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Ruthenium ammonia synthesis catalyst taking ruthenium ammonia complex as precursor

A technology for the synthesis of ammonia complexes and ammonia, which is applied in the direction of physical/chemical process catalysts, metal/metal oxide/metal hydroxide catalysts, preparation/separation of ammonia, etc., and can solve the problem of affecting catalyst production efficiency and low catalyst cost performance , large amount of residual chloride ions, etc., to achieve the effects of improved preparation efficiency, strong anti-sintering ability, and high utilization rate

Active Publication Date: 2012-10-03
福建三聚福大化肥催化剂国家工程研究中心有限公司 +1
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0003]U.S. Patent (U. S. Patent 4 600 571; U. S. Patent 4 142 993) using ruthenium chloride as a precursor has a cumbersome preparation process, complex preparation equipment, and relatively difficult industrialization Large; Chinese patents (CN161148A, CN1270081A, CN101053834A, 200810071876.X) use ruthenium chloride as a precursor, use hydrogen or hydrazine hydrate to reduce, or use precipitation to prepare ruthenium-based ammonia synthesis catalysts. The residual amount of chloride ions is large, and the preparation The efficiency is low, which affects the production efficiency of the catalyst, and the cost performance of the catalyst is low

Method used

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Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0034] Take 0.40 grams of ruthenium powder, add 1.15 grams of potassium nitrate and 0.64 grams of potassium hydroxide in a nickel crucible and mix evenly, place it in a muffle furnace at 600 °C for 1 hour, and dissolve the ruthenium with 10 ml of deionized water after cooling to room temperature Potassium ruthenate, at room temperature, add aqueous solution of potassium ruthenate to ammonia solution (ratio of ammonia to ruthenium is 6:1, ammonia solution 2 milliliters), adjust the pH of the solution to 2 with nitric acid after the addition is completed, Add 10% barium (based on the mass of activated carbon, and barium nitrate as the precursor), dissolve it, impregnate it with equal volume, and dry it. A series of ammonia synthesis catalysts with different ratios of barium to ruthenium can be prepared by changing the added amount of ruthenium complex and additives. The ratio of hydrogen to nitrogen in the mixed gas is 3:1, and the space velocity is 10000 h -1 , the reaction pr...

Embodiment 2

[0036]Take 0.40 grams of ruthenium powder, add 1.15 grams of potassium nitrate and 0.64 grams of potassium hydroxide in a nickel crucible and mix evenly, place it in a muffle furnace at 600 °C for 1 hour, and dissolve the ruthenium with 10 ml of deionized water after cooling to room temperature Potassium ruthenate, at room temperature, add aqueous solution of potassium ruthenate to ammonia solution (ratio of ammonia to ruthenium is 6:1, ammonia solution 2 milliliters), adjust solution pH= 4. Add 10% barium (based on the quality of activated carbon, barium nitrate as the precursor), dissolve and impregnate with equal volume, and dry. A series of ammonia synthesis catalysts with different ratios of barium to ruthenium can be prepared by changing the added amount of ruthenium complex and additives. The ratio of hydrogen to nitrogen in the mixed gas is 3:1, and the space velocity is 10000 h -1 , the reaction pressure is 10 MPa, and the reaction temperature is 400 ℃, the ammonia s...

Embodiment 3

[0038] Take 0.40 grams of ruthenium powder, add 1.15 grams of potassium nitrate and 0.64 grams of potassium hydroxide in a nickel crucible and mix evenly, place it in a muffle furnace at 600 °C for 1 hour, and dissolve the ruthenium with 10 ml of deionized water after cooling to room temperature Potassium ruthenate, at room temperature, add aqueous solution of potassium ruthenate to ammonia solution (ratio of ammonia to ruthenium is 6:1, ammonia solution 2 milliliters), adjust solution pH= 6. Add 10% barium (based on the mass of activated carbon, barium nitrate as the precursor), dissolve and impregnate with equal volume and dry. A series of ammonia synthesis catalysts with different ratios of barium to ruthenium can be prepared by changing the added amount of ruthenium complex and additives. The ratio of hydrogen to nitrogen in the mixed gas is 3:1, and the space velocity is 10000 h -1 , the reaction pressure is 10 MPa, and the reaction temperature is 400 ℃, the ammonia synt...

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Abstract

The invention discloses a ruthenium ammonia synthesis catalyst taking a ruthenium ammonia complex as a precursor and a preparation method thereof. The ruthenium ammonia synthesis catalyst comprises the following components: one of RuL+M1+M2 / AC, M1-(RuL+M1+M2) / AC, (RuL+M1+M2)-M1 / AC, and (RuL+M1+M2)-M2-M1 / AC, wherein RuL is a soluble ruthenium complex generated from reaction of potassium ruthenate and ammonia; M1 is one of or a mixture of more of barium nitrate, barium acetate, magnesium nitrate, ammonium nitrate, aluminum nitrate and zirconium nitrate; M2 is one of or a mixture of more of alkali metals such as sodium, potassium, rubidium and caesium, nitrates of rare earth metals, acetates, hydroxides or oxides; and AC is a carrier, namely active carbon or graphitized active carbon. According to the method, the graphitized active carbon is used as the carrier, and the ammonia synthesis catalyst is prepared by the following steps of preparing the potassium ruthenate, preparing the precursor, preparing mixed solution, preparing the catalyst, drying and the like. The preparation method has the advantages of simple equipment and procedure, short preparation period, high efficiency, energy conservation and environmental protection; large-scale production is easy to realize; and the prepared catalyst has high performance price ratio.

Description

technical field [0001] The invention belongs to the technical field of ammonia synthesis catalyst preparation, and more specifically relates to a ruthenium-based ammonia synthesis catalyst using ruthenium ammonia complex as a precursor and a preparation method thereof. Background technique [0002] Ammonia synthesis is a pillar industry in the chemical industry, and ruthenium-based ammonia synthesis catalysts are considered to be the second generation of ammonia synthesis catalysts after iron catalysts. In the 1980s and 1990s, people have studied the application of various ruthenium precursors in ruthenium-based ammonia synthesis catalysts, and the preparation methods of different catalysts corresponding to different ruthenium precursors. Some early literature introductions This part of the research results: the main precursor of ruthenium catalyst is Ru 3 (CO) 12 、RuCl 3 、Ru(acac) 3 (acac=acetylacetone), RuNO(NO 3 ) 3 、RuCl 3 etc., but the high input of noble metals...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J23/58C01C1/04
CPCY02P20/10Y02P20/52
Inventor 倪军陈赓魏可镁林建新林炳裕
Owner 福建三聚福大化肥催化剂国家工程研究中心有限公司
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