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A rhodium catalyst for nitrogen reduction synthesis of ammonia and its preparation method and application

A rhodium catalyst, a technology for synthesizing ammonia, applied in the directions of catalyst activation/preparation, chemical instruments and methods, physical/chemical process catalysts, etc., can solve the problems of poor mass transfer active sites, and the nitrogen reduction performance needs to be further improved. Electrocatalytic nitrogen reduction performance, good catalytic selectivity and stability, the effect of maintaining stable current density

Active Publication Date: 2020-09-01
SHANDONG UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

The currently reported noble metal catalysts exhibit excellent nitrogen reduction performance. For example, in the literature "J.Mater.Chem.A 2018, 6(7), 3211-3217", K 3 Co(CN) 6 and RhCl 3 ·3H 2 O equimolar mixture, Mr. RhCl 3 –K 3 Co(CN) 6 cyanogel, and then adding the reducing agent HCHO to prepare two-dimensional rhodium nanosheets; the obtained rhodium was used to catalyze nitrogen reduction, and its average ammonia yield was 23.88 μg h at -0.2V -1 mg cat. -1 , the Faraday efficiency is 0.217%, indicating that the two-dimensional rhodium nanosheets have certain catalytic performance for nitrogen reduction, but they are still not good in terms of mass transfer and exposed active sites, and the nitrogen reduction performance needs to be further improved

Method used

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  • A rhodium catalyst for nitrogen reduction synthesis of ammonia and its preparation method and application
  • A rhodium catalyst for nitrogen reduction synthesis of ammonia and its preparation method and application
  • A rhodium catalyst for nitrogen reduction synthesis of ammonia and its preparation method and application

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Embodiment 1

[0031] A preparation method for a rhodium catalyst for nitrogen reduction synthesis of ammonia, comprising steps:

[0032] Weigh 3.68g of octylamine into a round-bottomed flask, place it in an ice-water bath at 0°C, and drop 1.32g of formic acid into octylamine drop by drop under constant stirring, and mix well until a white powdery solid particle is formed to obtain 5g N-octylammonium formate reducing ionic liquid.

[0033] In a 90°C oil bath, 10 mg of RhCl 3 ·3H 2 O was dissolved in the above 5g ionic liquid, and after it was completely dissolved, it was transferred to an airtight reaction kettle and subjected to ionothermal reaction at 180°C for 24 hours. After cooling to room temperature, it was washed three times with absolute ethanol and ultrapure water, and then the product was placed In a vacuum oven, dry at room temperature for 12 hours to obtain black solid powder nitrogen reduction catalyst three-dimensional rhodium particles.

[0034] The material composition of...

Embodiment 2

[0043] A preparation method for a rhodium catalyst for nitrogen reduction synthesis of ammonia, comprising steps:

[0044] Weigh 3.68g of octylamine into a round-bottomed flask, place it in an ice-water bath at 0°C, and drop 1.32g of formic acid into octylamine drop by drop under constant stirring, and mix well until a white powdery solid particle is formed to obtain 5g N-octylammonium formate reducing ionic liquid.

[0045] In a 90°C oil bath, 8 mg RhCl 3 ·3H 2 O was dissolved in the above 5g ionic liquid, and after it was completely dissolved, it was transferred to an airtight reaction kettle and subjected to ionothermal reaction at 180°C for 24 hours. After cooling to room temperature, it was washed three times with absolute ethanol and ultrapure water, and then the product was placed In a vacuum oven, dry at room temperature for 12 hours to obtain black solid powder nitrogen reduction catalyst three-dimensional rhodium particles.

Embodiment 3

[0047] A preparation method for a rhodium catalyst for nitrogen reduction synthesis of ammonia, comprising steps:

[0048] Weigh 3.68g of octylamine into a round-bottomed flask, place it in an ice-water bath at 0°C, and drop 1.32g of formic acid into octylamine drop by drop under constant stirring, and mix well until a white powdery solid particle is formed to obtain 5g N-octylammonium formate reducing ionic liquid.

[0049] In a 90°C oil bath, 10 mg of RhCl 3 ·3H 2 O was dissolved in the above 4.5g ionic liquid, and after it was completely dissolved, it was transferred to an airtight reactor, and was subjected to ionothermal reaction at 180°C for 24 hours. After cooling to room temperature, it was washed three times with absolute ethanol and ultrapure water, and then the product Place in a vacuum drying oven and dry at room temperature for 12 hours to obtain black solid powder nitrogen reduction catalyst three-dimensional rhodium particles.

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Abstract

The invention provides a rhodium catalyst used for nitrogen reduction to synthesize ammonia and its preparation method and application. First, formic acid and octylamine are used as raw materials to prepare reducing ionic liquid; then rhodium trichloride is dissolved in the ionic liquid, and the rhodium catalyst is obtained through ionothermal reaction at 150 to 200°C, centrifugation, washing, and drying. The preparation method of the invention is simple and quick, and can be completed in one step; the obtained rhodium catalyst is a three-dimensional porous rhodium particle with nanowires as a substructure, and has good electrocatalytic nitrogen reduction performance.

Description

technical field [0001] The invention relates to a rhodium catalyst used for nitrogen reduction to synthesize ammonia, a preparation method and application thereof, and belongs to the field of energy materials. Background technique [0002] As the main product of nitrogen fixation, ammonia is widely used in fertilizers, industrial chemicals and other fields. While maintaining the needs of the growing world population, ammonia acts as a carbon-free energy carrier and energy storage intermediate. NH 3 Play an important role in the sustainable development of modern society. But since N 2 Chemical inertness and low polarizability, synthesis of NH 3 Stricter reaction conditions are required. Currently NH 3 It is mainly produced by the Harper method under high temperature and pressure, and the reactant H is required for this reaction 2 and most of the energy comes from limited fossil raw materials, resulting in a large amount of energy loss and CO 2 emissions. Therefore, it ...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): B01J23/46B01J37/16B01J37/08C25B1/00C25B11/06
CPCB01J23/464B01J37/16B01J37/08C25B1/00C25B11/091B01J35/23B01J35/33
Inventor 李钟号陈婷婷
Owner SHANDONG UNIV