium electrocatalyst. The particle size of the sulfur-doped metal indium is about 130nm, and it is evenly loaded on the carbon fiber of the carbon paper. The catalyst is used as the cathode, the Pt sheet is used as the anode, and the saturated calomel electrode is used as the reference electrode, and the reaction is carried out in an H-type electrolytic cell. Bo...

Embodiment 2

[0035] 16μmol thioacetamide and 0.4mmol InCl 3 Dissolve in 15mL DMF, stir vigorously for 15min; then transfer to a 25mL PTFE-lined stainless steel autoclave, put in a clean 1×3cm 2 Carbon paper, sealed, heat-treated at 150°C for 12h; after cooling, the carbon paper was taken out, washed with deionized water, and dried to obtain S-doped In 2 o 3 Precursor; final in 0.5M KHCO 3 The carbon paper-supported 4.9mol% S-doped In metal electrocatalyst (S-In) was obtained by electroreduction at -0.98V vs. RHE in the electrolyte for 5min. The catalyst is used as the cathode, the Pt sheet is used as the anode, and the saturated calomel electrode is used as the reference electrode; the reaction is carried out in an H-type electrolytic cell, and both the cathode chamber and the anode chamber are 30mL 0.5M CsHCO 3 Electrolyte; carbon dioxide at a certain 20mLmin -1 The flow rate is passed into the catholyte, and the potential reaction of -0.98V vs. RHE is applied for 1h; the current dens...

Embodiment 3

[0037] 16μmol thioacetamide and 0.4mmol InCl 3Dissolve in 15mL DMF, stir vigorously for 15min; then transfer to a 25mL PTFE-lined stainless steel autoclave, put in a clean 1×3cm 2 Carbon cloth, sealed, heat treatment at 150°C for 12h; after cooling, the carbon cloth was taken out, washed with deionized water, and dried to obtain S-doped In 2 o 3 Precursor; final in 0.5M KHCO 3 The carbon cloth-supported 4.9mol% S-doped In metal electrocatalyst (S-In) was obtained by electroreduction at -0.98V vs. RHE in the electrolyte for 5 minutes. The catalyst is used as the cathode, the Pt sheet is used as the anode, and the saturated calomel electrode is used as the reference electrode; the reaction is carried out in an H-type electrolytic cell, and both the cathode chamber and the anode chamber are 30mL 0.5M KHCO 3 Electrolyte; carbon dioxide at a certain 20mL min -1 The flow rate is passed into the catholyte, and the potential reaction of -0.98V vs. RHE is applied for 1h; the curren...

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Abstract

The invention provides a catalyst for preparing formic acid from carbon dioxide by electroreduction and a preparation method of the catalyst, and belongs to the field of electro-catalysis. The catalyst is a chalcogen-doped metal electrocatalyst, chalcogen contains at least one of sulfur, selenium and tellurium, and metal contains at least one of indium, stannum, lead and bismuth. The preparation method comprises following steps: 1), an elementary substance of chalcogen or a compound of chalcogen is dissolved in N,N-dimethyl formamide with metal salts, a carbon material is placed, and a mixtureis transferred into a high-pressure kettle and subjected to solvent heat treatment; 2), after the solvent heat treatment, the carbon material is taken out, washed by deionized water and dried, a carbon material supported chalcogen-doped metal oxide precursor is obtained and then subjected to electroreduction, and the carbon material supported chalcogen-doped metal electrocatalyst is obtained. When applied to the reaction of preparing formic acid from carbon dioxide by electroreduction, the catalyst is high in reactivity, high in selectivity and stable in catalytic performance and maintains high formic acid selectivity in a wide current range.

Description

technical field [0001] The invention belongs to the field of electrocatalysis, in particular to a catalyst for producing formic acid by electroreducing carbon dioxide and a preparation method thereof. Background technique [0002] Catalytic conversion of carbon dioxide into high value-added chemicals or fuels can not only turn waste into wealth, reduce carbon dioxide emissions, but also convert renewable energy into high energy density fuel storage, which has important practical significance. Electricity can be generated from renewable energy sources such as solar and wind power, and has the advantages of being clean, gentle, and sustainable. Therefore, the conversion of CO2 into important fuels or chemicals through electrochemical methods is one of the most attractive ways to realize resource utilization of CO2. [0003] By comparing the energy input cost and market price of different products (such as carbon monoxide, methane, formic acid, ethane, and ethylene) of electro...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): B01J27/04B01J27/057C07C53/02C07C51/00
CPCB01J27/04B01J27/0573B01J27/0576B01J35/0033C07C51/00C07C53/02
Inventor 谢顺吉马文超张庆红王野
Owner XIAMEN UNIV
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