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Barium-barium-tantalum oxide solid electrolyte and preparation method thereof

A solid electrolyte and tantalum oxide technology, applied in the field of materials, can solve the problems of low proton transfer number, hydrogen measurement error, sensor display error, etc., achieve high proton transfer number, good conductivity, and improve accuracy

Active Publication Date: 2021-01-15
NORTHEASTERN UNIV LIAONING
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0011] in ABO 3 In the simple perovskite structure, doped CaZrO 3 The material with the highest proton migration number can reach 0.5 in an oxygen-containing atmosphere at 800°C, but when this material is used in the hydrogen measurement experiment of aluminum liquid, the sensor readings have a large error; in 1993, A.S.Nowic [4] found A 3 (B' 1+x B″ 2-x )O 9-δ Complex perovskite structure, where Ba 3 Ca 1.18 Nb 1.82 o 9-δ (BCN18) material has the highest electrical conductivity, which has attracted extensive attention and research, but its proton migration number at 700 °C can only reach 0.16; in the complex perovskite structure, Ba 4–x La x Ca 2 Nb 2 o 11+0.5x The proton migration number of the material is the highest, which can reach 0.35 at 700 °C, but the proton migration number of this material is still low, and there will be a lot of errors when measuring hydrogen, which is difficult to meet the needs of sensor work.

Method used

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  • Barium-barium-tantalum oxide solid electrolyte and preparation method thereof
  • Barium-barium-tantalum oxide solid electrolyte and preparation method thereof
  • Barium-barium-tantalum oxide solid electrolyte and preparation method thereof

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Experimental program
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Effect test

Embodiment 1

[0039] The molecular formula of barium barium tantalum oxide solid electrolyte is Ba 1.5 Ba 0.5+x Ta 1-x O 4.5-δ , where x=0, δ=0;

[0040] The preparation method is:

[0041] Prepare barium carbonate powder and tantalum oxide powder as raw materials; mix the raw materials in a molar ratio Ba:Ta=2:1 to make powder;

[0042] Using absolute ethanol as the ball-milling medium, the mixed powder was ball-milled to a particle size of less than 400 mesh, and then dried to remove the ball-milling medium to obtain ball-milling powder;

[0043]The ball mill powder is pressed into shape, then roasted at 1100°C for 5 hours, cooled to room temperature with the furnace, and the roasted material is obtained; the press shape is to place the ball mill powder in a mold, and use a press to shape it under a pressure of 30MPa;

[0044] Grind the calcined material to a particle size of 200 mesh or less, and then press it for the second time. The second press is to put the ground calcined mater...

Embodiment 2

[0047] The molecular formula of barium barium tantalum oxide solid electrolyte is Ba 1.5 Ba 0.5+x Ta 1-x o 4.5-δ , where x=0.05, δ=0.075;

[0048] Method is with embodiment 1, and difference is:

[0049] (1) The molar ratio of powder Ba:Ta=2.05:0.95;

[0050] (2) Carry out ball milling with water as the ball milling medium;

[0051] (3) Roasting at 1300°C for 1 hour; press molding under a pressure of 50MPa using a press machine;

[0052] (4) Press into tablets under 50MPa pressure during secondary pressing, use a cold isostatic pressing device under 200±10MPa pressure for 15min, and then calcinate at 1500°C for 1h;

[0053] Barium, barium and tantalum oxide solid electrolytes have a conductivity of 3.0×10 at a temperature of 400-800°C, an oxygen volume concentration of 3%, a water vapor volume concentration of 1.8%, and the rest in an argon atmosphere. -5 ~1.4×10 -4 S cm -1 , the proton transfer number is 0.97-0.49; the conductivity at 700 °C is 1.1×10 -4 S cm -1 , ...

Embodiment 3

[0055] The molecular formula of barium barium tantalum oxide solid electrolyte is Ba 1.5 Ba 0.5+x Ta 1-x o 4.5-δ , where x=0.15, δ=0.225;

[0056] Method is with embodiment 1, and difference is:

[0057] (1) The molar ratio of powder Ba:Ta=2.15:0.85;

[0058] (2) Roasting at 900°C for 10 hours; press molding under a pressure of 10MPa using a press machine;

[0059] (3) During the secondary pressing, it was compressed into tablets under a pressure of 10MPa, and the cold isostatic pressing device was used to press at a constant pressure of 200±10MPa for 30min; after calcination at 1000°C for 10h; the XRD diagram is as follows figure 2 shown;

[0060] Barium, barium and tantalum oxide solid electrolytes have a conductivity of 1.1×10 at a temperature of 400-800°C, an oxygen volume concentration of 3%, a water vapor volume concentration of 1.8%, and the rest in an argon atmosphere. -4 ~8.6×10 -4 S cm -1 , the proton transfer number is 0.95-0.50; the conductivity at 700°C ...

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Abstract

The invention discloses a barium-barium-tantalum oxide solid electrolyte and a preparation method thereof. The molecular formula of the electrolyte is Ba<1.5>Ba <0.5+x>Ta<1-x>O<4.5-delta>. The preparation method comprises the following steps of: (1) mixing barium carbonate powder and tantalum oxide powder according to a molar ratio (Ba: Ta) of (2+x): (1-x); (2) taking water or absolute ethyl alcohol as a ball milling medium, and drying the mixed powder after ball milling; (3) carrying out compression molding, then roasting at 900-1300 DEG C for 1-10 hours, and carrying out cooling along with the furnace; and (4) grinding the roasted material, carrying out secondary compression molding, calcining at 1000-1500 DEG C for 1-10 hours, and carrying out cooling along with the furnace. The oxygenvacancy lattice defect is generated by changing the stoichiometric ratio of the Ba element at the B' position to the Ta element at the B'' position, so that the formed electrolyte material has good conductivity under a high-temperature condition, and meanwhile, has a relatively high proton transference number; and the material is applied to sensor equipment, and is helpful for improving the accuracy of hydrogen measurement in a hydrogen sensor.

Description

technical field [0001] The invention belongs to the technical field of materials, in particular to a barium barium tantalum oxide solid electrolyte and a preparation method thereof. [0002] technical background [0003] Solid electrolytes are a class of materials that exhibit ionic conductivity in the solid state, and can be classified according to different carriers, such as Na + , O 2- , S 2- , H + etc.; in which H + The solid electrolyte material that conducts electricity for the carrier is a functional material that can conduct protons; the oxygen vacancies in the solid electrolyte lattice combine with hydrogen or water in the atmosphere to generate protons; according to the proton conduction of solid electrolytes at different temperatures The solid electrolyte can be used in different fields such as fuel cells, chemical sensors, aluminum liquid dehydrogenation, and ammonia synthesis. [0004] In perovskite solid electrolytes, there are mainly simple perovskite stru...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): C04B35/01C04B35/622C04B35/626B28B3/00B28B3/02G01N27/00
CPCB28B3/003B28B3/02C04B35/01C04B35/622C04B35/62655C04B35/62675C04B2235/3215C04B2235/3251C04B2235/5436C04B2235/656C04B2235/6567C04B2235/96G01N27/00
Inventor 厉英王泽众黄文龙
Owner NORTHEASTERN UNIV LIAONING
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