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CN-122000370-A - Electrode material and preparation method and application thereof

CN122000370ACN 122000370 ACN122000370 ACN 122000370ACN-122000370-A

Abstract

The invention relates to the technical field of fuel cells, in particular to an electrode material, a preparation method and application thereof. The electrode materials being mixed in solid phase Is a precursor, and is obtained by in-situ reduction. Wherein x is more than or equal to 0 and less than or equal to 0.3, y is more than or equal to 0 and less than or equal to 0.3, z is more than or equal to 0 and less than or equal to 0.3, and delta is oxygen vacancy content. The preparation method of the electrode material is simple, convenient, economical and high in repeatability, and the reaction condition is mild and controllable. When the electrode material is applied as a solid oxide electrolytic cell and a fuel electrode of a fuel cell, the electrode material has excellent electrochemical performance when the hydrocarbon fuel is subjected to electrochemical oxidation power generation and carbon dioxide electrolytic reduction.

Inventors

  • GAN TIAN
  • ZHOU XINYU
  • HAN YUJUN
  • Che Xianzhi
  • ZHEN WENYA

Assignees

  • 苏州科技大学

Dates

Publication Date
20260508
Application Date
20260130

Claims (10)

  1. 1. An electrode material characterized in that the electrode material is mixed by a solid phase And Is obtained by in-situ reduction of a precursor, wherein x is more than or equal to 0 and less than or equal to 0.3, y is more than or equal to 0 and less than or equal to 0.3, z is more than or equal to 0 and less than or equal to 0.3, delta is oxygen vacancy content, and the oxygen vacancy content is equal to or less than or equal to 0 and less than or equal to 0.3 The mass percentage of the catalyst is 50% -70%, and the mass percentage of the catalyst is 50%) The mass percentage of the catalyst is 30% -50%.
  2. 2. The electrode material of claim 1, wherein the electrode material exhibits an oxygen-enriched vacancy perovskite structure comprising uniformly distributed active metal nanoparticles, the active metal nanoparticles being an FeSn alloy phase.
  3. 3. The electrode material of claim 1, wherein the Is prepared from praseodymium, strontium, lithium, iron, tin and molybdenum ions by taking the quantity of the target elements as the molar ratio.
  4. 4. A method for producing an electrode material according to any one of claims 1 to 3, comprising the steps of: s1, putting nitrate of praseodymium, strontium, lithium, iron, tin and molybdenum into water for mixing and dissolving, adding ammonia water solution dissolved with a chelating agent, and uniformly mixing to obtain a solution A; s2, adding citric acid into the solution A, adjusting the pH value of the solution A to be within a range of 5-8, and stirring at a temperature of 80-90 ℃ to perform chemical reaction to obtain sol A; S3, drying the sol A at a temperature of 100-120 ℃, and then transferring to a temperature of 950-1200 ℃ for calcination to obtain ; S4, putting the nitrate of samarium and cerium into water for mixing and dissolving, adding the alkaline solution dissolved with ethylenediamine tetraacetic acid, and uniformly mixing to obtain a solution B; s5, adding citric acid into the solution B, adjusting the pH value of the solution B to be within a range of 5-8, and stirring at a temperature of 80-90 ℃ to perform chemical reaction to obtain sol B; S6, drying the sol B at a temperature of 100-120 ℃, and then transferring to a temperature of 650-750 ℃ for calcination to obtain ; S7, the step of And said And mixing, performing ball milling treatment, calcining at 700-800 ℃ in an air atmosphere, and performing reduction treatment at 650-800 ℃ in a mixed gas atmosphere of hydrogen and argon to obtain the electrode material.
  5. 5. The method according to claim 4, wherein the total concentration of metal ions in the sol A and the sol B is any one of 0.2 to 0.45 mol/L; In step S1, the molar ratio of the chelating agent to the total metal ions in the sol A is (1.5-2): 1, and in step S4, the molar ratio of the chelating agent to the total metal ions in the sol B is (1.5-2): 1.
  6. 6. The method according to claim 4, wherein the chelating agent is any one of ethylenediamine tetraacetic acid, glycine, ethylene glycol and oxalic acid.
  7. 7. The method according to claim 4, wherein the molar ratio of the citric acid to the total metal ion solution in the solution A is (1-1.1): 1; in the solution B, the molar ratio of the citric acid to the total metal ion solution in the solution B is (1-1.1): 1.
  8. 8. The method according to claim 4, wherein in step S7, sieving is performed after the completion of the calcination treatment, and a 180-300 mesh sieve is selected for the sieving treatment.
  9. 9. The method according to claim 4, wherein in the step S7, the flow rate of the hydrogen gas is any one of 50mL/min to 100mL/min, and the volume of the hydrogen gas is 5% -10% of the mixed gas.
  10. 10. The use of an electrode material according to any one of claims 1 to 3 in hydrocarbon fuel solid oxide fuel cells and solid oxide cells for electrochemical reduction of carbon dioxide.

