Iridium catalyst used for catalyzing ammonia borane hydrolysis hydrogen production process, and preparation method and application thereof

A technology for hydrogen production by catalyzing ammonia borane and hydrolysis, which is applied in the field of iridium catalyst, preparation and application by catalyzing the hydrolysis of ammonia borane to produce hydrogen, and can solve the problems of not unique reaction products, a large amount of organic solvents, and unsolved problems such as borazine , to achieve the effect of excellent water solubility

Active Publication Date: 2015-09-23
DALIAN UNIV OF TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

The use of metal-catalyzed dehydrogenation of ammonia borane was carried out earlier, Jaska et al. [1] In 2003, the heterogeneous catalyst Rh complex ([Rh(1,5-cod)-(μ-Cl)] was first reported 2 (cod=1,5-cyclooctadiene)) catalyzes the dehydrogenation of ammonia borane, but this catalyst requires a large amount of organic solvent in the catalytic process, the reaction product is not unique, and the reaction process is accompanied by the generation of borazine toxic gas impurities
2008 Friedrich et al. [2] For the first time, a transition metal Ru-PNP homogeneous catalyst was reported for the catalytic dehydrogenation of ammonia borane. Although the catalytic performance is excellent, the process requires tetrahydrofuran (THF) as a solvent, and the hydrogen release process will release toxic gas borazine
2010 Williams et al. [3] Shvo catalysts containing hydroxyl groups have been reported, but the problem of the release of toxic gas borazine during the hydrogen release process has not yet been solved
2010 Ciganda et al. [4] For the first time, transition metal homogeneous catalysts (HCl{(PPh 2 (o-C 6 h 4 CO)) 2 H}]), although the catalytic hydrogen desorption performance is excellent, but the water solubility of the catalyst is too poor
[0011] The shortcomings of the catalyst used for the hydrolysis of ammonia borane to decompose hydrogen are: the catalytic performance is not high, the release of toxic gas impurities during the dehydrogenation process, and the catalyst has poor water solubility

Method used

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  • Iridium catalyst used for catalyzing ammonia borane hydrolysis hydrogen production process, and preparation method and application thereof
  • Iridium catalyst used for catalyzing ammonia borane hydrolysis hydrogen production process, and preparation method and application thereof
  • Iridium catalyst used for catalyzing ammonia borane hydrolysis hydrogen production process, and preparation method and application thereof

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Experimental program
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Embodiment 1

[0042] Embodiment 1: Catalyst (I) [(X 1 =C)(X 2 =C)(X 3 =C)(L=H 2 O)(R 1 =Me)(R 2 =H)(m=+2)(W=SO 4 2- )]: ([Cp*Ir(6-Me-py-pz)(H 2 O)] SO 4 ) preparation

[0043] Under nitrogen protection, 2-bromo-6-picoline (2.0 mmol), pyrazole (3 mmol, 1.5 equiv), Cu 2 O (0.2mmol, 0.1equiv), ninhydrin (0.4mmol, 0.2equiv), KOH (4mmol, 2.0equiv) and 15mL dry solvent DMSO, heated to 120°C, followed by TLC spot plate during the experiment (developing agent: n-hexane / dichloromethane=4 / 1) until the reaction of the substrate was complete, and the reaction was stirred for a total of 36 hours. The reaction was stopped, cooled to room temperature, and 5 mL of water was added. The reaction mixture was filtered through celite, and the filter cake was washed with dichloromethane. Dichloromethane extracted the filtrate two to three times, collected the organic phase extract, washed twice with water, and washed two to three times with brine. Anhydrous Na 2 SO 4 dry. After filtration, the so...

Embodiment 2

[0047] Embodiment 2: Catalyst (I) [(X 1 =C)(X 2 =C)(X 3 =C)(L=H 2 O)(R 1 =OH)(R 2 =H)(m=+2)(W=SO 4 2- )]: ([Cp * Ir(6-OH-py-pz)(H 2 O)] SO 4 ) preparation:

[0048] Take a 50mL two-necked flask, put it into a magnet, and add 2-bromo-6-methoxypyridine (2.0mmol), pyrazole (3mmol, 1.5equiv), Cu 2 O (0.2mmol, 0.1equiv), ninhydrin (0.4mmol, 0.2equiv), KOH (4mmol, 2.0equiv) and 15mL of dry solvent DMSO, oil bath constant temperature 120 ℃, heating and reflux stirring reaction, the reaction process was tracked by TLC (Developer: n-hexane / dichloromethane=4 / 1), after 72h the reaction of the substrate was complete. After cooling to room temperature, 15 mL of deionized water was added. The reaction mixture was filtered through celite, and the filter cake was washed with dichloromethane. Then extract the filtrate with dichloromethane, emulsification occurs, add a small amount of NaCl to break the emulsion, let it stand until the solution is separated, continue to extract five...

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Abstract

The invention provides an iridium catalyst used for catalyzing ab ammonia borane hydrolysis hydrogen production process, and a preparation method and an application thereof. The iridium catalyst provided by the invention is a homogeneous catalyst. According to the preparation method, a ligand is prepared with halogenated hexanitrogen heterocyclopyridine and pentanitrogen heterocycle as raw materials; and the ligand is subjected to a hydration reaction with an iridium compound, such that the catalyst is obtained. An activity center is metal iridium. The iridium catalyst used for catalyzing the ammonia borane hydrolysis hydrogen production process has good water solubility, wherein the solubility is 5-50mmol / L. The catalyst performs good catalytic activity in catalyzing the ammonia borane hydrolysis hydrogen production process, wherein a turnover number TON is 1622.

Description

technical field [0001] The invention relates to a preparation method of an iridium catalyst for catalyzing the hydrolysis of ammonia borane to produce hydrogen and its application in catalyzing the hydrolysis of ammonia borane to produce hydrogen. Background technique [0002] Ammonia borane is a new type of chemical hydrogen storage material. Its mass hydrogen storage density is as high as 19.6wt%. It has the characteristics of suitable hydrogen release temperature, safe and non-toxic hydrogen release process, thermal stability and chemical stability. However, the key to the commercial utilization of ammonia borane is to solve technical problems such as slow hydrogen desorption kinetics, low hydrogen desorption, and release of impurity gas pollutants. catalyst. [0003] Over the years, researchers have been working on the research and development of new efficient and highly selective catalysts for the hydrogen release of ammonia borane. The use of metal-catalyzed dehydrog...

Claims

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Application Information

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IPC IPC(8): B01J31/22C07F15/00C01B3/04
CPCY02E60/36
Inventor王万辉杨堃包明
OwnerDALIAN UNIV OF TECH