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Oxynitride hydride, metal carrier containing oxynitride hydride, and catalyst for ammonia synthesis

A technology of oxygen-nitrogen hydrides and loads, which is applied in the field of catalysts for ammonia synthesis, can solve the problems of undisclosed catalysts, and achieve the effect of excellent productivity and cost

Pending Publication Date: 2021-12-03
JAPAN SCI & TECH CORP
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0006] On the other hand, although BaCe doped with nitrogen was reported 2 o 4 (Oxynitride, BaCe 2 (O, N) 4 ) synthesis method, etc., but it is not disclosed that it is used as a catalyst for ammonia synthesis (for example, non-patent document 3)

Method used

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  • Oxynitride hydride, metal carrier containing oxynitride hydride, and catalyst for ammonia synthesis
  • Oxynitride hydride, metal carrier containing oxynitride hydride, and catalyst for ammonia synthesis
  • Oxynitride hydride, metal carrier containing oxynitride hydride, and catalyst for ammonia synthesis

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no. 1 approach

[0084] (Perovskite Oxygen Nitrogen Hydride)

[0085] The oxynitrogen hydride of the first embodiment of the present invention is a perovskite-type oxynitrogen hydride having a perovskite-type crystal structure. Perovskite-type oxynitride hydride is a mixture of nitrogen and hydrogen in BaCeO 3 Perovskite-type oxynitride hydride obtained by doping on the oxygen site. The perovskite-type oxynitrogen hydride of the first embodiment of the present invention (hereinafter, sometimes referred to as the present embodiment) is a compound represented by the following general formula (2) and has a perovskite-type crystal structure. It has BaCeO with no nitrogen and hydrogen doping 3same type of crystal structure. That is, for the perovskite-type oxynitrogen hydride of the present embodiment, preferably, after doping BaCeO with nitrogen and hydrogen 3 While maintaining the perovskite crystal structure.

[0086] BaCeO 3-x N y h z (2)

[0087] In the above general formula (2), x r...

Embodiment 1

[0195] (Preparation of catalyst for ammonia synthesis)

[0196] [BaCeO 3-x N y h z Synthesis of powder]

[0197] By adding CeO 2 Vacuum heat treatment was carried out at 600°C to remove water adsorbed on the surface, and the dehydrated CeO 2 and Ba(NH 2 ) 2 Mixing was performed in an Ar glove box using an agate mortar. At this time, mixing was performed so that the molar ratio of Ce and Ba became 1:1. By dissolving the obtained powder in NH 3 Heat treatment at 600 °C for 6 hours in air flow to obtain BaCeO 3-x N y h z powder.

[0198] [to BaCeO 3-x N y h z Loading of Ru]

[0199] The powdered BaCeO obtained by the above-mentioned method 3-x N y h z 0.50g and Ru 3 (CO) 12 (Aldrich, 99%) 0.056g (with respect to BaCeO 3-x N y h z In other words, as the supported metal Ru (corresponding to 5% by mass) was inserted into a quartz glass tube, heated at 70° C. for 1 hour in a vacuum, followed by heating at 120° C. for 1 hour, so that Ru 3 (CO) 12 attached to...

Embodiment 2

[0208] [to BaCeO 3-x N y h z load of Co]

[0209] The powdered BaCeO obtained by the above-mentioned method 3-x N y h z 95mg with Co 2 (CO) 8 14.5mg (relative to BaCeO 3-x N y h z In other words, Co as the supported metal (corresponding to 5% by mass) was placed in a quartz glass reaction tube, and then 15 mL / min of nitrogen gas and 45 mL / min of hydrogen gas (60 mL / min in total) were circulated in the reaction tube, and the temperature was raised for 2 hours. Up to 400 ° C, maintained for 5 hours, obtained in BaCeO 3-x N y h z The load with Co immobilized on it (hereinafter, Co / BaCeO 3-x N y h z ).

[0210] Hereinafter, ammonia synthesis was performed using the catalyst for ammonia synthesis described above.

[0211] [BaCeO loaded with Co 3-x N y h z Ammonia Synthesis]

[0212]

[0213] In addition to using the above Co / BaCeO 3-x N y h z As a catalyst to replace the Ru / BaCeO of Example 1 3-x N y h z Except, by using the same method and conditions...

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Abstract

Provided is a perovskite-type oxynitride hydride that is, when used as a catalyst carrier, capable of facilitating synthesis by achieving both enhancement and stabilization of the catalyst performance. The present invention provides an oxynitride hydride represented by general formula (1a) that is ABO<3-x>NyHz or (1b) that is AB2O<4-x>NyHz. In general formulas (1a) and (1b), A indicates at least one type selected from the group consisting of Ba and Sr; B indicates at least one type selected from the group consisting of Ce, La, and Y; x indicates a number represented by 0.2 <= x <= 2.0; y indicates a number represented by 0.1 <= y <= 1.0; and z indicates a number represented by 0.1 <= z <= 1.0.

Description

technical field [0001] The present invention relates to oxynitrogen hydrides, metal supports containing oxynitrogen hydrides, and catalysts for ammonia synthesis. [0002] This application claims priority based on Japanese Patent Application No. 2019-034878 for which it applied in Japan on February 27, 2019, and uses the content here. Background technique [0003] Haber-Bosch process (Haber-Bosch process) is a representative ammonia synthesis method, which is used in Fe 3 o 4 Contains a few mass% of Al in 2 o 3 and K 2 A double-promoted iron (Doubly promoted iron) catalyst for O, and a method for producing ammonia by directly reacting a mixed gas of nitrogen and hydrogen with the catalyst under high-temperature and high-pressure conditions. Even at present, this technology is used in industry almost in the same manufacturing process as when it was completed at that time. [0004] On the other hand, a method of synthesizing ammonia at a temperature lower than the reacti...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J27/24B01J32/00B01J37/08C01B21/092C01C1/02
CPCY02P20/52C01C1/0411B01J23/002B01J37/0207B01J23/745B01J23/75B01J23/462B01J31/20B01J37/086B01J35/30B01J23/10B01J37/04B01J37/08C01P2002/72C01P2002/84
Inventor 北野政明细野秀雄横山寿治鲸井纯
Owner JAPAN SCI & TECH CORP
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