Description

Electrode material and preparation method and application thereof Technical Field The invention relates to the technical field of electrode material preparation, in particular to an electrode material, a preparation method and application thereof. Background The excessive use of fossil fuels causes problems such as climate change and global warming, and solid oxide cells (Solid Oxide Cells, SOCs) are of great interest as key efficient clean energy conversion technologies. Solid oxide cells mainly include Solid Oxide Fuel Cells (SOFCs) for power generation and Solid Oxide Electrolysis Cells (SOECs) that electrochemically convert CO 2 or H 2 O to CO or H 2. The SOECs have the advantages of low overpotential, high energy efficiency and the like, can be coupled with intermittent renewable energy sources such as wind energy, solar energy and the like and nuclear energy and industrial waste heat systems, and are considered to be an effective way for realizing the purposes of CO 2 resource utilization and carbon neutralization. However, efficient, stable cathode materials for high temperature CO 2 electroreduction reactions (CO 2 RR) remain a key bottleneck limiting the technological development. Perovskite oxide (ABO 3) has great prospect in the field of high-temperature electrochemical application due to the ion-electron mixed conductivity, carbon deposition resistance and thermal/redox stability, but compared with a commercial nickel-based ceramic cathode, the perovskite oxide (ABO 3) has insufficient dynamic performance of the reduction reaction of CO 2 (CO 2 RR). Most unmodified perovskite oxides have poor cathode catalytic activity, and long-term exposure to pure CO 2 environment at high temperature can lead to destabilization of crystal structure and performance decay. Taking the common Sr 2Fe1.5Mo0.5O6−δ (SFM) perovskite as an example, the intrinsic reactivity of lattice oxygen is low, and the adsorption and activation of CO 2, the formation of oxygen vacancies and the ion migration of bulk O 2- are limited, so that the kinetics of CO 2 RR are slow. At present, modification strategies such as morphology regulation, surface engineering, chemical doping and the like are developed for improving the CO 2 electrolysis catalytic performance of perovskite oxides. Among them, the impregnation method is effective, but the preparation temperature is low, so that the impregnated nano particles are easy to be Wen Cuhua high. Another efficient approach is to dope the perovskite oxide with low valence metal ions at the a-site or/and B-site to create oxygen vacancies to enhance its activity. In addition, the introduced catalyst metal doping element is separated out under a specific condition to form nano particles, so that the catalytic activity can be improved, for example, the SFM perovskite doped with Bi, ni, co, ir, cu and other elements can be obviously improved in the CO 2 electrolysis performance. For example, co 7W6@WOx nano particles dispersed on the surface of La 0.4Sr0.6TiO3 and precipitated nano particles with Co-Fe@CoFeO 4 core-shell structures on the surface of LaBaMn 2O5 can expand the three-phase boundary and promote the catalytic activity and the anti-carbon deposition performance, which is mainly beneficial to the synergistic effect of the core-shell structure and the oxygen vacancy active site. In addition, the perovskite oxide and oxygen ion conductor (such as doped cerium oxide) cooperate to enhance the CO 2 RR performance. However, when the composite cathode is prepared by adopting a mechanical grinding or dipping method, the problems of complex process, uneven distribution and the like exist. On the other hand, no material or preparation method has been reported so far to achieve the above advantages at the same time. Therefore, there is a need to develop a novel solid oxide battery electrode material to solve the above-described problems. Disclosure of Invention The invention aims to provide an electrode material and a preparation method thereof, which are used for solving the problems of complicated preparation process, uneven distribution of doped elements and low oxygen activity of the existing electrode material in the prior art. The invention also provides application of the electrode material to improve the overall efficiency of the battery or the electrolytic cell. The electrode material is obtained by in-situ reduction of Pr ySr2-x-yLixFe1.5-zSnzMo0.5O6–δ and Ce 0.8Sm0.2O1.9 which are mixed in a solid phase, wherein x is more than or equal to 0 and less than or equal to 0.3, y is more than or equal to 0 and less than or equal to 0.3, z is more than or equal to 0 and less than or equal to 0.3, delta is oxygen vacancy, the mass percent of Pr ySr2-x-yLixFe1.5-zSnzMo0.5O6–δ is 50% -70%, and the mass percent of Ce 0.8Sm0.2O1.9 is 30% -50%. Further, the electrode material presents an oxygen-enriched vacancy perovskite structure comprising uniformly distributed active metal nanoparticles, wherein