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Solid oxide battery based on LSCF anode, preparation method of solid oxide battery and application of solid oxide battery in preparation of ethylene and ethane through oxidative coupling of methane

A solid oxide, LSCF-SDC technology, applied in the field of comfort and electrochemistry, can solve the problems of limited yield of C2 products, and achieve the effects of good thermoelectric reaction stability, high oxygen transport performance, and low price.

Pending Publication Date: 2022-07-08
FUJIAN AGRI & FORESTRY UNIV
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Problems solved by technology

However, the reaction is usually carried out at higher temperature, and the yield of C2 products is obviously limited

Method used

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  • Solid oxide battery based on LSCF anode, preparation method of solid oxide battery and application of solid oxide battery in preparation of ethylene and ethane through oxidative coupling of methane
  • Solid oxide battery based on LSCF anode, preparation method of solid oxide battery and application of solid oxide battery in preparation of ethylene and ethane through oxidative coupling of methane
  • Solid oxide battery based on LSCF anode, preparation method of solid oxide battery and application of solid oxide battery in preparation of ethylene and ethane through oxidative coupling of methane

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0055] A series of ABOs 3 type perovskite material La 0.75 Sr 0.25 Cr 0.5 Fe 0.5+x O 3-δ (LSCrF x , x=0, LSCrF 0 ;x=0.025, LSCrF 0.025 ;x=0.05, LSCrF 0.05 ;x=0.075, LSCrF 0 .075 ;x=0.1, LSCrF 0.1 ) materials were synthesized by the liquid phase combustion method, and the LSCF in the oxidized state and the reduced state were x The powder was analyzed by XRD test. Figure 2(a) is the diffraction pattern of the oxidation state of the material, compared with the standard card PDF#01-075-0441, it can be seen that LSCrF x It is a pure perovskite phase, indicating a cubic structure with a space group of Pm-3m. figure 2 (b) for the material at 5 wt % H 2 The XRD diffraction pattern after pretreatment at 850 °C for 20 hours in an atmosphere of / 95wt% Ar shows that a metallic iron peak appears at 45.1 ° (PDF#96-230-0201). This clearly shows that after H 2 After / Ar pretreatment, the excess metallic iron at the B site can be converted from La 0.75 Sr 0.25 Cr 0.5 Fe 0.5...

Embodiment 2

[0057] (a) Zr 0.8 Y 0.2 O 2-δ The (YSZ) powder is pressed into a disc using a tablet press, and then placed in a muffle furnace for heat treatment at a temperature of 1500-1550 °C for 10-15 hours to obtain a dense solid ceramic electrolyte support;

[0058] (b) The different series of LSCrF x Powder and Ce 0.8 Sm 0.2 O 2-δ (SDC) was mixed at a ratio of 65:35, and then 10% by mass of ethyl cellulose and 5% of starch were added for uniform mixing. Finally, the mixed powder is uniformly ground, and 1-10 mL of turpentine is added dropwise during the grinding process, and the LSCrF required for the experiment is obtained by grinding for 3-5 hours. x -SDC composite electrode slurry, in which the LSCrFx powder is La 0.75 Sr 0.25 Cr 0.5 Fe 0.5+xO 3-δ (LSCrF x , x=0, LSCrF 0 ;x=0.025, LSCrF 0.025 ;x=0.05, LSCrF 0.05 ;x=0.075, LSCrF 0 .075 ;x=0.1, LSCrF 0.1 )

[0059] (c) The cathode electrode paste LSCrF-SDC was uniformly printed on one side of the electrolyte suppo...

Embodiment 3

[0064] image 3 for different series of La 0.75 Sr 0.25 Cr 0.5 Fe 0.5+x O 3-δ Analysis results of anodic methane oxidation to ethylene and ethane. Supply 100 % concentration of CH to the anode 4 , and apply a voltage of 1.0-1.4 V while analyzing the products in the anode off-gas stream using on-line gas chromatography. As can be seen from Fig. 3(a) and Fig. 3(b), when the applied potential increases, the methane conversion also increases. When 1.4 V is applied, LSCrF 0.075 The methane conversion reached 11.7 % and the selectivity (C2) was found to be 15.5 %. Meanwhile, H was detected during the reaction 2 O and CO 2 The formation of , which is unavoidable during the reaction. from image 3 (c) It can be seen that as the applied potential increases, the LSCF 0.075 The yield of C2 product reaches a maximum of 1.8% at 1.4 V. with LSCrF without metal-oxide interface (no in situ precipitated Fe) 0 Compared to LSCrF 0.075 The constructed metal-oxide interface incr...

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Abstract

The invention discloses a solid oxide battery based on an LSCF anode and a method for preparing ethylene and ethane by coupling secondary enhanced electrochemical oxidation methane. According to the LSCF anode material, an iron element is separated out on a La < 0.75 > Sr < 0.25 > Cr < 0.5 > Fe < 0.5 + x > O < 3-delta > substrate through desolvation, and a metal-oxide interface is constructed. Methane oxidative coupling is carried out by applying a stable voltage of 1.0-1.4 V between the cathode and the anode of the oxide cell at the temperature of 800-850 DEG C, and methane gas is directly subjected to contact reaction at the anode end to generate ethylene and ethane with certain mass. The prepared anode material based on La < 0.75 > Sr < 0.25 > Cr < 0.5 > Fe < 0.5 + x > O < 3-delta > has extremely high electrochemical reaction performance and carbon deposition resistance, and has positive significance in preparation of ethylene and ethane materials and storage of renewable electric energy.

Description

technical field [0001] The present invention relates to the technical field of comfort and electrochemistry, in particular to a solid oxide battery based on an LSCF anode, a preparation method thereof, and an application in the oxidative coupling of methane to produce ethylene and ethane. Background technique [0002] The economical natural gas (CH 4 ) into high-energy-density fuels and high-value-added chemicals has become the research direction of many scholars. Methane can be converted into high value-added ethane and ethylene (C2) chemicals through oxidative coupling reactions (OCM) compared to the energy-intensive methods of indirect conversion of methane to syngas. CH 4 Direct conversion to ethane and ethylene (C2 products) is a challenging route, but it is both environmentally friendly and economical. Oxidative Coupling of Methane (OCM) directly converts methane to (C2 product). However, the reaction is usually carried out at higher temperatures and the yield of ...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): C25B11/047C25B9/17C25B3/29C25B3/23C04B35/48C04B35/622
CPCC25B11/047C25B9/17C25B3/29C25B3/295C25B3/23C04B35/48C04B35/622C04B2235/3225Y02E60/50
Inventor 甘丽珍张优凯
Owner FUJIAN AGRI & FORESTRY UNIV
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