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A rare earth element-doped perovskite-type supported ruthenium ammonia synthesis catalyst

A rare earth element, perovskite-type technology, applied in catalyst supports, physical/chemical process catalysts, ammonia preparation/separation, etc., can solve the problem of reducing catalyst stability and life, low ammonia synthesis activity, and no industrialized application value. and other problems, to achieve the effects of inhibiting hydrogen adsorption, low noble metal dosage, and improved low temperature and low pressure ammonia synthesis activity

Inactive Publication Date: 2016-05-04
FUZHOU UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

However, the contact between carbon materials and ruthenium makes methanation reaction prone to occur under ammonia synthesis conditions, which reduces the stability and life of the catalyst, thus adversely affecting the industrial application of ruthenium catalysts.
Therefore, the preparation of highly active ruthenium-based ammonia synthesis catalysts using highly stable oxide materials instead of activated carbon as a carrier has become a research hotspot in this field; the common oxide carriers in the field of ruthenium-based ammonia synthesis catalysts are mainly Al 2 o 3 , MgO, rare earth oxides and other porous nanomaterials have low ammonia synthesis activity under low temperature and low pressure conditions, and have no industrial application value

Method used

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Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0041] Ba(NO 3 ) 2 :Zr(NO 3 ) 4 . 5H 2 O:Y(NO 3 ) 3 . 6H 2 O: The mixture with the molar ratio of citric acid 1:0.9:0.1:3.0 was dissolved in an appropriate amount of distilled water to obtain a colorless clear viscous liquid. The solution was slowly heated in a water bath at 80°C for 4h to evaporate excess water, and then heated at a constant temperature of 90°C for 12h to promote the gelation of the mixture. Finally, the obtained yellow gel was calcined at 300 °C for 1 h to obtain the precursor, and then calcined at 1000 °C for 10 h to obtain BaZr 0.9 Y 0.1 o 2.95 carrier material. The active component ruthenium was impregnated into the carrier by equal volume impregnation method, and then reduced with absolute ethanol. The active component Ru accounted for 2% of the mass fraction of the carrier. The catalyst is at 3MPa and the space velocity is 10000h -1 At 350°C, 375°C, 400°C and 425°C, the outlet ammonia concentrations were 2.42%, 5.80%, 7.86% and 7.75%, resp...

Embodiment 2

[0043] Catalyst preparation method is the same as embodiment 1, but BaZr 0.9 Y 0.1 o 2.95 The calcination temperature of the precursor is 800°C, and other conditions are the same. Get BaZr 0.9 Y 0.1 o 2.95 The specific surface area is 9.97m 2 .g -1 , the ruthenium catalyst was obtained by equal volume impregnation method. At 3MPa, the space velocity is 10000h -1 At 350°C, 375°C, 400°C and 425°C, the outlet ammonia concentrations were 2.13%, 4.72%, 7.03% and 7.69%, respectively.

Embodiment 3

[0045] Catalyst preparation method is the same as embodiment 1, but BaZr 0.9 Y 0.1 o 2.95 The calcination temperature of the precursor is 1100°C, and other conditions are the same. Get BaZr 0.9 Y 0.1 o 2.95 The specific surface area is 6.69m 2 .g -1 , the ruthenium catalyst was obtained by equal volume impregnation method. At 3MPa, the space velocity is 10000h -1 At 350°C, 375°C, 400°C and 425°C, the outlet ammonia concentrations were 0.46%, 0.92%, 2.06% and 4.15%, respectively.

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Abstract

The invention discloses a BaZrO3-δ-based perovskite-type supported ruthenium ammonia synthesis catalyst doped with rare earth elements and a preparation method thereof. The ruthenium-based ammonia synthesis catalyst is BaZrO3-δ-based perovskite doped with rare earth elements The type composite oxide is the carrier, the molecular formula is Ba1-xLnx+yZr1-yO3-δ, and metal ruthenium is the active component. The doping amount of rare earth elements is 1-20% of the total mass of the carrier, and the active component uses K2RuO4 as a precursor, which is directly impregnated into the carrier material, and the loading amount is 0.5%-10% of the weight of the carrier in terms of Ru. The preparation method of the invention is simple, the equipment is simple, no additives need to be added, the amount of noble metal is low, and the prepared catalyst has good activity at low temperature and low pressure and high stability.

Description

technical field [0001] The invention relates to a BaZrO doped with rare earth elements, which takes metal ruthenium as the active component 3-δ The invention discloses an ammonia synthesis catalyst and a preparation method of a perovskite-based carrier loaded with ruthenium, which belong to the technical field of fertilizer catalysts and are applied to the synthesis of ammonia from a mixture of hydrogen and nitrogen. Background technique [0002] The ruthenium-based ammonia synthesis catalyst is known as the second-generation ammonia synthesis catalyst after the molten iron catalyst, and has the characteristics of low temperature, low pressure and high activity. Among them, the ruthenium-based ammonia synthesis catalyst supported by graphitized activated carbon materials has achieved industrial application in the 1990s. Chinese patents CN101362080A and CN101053834A disclose an ammonia synthesis catalyst with ruthenium as an active component, activated carbon as a carrier, a...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): B01J23/63B01J32/00C01C1/04
CPCY02P20/52
Inventor 林建新马运翠王自庆倪军林炳裕魏可镁
Owner FUZHOU UNIV
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