Catalyst for catalyzing formaldehyde or derivative thereof to prepare hydrogen, and synthesis method and application thereof

A synthesis method and technology of derivatives, which can be used in organic compound/hydride/coordination complex catalysts, physical/chemical process catalysts, chemical instruments and methods, etc. poisoning effect

Active Publication Date: 2018-09-07
SUZHOU INST OF NANO TECH & NANO BIONICS CHINESE ACEDEMY OF SCI
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

However, the reaction process requires the participation of a larg...

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  • Catalyst for catalyzing formaldehyde or derivative thereof to prepare hydrogen, and synthesis method and application thereof
  • Catalyst for catalyzing formaldehyde or derivative thereof to prepare hydrogen, and synthesis method and application thereof
  • Catalyst for catalyzing formaldehyde or derivative thereof to prepare hydrogen, and synthesis method and application thereof

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[0033] The embodiment of the present invention also provides a synthesis method of the aforementioned catalyst that catalyzes the production of hydrogen from formaldehyde or its derivatives, which includes:

[0034] Provides [Ru(Y)] n Z m , wherein Y includes 4-methylisopropylphenyl, pentamethylcyclopentadienyl, phenyl, tolyl, trimethylphenyl, 1,2,4,5-tetramethylphenyl, hexamethylphenyl Any one, but not limited thereto, Z includes and is not limited to any one or a combination of two or more of I, Cl, Br, n and m are natural numbers, and the value range of n and m is 1-10;

[0035] The [Ru(Y)] n Z m Dispersed in water to form a suspension, the temperature of the suspension is controlled between 0 and 100°C, preferably 60°C, then silver salt is added, and the water is removed after the reaction to obtain Ru(Y)(H 2 O) n x m .

[0036]In some embodiments, the synthesis method further comprises: combining the Ru(Y)(H 2 O) n x m Add water, then add ammonia water, remove w...

Embodiment 1

[0057] 1. the method for preparing described catalyst in the present embodiment is:

[0058] 1) Put [Ru(Y)] n Z m (wherein Y is 4-methylisopropylphenyl, Z is Cl, n is 2, and m is 4), add in water, make suspension after stirring, be heated to 60 ℃, then add 2 equivalents of silver salt ( It can be silver nitrate, silver sulfate, silver phosphate, silver tetrafluoroborate, silver hexafluorophosphate) reaction, during [Ru(Y)] n Z m Will gradually dissolve, while forming a white silver chloride precipitate. Then the solvent water was removed by a rotary evaporator, and a series of water-soluble catalysts Ru(Y)(H 2 O) n x m , where Y is 4-methylisopropylphenyl, X can be PO 4 , NO 3 , BF 4 , SO 4 、PF 6 Any one of them, n and m are natural numbers with a value range of 1-9 (the values ​​of n and m vary according to X).

[0059] 2) The aforementioned series of Ru(Y)(H 2 O) n x m Add water, stir to make a solution, slowly add ammonia solution dropwise to the solution, an...

Embodiment 2- Embodiment 7

[0066] The preparation method of catalyst in this embodiment 2-7 is basically the same as embodiment 1, and difference is the raw material [Ru(Y)] that adopts n Z m Among them, Y is respectively pentamethylcyclopentadienyl, phenyl, tolyl, trimethylphenyl, 1,2,4,5-tetramethylphenyl, hexamethylphenyl, Z is any of I, Cl, Br one. This embodiment 2-7 also made a series of catalysts Ru(Y)(NH 3 ) n x m 、Ru(Y)(H 2 O) n x m , where n and m are natural numbers with a value range of 1-9, and the values ​​of n and m vary depending on X. Similarly, when these catalysts are used to catalyze formaldehyde, paraformaldehyde and polyoxymethylene to react directly with water to produce hydrogen, it can be found that the molar ratios of hydrogen and carbon dioxide in the gas products produced are basically in the 2:1 or so, the carbon monoxide content is lower than 10ppm.

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Abstract

The invention discloses a catalyst for catalyzing formaldehyde or a derivative thereof to prepare hydrogen, and a synthesis method and application thereof. The chemical formula of the catalyst is Ru(Y)BnXm, wherein Y comprises any one selected from the group consisting of 4-methylisopropylphenyl, pentamethylcyclopentadienyl, phenyl, tolyl, trimethylphenyl, 1,2,4, 5-tetramethylphenyl and hexamethylphenyl; B comprises H2O or NH3; and X comprises any one selected from the group consisting of PO4, NO3, BF4, SO4 and PF6, or a mixture of two or more selected from the group. The synthesis method forthe catalyst comprises the following steps: providing [Ru(Y)]nZm, dispersing [Ru(Y)]nZm in water to form a suspension, controlling the temperature of the suspension to be in a range of 0 and 100 DEG C, then adding a silver salt, and carrying out a reaction, wherein Ru(Y)BnXm is obtained after completion of the reaction. The catalyst of the invention has high catalytic activity, is easily soluble in water, does not need strong alkali; the concentration of carbon monoxide in generated gas is less than 10 ppm; and the catalyst can be directly applied to a hydrogen-oxygen fuel cell system and eradicates the problem of fuel cell poisoning caused by high concentration of carbon monoxide.

Description

technical field [0001] The invention relates to an organic ruthenium catalyst, in particular to a catalyst capable of catalyzing the reforming reaction of formaldehyde and its derivatives such as paraformaldehyde and polyoxymethylene with water in an aqueous solution to produce hydrogen, its synthesis method and application, belonging to energy catalytic materials, Hydrogen manufacturing technology field. Background technique [0002] Formaldehyde is a common air and water pollutant. Every year, many people lose their lives due to indoor formaldehyde pollution. Therefore, how to efficiently and quickly convert formaldehyde and make full use of it has become a difficult problem. Formaldehyde is not only a great pollution to the environment, but also a potential hydrogen carrier, its mass hydrogen content is as high as 6.67%, so it has great application value. Formaldehyde has a high chemical reactivity and is relatively easily catalytically converted into other substances, s...

Claims

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Application Information

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IPC IPC(8): B01J31/12C01B3/32
CPCB01J31/12B01J35/0033C01B3/326
Inventor 周小春沈杨彬展裕璐
Owner SUZHOU INST OF NANO TECH & NANO BIONICS CHINESE ACEDEMY OF SCI
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