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Support metal catalyst and method for synthesizing ammonia using same catalyst

A technology for supporting metals and catalysts, applied in metal/metal oxide/metal hydroxide catalysts, nitrogen-metal/silicon/boron binary compounds, chemical instruments and methods, etc., can solve the problem of easy oxidation, instability, etc. problem, to achieve the effect of efficient synthesis

Active Publication Date: 2016-11-23
JAPAN SCI & TECH CORP +1
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0006] In addition, it is known that Ca 2 N is easily oxidized and is an extremely unstable substance. It has been reported that Ca 2 The stable range of N is in argon below 1000°C or in nitrogen at 250°C to 800°C (Non-Patent Document 1)

Method used

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  • Support metal catalyst and method for synthesizing ammonia using same catalyst
  • Support metal catalyst and method for synthesizing ammonia using same catalyst
  • Support metal catalyst and method for synthesizing ammonia using same catalyst

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0082] 3 N 2 Preparation of >

[0083] 1 g of commercially available reagent Ca 3 N 2 Powder (BET surface area approx. 1m 2 g -1 ) in the glove box of Ar environment with 0.042g of Ru 3 (CO) 12 The powders are mixed and packed into vacuumed quartz glass tubes. While rotating the sample contained in the glass tube, it was heated at a temperature of 250° C. for 15 hours. Ca loaded with 2 wt% Ru metal particles was thus prepared 3 N 2 catalyst. The catalyst has a BET surface area of ​​about 1 m 2 g -1 , there is almost no change in the BET surface area after loading. Ru dispersion (%) measured by CO adsorption method was 3.0.

[0084]

[0085] Nitrogen (N 2 ) and hydrogen (H 2 ) react to form ammonia (NH 3 ) synthesis reaction. When the reaction temperature is 400°C, put 0.2g of the catalyst prepared by the above method into a glass tube, and when the reaction temperature is 340°C, put 0.1g of the above catalyst into the glass tube, and use a fixed-bed flow-thr...

Embodiment 2

[0087] In addition to using Ca 2 N (BET surface area is 1m 2 g -1 ) instead of Ca in Example 1 3 N 2 In addition, the same method as in Example 1 was used to prepare 2wt% Ru / Ca 2 N catalyst, under the same conditions as in Example 1, the ammonia synthesis reaction was implemented. The rate of ammonia synthesis at 400°C is figure 1 As shown, it is 2750μmolg -1 h -1 . The rate of ammonia synthesis at 340°C is shown in Table 1, which is 3386 μmolg -1 h -1 . TOF (×10 -3 the s -1 ) is 171.2.

Embodiment 3

[0089] In addition to using Ca(NH 2 ) 2 (BET surface area is 120m 2 g -1 ) instead of Ca in Example 1 3 N 2 In addition, the same method as in Example 1 was used to prepare 2wt% Ru / Ca (NH 2 ) 2 Catalyst, implement ammonia synthesis reaction under the same conditions as in Example 1. The rate of ammonia synthesis at 340°C is shown in Table 1, which is 2118 μmolg -1 h -1 . TOF (×10 -3 the s -1 ) is 3.2.

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Abstract

A catalyst for continuous synthesis of ammonia using gas containing hydrogen and nitrogen as raw materials is characterized in that a vector supporting a transition metal exhibiting catalytic activity is a two-dimensional electride or a precursor thereof. The two-dimensional electride or the precursor thereof is: MxNyHz (M is one or more types of group 2 metals selected from the group consisting of Mg, Ca, Sr, and Ba; x, y, and z are defined as 1 <= x <= 11, 1 <= y <= 8, and 0 <= z <= 4, respectively; x is an integer; and y and z are not limited to being integers); a metal nitride represented by M3N2 (M being as defined above); or a metal carbide selected from the group consisting of Y2C, Sc2C, Gd2C, Tb2C, Dy2C, Ho2C, and Er2C. Using such catalysts, the nitrogen and hydrogen as raw materials are continuously reacted on the catalyst in an ammonia synthesis reaction device under the following conditions: a reaction temperature of preferably 100 to 600 DEG C and a reaction pressure of 10 kPa or greater and less than 20 MPa.

Description

technical field [0001] The present invention relates to a kind of catalyst that is loaded with metal on carrier, especially a kind of loaded metal catalyst for ammonia synthesis with electron compound (electride) as carrier and ammonia synthesis method using the catalyst, said electron compound is electron in A substance in which anion electrons exist between the layers of a layered compound. Background technique [0002] with M 3 N 2 Alkaline earth metal nitrides represented by (M is Ca, Sr or Ba) are used in aluminum nitride raw materials for semiconductor devices, ceramic particles for metal sliding parts, battery electrode constituent materials, conductive particles, etc. (Patent Document 1). Patent Document 1 discloses thermally decomposing Group II metal amides to produce M 3 N 2 (M is Be, Mg, Ca, Sr or Ba) or M 2 N (M is Be, Mg, Ca, Sr or Ba) and other methods. Patent Document 2 discloses that ammonia is reacted with a Group II metal to liquefy it to obtain a Gr...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J27/24B01J27/22C01B21/06C01B31/30C01C1/04
CPCB01J23/462B01J27/22B01J27/24B01J35/1009C01B21/0612C01C1/0411C01P2006/12Y02P20/52B01J23/745B01J23/75B01J35/0006
Inventor 细野秀雄原亨和北野政明横山寿治井上泰德神原慎志
Owner JAPAN SCI & TECH CORP
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