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Dinuclear complex catalyst, preparation method and application thereof in preparing hydrogen by catalyzing formic acid decomposition

A technology for binuclear complexes and catalysts, applied in the field of binuclear complex catalysts and their preparation, can solve the problems of complex preparation process and high catalyst cost, and achieve the effects of simple preparation process, good solubility and stable performance

Active Publication Date: 2016-08-10
DALIAN UNIV OF TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

However, this type of catalyst also has the problems of complicated preparation process and high catalyst cost.

Method used

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  • Dinuclear complex catalyst, preparation method and application thereof in preparing hydrogen by catalyzing formic acid decomposition
  • Dinuclear complex catalyst, preparation method and application thereof in preparing hydrogen by catalyzing formic acid decomposition
  • Dinuclear complex catalyst, preparation method and application thereof in preparing hydrogen by catalyzing formic acid decomposition

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0026] Ru 2 Cl 2 (PPh 3 ) 4 Preparation of (μ-biim) and Catalysis of HCO 2 H decomposes to produce hydrogen:

[0027] (1) RuCl 2 (PPh 3 ) 3 (96.6mg, 100.0μmol)) and bidiimidazole (14.2mg, 106.0μmol) were added to CH with a volume ratio of 1:1 2 Cl 2 / CH 3 OH solution (20mL), under nitrogen protection, stirred at 25°C for 3h; after the reaction, the solution was evaporated in vacuo to remove the solvent, washed with n-hexane, filtered under reduced pressure, the solid was collected and dried in vacuo to give dark green solid RuCl 2 (H 2 biim) (PPh 3 ) 2 Product 53.6mg, yield 65%;

[0028] (2) RuCl 2 (H 2 biim) (PPh 3 ) 2 (53.6mg, 64.5μmol) by adding CH at a volume ratio of 1:1 2 Cl 2 / CH 3 In OH solution (20mL), KOH solid (3.6mg, 64.5μmol) was added thereto, under the protection of nitrogen, stirred at 25°C for 2h; use CH 2 Cl 2 (10mL) was dissolved, filtered under reduced pressure, the filtrate was evaporated under reduced pressure to remove the solvent,...

Embodiment 2

[0033] Ru 2 Cl 4 (PPh 3 ) 4 Preparation of (μ-bpym) and Catalytic Decomposition of Formic Acid to Hydrogen Production:

[0034] (1) Weigh RuCl 2 (PPh 3 ) 3 Add (104.0mg, 108.5μmol) and bipyrimidine (8.6mg, 54.2μmol) into 20mL of anhydrous methanol; vacuumize with an oil pump, fill in nitrogen, and repeat this gas replacement step three times. Under the protection of nitrogen, stir and react at 20°C for 3 hours, and the solution turns dark green; after the reaction, cool to room temperature, filter under reduced pressure, and collect the solid; wash the solid with ether, filter under reduced pressure, collect the solid, and dry in vacuum to obtain a brick red color Solid Ru 2 Cl 4 (PPh 3 ) 4 (μ-bpym) product 56.4 mg, yield 67%.

[0035] (2) HCO 2 H / NEt 3 System preparation: measure 3mL NEt 3 , 2mL anhydrous HCO 2 H. Prepare HCO with 2mL DMF 2 H / NEt 3 solution; under nitrogen protection, the HCO 2 H / NEt 3 - The DMF solution is frozen in liquid nitrogen until i...

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PUM

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Abstract

The invention provides a dinuclear complex catalyst, a preparation method and application thereof in preparing hydrogen by catalyzing formic acid decomposition. Central metal ions in both sides of the synthetic dinuclear complex catalyst are the same species of metal ions, and the ligand coordinating with each side of the metal ion contains two triphenylphosphine and 1-2 chloridion. The bridging ligand is bisglyoxalidine or bipyrimidine, and the dinuclear complex catalyst is used for preparing hydrogen by catalyzing formic acid decomposition. The dinuclear complex catalyst has good solubleness in formic acid / triethylamine organic solvent system, has good catalytic performance, and has long service life. The method provides an easily-prepared novel transition-metal catalyst with good performance and high efficiency for preparing hydrogen by catalyzing formic acid decomposition.

Description

technical field [0001] The invention relates to a dinuclear complex catalyst and a preparation method thereof, in particular to a method for using the dinuclear complex catalyst to catalyze the decomposition of formic acid to produce hydrogen. Background technique [0002] Hydrogen has the characteristics of environmental friendliness, abundant sources, high calorific value, good combustion performance, and high potential economic benefits, and is considered to be an ideal clean fuel. However, because hydrogen exists in gaseous form under normal conditions, and is flammable, explosive, easy to diffuse, and has a very low volumetric energy density, the safe and efficient storage and transportation of hydrogen has become the key to the promotion of hydrogen energy applications and the development of hydrogen economy. . [0003] Among many hydrogen storage materials, formic acid has the characteristics of moderate hydrogen release temperature, safety and non-toxicity, and high...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J31/24C01B3/22
CPCB01J31/2409B01J2531/0205B01J2531/0216B01J2531/821C01B3/22
Inventor 王万辉包明李桂平刘胜先戚妙韩东王宏
Owner DALIAN UNIV OF TECH
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