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Core-shell structured supported carbon nanotube catalyst and preparation method thereof

A technology of carbon nanotubes and core-shell structure, which is applied in the field of core-shell structure-loaded carbon nanotube catalysts and their preparation, can solve the problems of high cost and complicated process, and achieve the effects of low equipment requirements, simple raw materials, and easy realization

Inactive Publication Date: 2017-01-18
HUBEI UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0007] In view of the complex process and high cost of catalysts synthesized in the prior art to catalyze the interpretation of hydrogen from ammonia borane water, the object of the present invention is to provide a core-shell structure-supported carbon nanotube catalyst and a preparation method thereof

Method used

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  • Core-shell structured supported carbon nanotube catalyst and preparation method thereof
  • Core-shell structured supported carbon nanotube catalyst and preparation method thereof
  • Core-shell structured supported carbon nanotube catalyst and preparation method thereof

Examples

Experimental program
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Effect test

Embodiment 1

[0028] Example 1: Preparation of core-shell structure Ru@CoNi / CNTs supported carbon nanotube catalyst

[0029] Weigh a certain amount of commercial carbon nanotubes (40-60nm) and add mixed acid (H 2 SO 4 :HNO 3 =3:1) solution, condensed and refluxed at 120° C. for 2 hours; cooled the solution, adjusted the pH to neutral with alkali, filtered, washed, and dried to obtain activated carbon nanotubes.

[0030] Weigh 8 mg of the above-mentioned carbon nanotubes, in a solution (40 mL) with a volume ratio of 1:1 of ethylene glycol and water, sonicate for 10 minutes, and then add RuCl 3 (0.24mL, 0.01mol / L), Co(NO 3 ) 2 (0.576mL, 0.01mol / L), Ni(NO 3 ) 2 (0.864mL, 0.01mol / L) solution, stirred for 24 hours. Dissolve 60.0 mg of ammonia borane solid (reducing agent) in 10 mL of deionized water, add this solution dropwise to the above solution, and continue stirring for 10 minutes until no bubbles are generated. The product was filtered, washed, and dried to obtain a core-shell stru...

Embodiment 2

[0032] Example 2 (Comparison 1): Preparation of Alloy Structure RuCoNi / CNTs Supported Catalyst

[0033] Weigh a certain amount of commercial carbon nanotubes (40-60nm) and add mixed acid (H 2 SO 4 :HNO 3 =3:1) solution, condensed and refluxed at 120° C. for 2 hours; cooled the solution, adjusted the pH to neutral with alkali, filtered, washed, and dried to obtain activated carbon nanotubes.

[0034] Weigh 8 mg of the above-mentioned carbon nanotubes, in a solution (40 mL) with a volume ratio of 1:1 of ethylene glycol and water, sonicate for 10 minutes, and then add RuCl 3 (0.24mL, 0.01mol / L), Co(NO 3 ) 2 (0.576mL, 0.01mol / L), Ni(NO 3 ) 2 (0.864mL, 0.01mol / L) solution, stirred for 24 hours. Dissolve 60.0 mg of sodium borohydride solid (reducing agent) in 10 mL of deionized water, add this solution dropwise to the above solution, and continue stirring for 10 minutes until no bubbles are generated. The product is filtered, washed and dried to obtain an alloy structure RuC...

Embodiment 3

[0035] Example 3 (Comparison 2): Preparation of Ru@CoNi nanoparticles with core-shell structure

[0036] Add RuCl 3 (0.24mL, 0.01mol / L), Co(NO 3 ) 2 (0.576mL, 0.01mol / L), Ni(NO 3 ) 2 (0.864mL, 0.01mol / L) solution was mixed and stirred for 24 hours. Dissolve 60.0 mg of ammonia borane solid (reducing agent) in 10 mL of deionized water, add this solution dropwise to the above solution, and continue stirring for 10 minutes until no bubbles are generated. The product was filtered, washed and dried to obtain the Ru@CoNi nanoparticle catalyst with core-shell structure.

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Abstract

The invention relates to a core-shell structured supported carbon nanotube catalyst and a preparation method thereof. The catalyst adopts carbon nanotubes (CNTs) as a carrier and adopts borazane as a reducing agent. The preparation method comprises the following steps: reducing precursors comprising a ruthenium salt, a cobalt salt and a nickel salt, loading the reduced precursors on the CNTs, filtering the above obtained product, washing the filtered product, and drying the washed product to obtain the core-shell structured Ru@CoNi / CNTs nanocatalyst. The average particle size of metals supported on the core-shell structured Ru@CoNi / CNTs nanocatalyst synthesized through the preparation method is 1.5 nm, the catalyst has high catalysis activity on hydrolysis of borazane for releasing hydrogen, the transformation frequency (TOF) is 408.9 H2 min<-1> (mol Ru)<-1>, and the activation energy (Ea) is 23.53 kJ mol<-1>. The catalyst still has good stability after 5 cycle test, the average particle size of metal particles is 1.64 nm, and the metal particles are uniformly dispersed. The noble metal / non-noble metal doped core-shell structured supported nanocatalyst adopting the CNTs as the carrier has the characteristics of uniform metal particle distribution, many catalysis activity sites and good stability; and compared with traditional noble metal catalysts, the nanocatalyst has the advantages of low cost, simplicity in preparation, easy obtaining of the raw materials, and suitableness for industrial production.

Description

technical field [0001] The invention belongs to the field of nano-catalysis materials, and relates to a core-shell structure-loaded carbon nanotube catalyst and a preparation method thereof, which are used for efficiently catalyzing ammonia borane water to decompose hydrogen. Background technique [0002] With the aggravation of energy crisis and more and more environmental problems, hydrogen energy is considered as an ideal clean energy alternative to traditional fossil fuels. In past research, great efforts have been made to develop suitable materials for storing and releasing hydrogen. Among the numerous hydrogen storage materials, ammonia borane (AB) is considered as one of the most desirable candidate materials because of its high hydrogen storage capacity (19.6 wt %), low density, non-toxicity, and stability in aqueous solution. [13-16] . At room temperature, without a catalyst, the hydrolysis rate of ammonia borane is extremely slow, and almost no hydrogen is produc...

Claims

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Application Information

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IPC IPC(8): B01J23/89
CPCB01J23/892B01J37/0207B01J37/16B01J35/396B01J35/393
Inventor 周立群熊星杨坤洲
Owner HUBEI UNIV
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