A method for hydrogen production by catalyzing the hydrolysis of ammonia borane with proton-responsive iridium complex

A technology for catalyzing ammonia borane and iridium complexes, applied in the field of energy and homogeneous catalysis, can solve the problems of poor water solubility of catalysts, and achieve good catalytic effect, good water solubility, and large hydrogen release effect

Active Publication Date: 2017-04-12
DALIAN UNIV OF TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

However, the catalysts are poor in water solubility and require the help of organic solvents to react well.

Method used

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  • A method for hydrogen production by catalyzing the hydrolysis of ammonia borane with proton-responsive iridium complex
  • A method for hydrogen production by catalyzing the hydrolysis of ammonia borane with proton-responsive iridium complex
  • A method for hydrogen production by catalyzing the hydrolysis of ammonia borane with proton-responsive iridium complex

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0036] [Cp*Ir(6,6'-(OH) 2 -bpy)(OH 2 )] SO 4 Preparation and catalysis of ammonia borane hydrolysis for hydrogen production:

[0037] (1) NiBr 2 (PPh 3 )2 (1.1146g, 1.5mmol), newly activated Zn powder (0.4904g, 7.5mmol), Et 4 NI (1.2858g, 5mmol) and 2-chloro-6-methoxypyridine (0.7179g, 5mmol) were added to anhydrous and oxygen-free tetrahydrofuran (20mL), and stirred at 50°C for 47h under an inert gas atmosphere.

[0038] (2) After the reaction, the solvent was evaporated to dryness, ammonia water (2mol / L, 30mL) was added, dichloromethane (10mL) was dissolved, and the insoluble matter was filtered off. The filtrate was extracted three times, washed with saturated sodium chloride solution, dried over anhydrous sodium sulfate, and filtered. The solvent was removed by rotary evaporation, and the crude product was obtained as a light yellow solid. Isopropanol was added to the crude product for recrystallization, and white crystals were precipitated. After filtration, 6,6'-d...

Embodiment 2

[0046] [{Cp*Ir(Cl)} 2 (thbm)]Cl 2 Preparation and catalysis of ammonia borane hydrolysis for hydrogen production:

[0047] (1) The synthesis of 4,4',6,6'-tetramethoxy-2,2'-bipyrimidine is the same as step (1) and (2) in Example 1

[0048] (2) Add 4,4',6,6'-tetrahydroxy-2,2'-bipyrimidine (0.1947g, 0.7mmol), iodotrimethylsilane (1mL, 7mmol) into anhydrous acetonitrile (5mL) , under an inert gas atmosphere, stirred and refluxed for 29h.

[0049] (3) After the reaction is finished, cool to room temperature. It was quenched by adding methanol, and the insoluble matter was collected by filtration, washed with methanol and ether successively to obtain a white solid. Dissolve and purify by heating with isopropanol, filter out insoluble matter, and dry to obtain 0.1181 g of pure product 4,4',6,6'-tetrahydroxy-2,2'-bipyrimidine, with a yield of 76%.

[0050] (4) Dissolve the ligand 4,4',6,6'-tetrahydroxy-2,2'-bipyrimidine (0.0444g, 0.2mmol) in anhydrous methanol, and then add [Cp*I...

Embodiment 3

[0054] [Cp*Ir(th4bpym)(OH 2 )] SO 4 Preparation and catalysis of ammonia borane hydrolysis for hydrogen production:

[0055] (1) The preparation of 2,2',6,6'-tetrahydroxy-4,4'-bipyrimidine is the same as steps (1), (2) and (3) in Example 2.

[0056] (2)[Cp*Ir(th4bpym)(OH 2 )] SO 4 The preparation is the same as step (6) in Example 1.

[0057] (3) Carry out deoxidation treatment to catalyst, deionized water, with embodiment 1 step (7).

[0058] (4) Under the protection of inert gas, take ammonia borane (30.8 mg, 1 mmol), add 10 mL of deoxygenated deionized water with pH=9 into the bottle, and heat to 65° C. under the protection of nitrogen. Catalyst solution (0.2 mL, 1 μmol) was added, the reaction was stirred, and the gas was collected by drainage. Record the hydrogen release volume and reaction time, calculate the TON of the catalytic reaction based on the hydrogen release amount is 1000, and the TOF of the initial 5min is 1230h -1 .

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Abstract

The invention belongs to the technical fields of energy and homogeneous catalysis, and provides a hydrogen production method by using a proton-responsive iridium complex for catalysis of ammonia borane hydrolysis. A series of electron-rich azacyclo-proton-responsive iridium complexes are synthesized as catalysts for catalysis of ammonia borane hydrolysis for hydrogen production. The invention has the advantages that the series of proton-responsive iridium complexes have high catalysis hydrogen desorption rate, large amount of hydrogen desorption and no generation of toxic by-products, and can achieve good catalytic effect under relatively mild conditions. The series of proton-responsive iridium complexes have good water solubility, and avoid the pollution caused by the use of organic solvent. Under alkaline conditions suitable for the preservation of ammonia borane, the hydroxy on the catalyst is subjected to deprotonation to form alkaline side O- with strong electron donating ability and to cooperate with the metal center for catalysis of ammonia borane dehydrogenation; and the method increases the reaction rate, and has great advantages in catalysis of ammonia borane hydrolysis.

Description

technical field [0001] The invention belongs to the technical field of energy and homogeneous catalysis, and relates to homogeneous catalysis for producing hydrogen from ammonia borane, in particular to a method for producing hydrogen by catalyzing the hydrolysis of ammonia borane with a proton-responsive iridium complex. Background technique [0002] As a clean and efficient green new energy, hydrogen has attracted much attention. After burning and releasing energy, only water is produced, which is a clean energy; it can be produced by photolysis or electrolysis of water, which is a renewable resource; and the thermal efficiency of hydrogen is extremely high. Therefore, hydrogen is considered to be the future energy source and the best substitute for fossil fuels. However, the development of the hydrogen economy is subject to many restrictions. Since hydrogen exists in gaseous form under normal conditions, and is flammable, explosive, and easy to diffuse, safe and efficien...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): C01B3/06B01J31/22C07F17/00
CPCY02E60/36
Inventor 王万辉陆文多包明
Owner DALIAN UNIV OF TECH
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